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Ischia Island (Naples, Italy)30|04 - 03|05 2009Aragonese CastlePhoto courtesy <strong>of</strong> Giovanni Mattera [www.giannimattera.it]Book<strong>of</strong>AbstractsORGANISING COMMITTEECarlo ALTUCCI (University <strong>of</strong> Naples, IT)Pietro Paolo CORSO (University <strong>of</strong> Palermo, IT)Rosario ESPOSITO (University <strong>of</strong> Naples, IT)Jonathan MARANGOS (Imperial College, UK)John TISCH (Imperial College, UK)Raffaele VELOTTA (University <strong>of</strong> Naples, IT)Università <strong>degli</strong> Studidi Napoli Federico IIImperial Collegehttp://ultrafast09.fisica.unina.it


<strong>UDIM09</strong>Second International Conference onUltra-fast Dynamic Imaging <strong>of</strong> MatterHotel Continental Terme, Ischia (Italy)30 th April – 3 rd May 2009


The organisers wish to thank <strong>the</strong> European Science Foundation who has strongly supported<strong>UDIM09</strong> through <strong>the</strong> activity DYNA (Ultrafast Structural Dynamics in Physics, Chemistry,Biology and Material Science).The European Science Foundation (ESF) was established in 1974 to create a common Europeanplatform for cross-border cooperation in all aspects <strong>of</strong> scientific research.With its emphasis on a multidisciplinary and pan-European approach, <strong>the</strong> Foundation provides<strong>the</strong> leadership necessary to open new frontiers in European science.Its activities include providing science policy advice (Science Strategy); stimulating cooperationbetween researchers and organisations to explore new directions (Science Synergy);and <strong>the</strong> administration <strong>of</strong> externally funded programmes (Science Management). These takeplace in <strong>the</strong> following areas: Physical and engineering sciences; Medical sciences; Life, earthand environmental sciences; Humanities; Social sciences; Polar; Marine; Space; Radioastronomy frequencies; Nuclear physics.Headquartered in Strasbourg with <strong>of</strong>fices in Brussels, <strong>the</strong> ESF’s membership comprises 75national funding agencies, research performing agencies and academies from 30 Europeannations.The Foundation’s independence allows <strong>the</strong> ESF to objectively represent <strong>the</strong> priorities <strong>of</strong> all<strong>the</strong>se members.


Journal <strong>of</strong>Modern OpticsCALL FOR PAPERSSpecial IssueUltra-Fast Dynamic ImagingGuest EditorsRaffaele Velotta — Università di Napoli, rvelotta@unina.itCarlo Altucci — Università di Napoli, caltucci@unina.itJournal <strong>of</strong> Modern OpticsEditorial BoardEditor:Jon Marangos — Imperial College London, UKAssociate Editor:William L. Barnes — University <strong>of</strong> Exeter, UKEditorial Board:G. S. Agarwal — Oklahoma State University, OK, USAS. M. Barnett FRS FRSE — University <strong>of</strong> Strathclyde, Glasgow,UKA. Beige — University <strong>of</strong> Leeds, UKK. Blow — Aston University, Birmingham, UKK. Burnett CBE FRS - University <strong>of</strong> Oxford, UKV. Buzek — Slovak Academy <strong>of</strong> Sciences, Bratislava, SlovakiaK. W. Cheah — Hong Kong Baptist University, Hong KongS. Enoch — Institut Fresnel, Marseille, FranceW. J. Firth FRSE — University <strong>of</strong> Strathclyde, Glasgow, UKA. Harvey — Heriot Watt University, Edinburgh, UKM. Ivanov — Steacie Institute for Molecular Sciences, CanadaP. L. Knight, KB, FRS — Imperial College London, UKV. Lakshminarayanan — University <strong>of</strong> Waterloo, Ontario, CanadaM. Padgett FRSE — University <strong>of</strong> Glasgow, UKF. Persico — University <strong>of</strong> Palermo, ItalyM. G. Raymer — University <strong>of</strong> Oregon, OR, USAI. Walmsley — University <strong>of</strong> Oxford, UKG. R.Welch — Texas A&M University, TX, USAE. Wolf — University <strong>of</strong> Rochester, NY, USAF. Wyrowski — University <strong>of</strong> Jena, Germanywww.tandf.co.uk/journals/jmoThe Guest Editors invite you tosubmit your papers for this specialissue <strong>of</strong> <strong>the</strong> Journal <strong>of</strong> Modern OpticsThis special issue aims to bring toge<strong>the</strong>r contributionsto ultrafast molecular imaging from researchersworking both with large scale facilities (synchrotronand free electron lasers) and with table top ultrashortsource. The following topics will be covered:••••••••AttoscienceHHG molecular imagingFEL and synchrotron researchNovel ultrafast spectroscopic techniquesUltrafast electron diffractionWavepacket motion and coherent control <strong>of</strong>reactionsKinetics <strong>of</strong> laser induced ChemistryUltrafast processes in BiologyDeadline for submissions: 31st July 2009Submission GuidelinesAll papers for consideration should besubmitted online at <strong>the</strong> Journal <strong>of</strong> ModernOptics Manuscript Central site at: http://mc.manuscriptcentral.com/tmop. Please includeon <strong>the</strong> title page that <strong>the</strong> paper is intended for<strong>the</strong> special issue “Ultra-Fast Dynamic Imaging”.More information is available at <strong>the</strong> Journalhomepage at www.tandf.co.uk/journals/jmounder <strong>the</strong> “Instructions for Authors” tab.Taylor & Francis | 4 Park Square | Milton Park | Abingdon | OX14 4RN | UK


Table <strong>of</strong> contentIntroduction 1Committees 2Conference program 3Abstracts 7List <strong>of</strong> participants 72


IntroductionUltra-Fast Dynamic Imaging <strong>of</strong> Matter has <strong>the</strong> aim to ga<strong>the</strong>r toge<strong>the</strong>r researchers working withaccelerator based light sources and ultrashort lasers. These two communities are experiencing a fastprogress in <strong>the</strong>ir fields with <strong>the</strong>ir interests converging towards <strong>the</strong> availability <strong>of</strong> femtosecond andsub-femtosecond light pulses which will make feasible <strong>the</strong> observation <strong>of</strong> physical and chemicalprocess in real time.Since <strong>the</strong> first meeting held in London, 9 th -11 th April 2006 <strong>the</strong>re has been significant progresstowards <strong>the</strong> goal <strong>of</strong> real time imaging <strong>of</strong> physical and chemical processes using both acceleratorbased sources (synchrotron sources, fourth generation light sources) and lasers. X-ray free-electronlasers are now being proposed in several countries and <strong>the</strong>se new machines are potentially capable<strong>of</strong> sub-10fs x-ray diffraction imaging on single bio-molecules. In parallel new laser basedtechniques, made possible by <strong>the</strong> advent <strong>of</strong> few-cycle amplified optical pulses, have recently beenadvanced that enable <strong>the</strong> access to sub-femtosecond (attosecond domain) imaging. These includetechniques based on attosecond XUV pulses generated by high order harmonic generation inmolecules and <strong>the</strong> direct probing <strong>of</strong> molecules using <strong>the</strong>ir own electrons driven under <strong>the</strong> influence<strong>of</strong> intense fields. It is <strong>the</strong>refore very timely to review in this second meeting on Ultra-Fast DynamicImaging <strong>of</strong> Matter <strong>the</strong> wide ranging advances that have been taking place across several differentfields in physics and chemistry. As it was <strong>the</strong> case for <strong>the</strong> first edition, <strong>the</strong> conference will attractboth <strong>the</strong> specialist practitioners <strong>of</strong> <strong>the</strong> techniques and <strong>the</strong> potential beneficiaries <strong>of</strong> <strong>the</strong>se ideas. Thisis a highly interdisciplinary topic with a broad interest to physicists, chemists, material scientistsand life-scientists. The purpose <strong>of</strong> <strong>the</strong> meeting will <strong>the</strong>refore be to bring toge<strong>the</strong>r leading membersfrom a number <strong>of</strong> diverse scientific communities that have been at <strong>the</strong> forefront in this area in recentyears. We hope that <strong>the</strong> cross-fertilisation between fields will promote fur<strong>the</strong>r research especially inareas <strong>of</strong> common interest.1


CommitteesInternational Advisory CommitteeRafael Abela (Swiss Light Source, Paul Scherrer Institut, Villigen, CH).Massimo Altarelli (DESY, Hamburg, DE)Paul Corkum (NRC Steacie Institute, Ottawa, CA)Louis DiMauro (Ohio State University, US)Roger Falcone (University <strong>of</strong> California, Berkeley, US)Misha Ivanov (NRC Steacie Institute, Ottawa, CA)Mauro Nisoli (Politecnico di Milano, IT)Marc Vrakking (Amolf FOM, Amsterdam, NL)Kiyoshi Ueda (Tohoku University, JP)Organising CommitteeCarlo Altucci (University <strong>of</strong> Naples, IT)Pietro Paolo Corso (University <strong>of</strong> Palermo, IT)Rosario Esposito (University <strong>of</strong> Naples, IT)Jonathan Marangos (Imperial College, UK)John Tisch (Imperial College, UK)Raffaele Velotta (University <strong>of</strong> Naples, IT)2


Conference ProgramWednesday 29 th April19:00 – 21:00 Ischia, Hotel Continental Terme, Registration & Welcome cocktailThursday 30 th April08:50 Opening RemarksMorning session: Attosecond Electron Dynamics I (Chair: R. Velotta)9.00 – 9.30 P. Abbamonte, Imaging attosecond electron dynamics in graphite and graphenewith inelastic X-ray scattering.9.30 – 10.00 R. Dörner, Interference and electron entanglement in photo-ionization <strong>of</strong> H 2 and N 2 .10.00 – 10.30 R. Kienberger, Attosecond physics.10.30 – 11.00 C<strong>of</strong>fee break.11.00 – 11.30 G. Sansone, Attosecond dynamics <strong>of</strong> electron wavepackets in atoms and molecules.11.30 – 12.00 O. Smirnova, Time and space resolved high harmonic imaging <strong>of</strong> electrontunnelling from molecules.12.30 - 13.30 LunchAfternoon session: Ultrafast Dynamics <strong>of</strong> Molecules I (Chair: A. L’Huillier)14.00 – 14.30 P. Corkum, A laser STM for molecules.14.30 – 15.00 H. Sakai, Controlling <strong>the</strong> molecular orientation in <strong>the</strong> laser-field-free condition.15.00 – 15.30 S. Baker, Probing molecular structure and dynamics using laser driven electronrecollisions.15.30 – 16.00 M. Lein, The phase in molecular high-harmonic generation.16.00 – 16.30 C<strong>of</strong>fee break.16.30 – 17.00 C. D. Lin, Quantitative rescattering <strong>the</strong>ory <strong>of</strong> dynamic chemical imaging withinfrared lasers.3


17.00 – 17.15 C. Vozzi, High order harmonics driven by IR parametric source.17.15 – 17.30 C. Figueira de Morisson Faria, Nonsequential double ionization in diatomicmolecules: one and two-centre rescattering17.30 – 17.45 M. Meckel, Laser-induced electron tunnelling and diffraction.17.45 – 18.00 R. de Nalda, Imaging real time bond breaking in molecules and clusters18.00 – 18.15 F. Lépine, Imaging electron dynamics in C 60 from femto- to microsecond timescale.18.15 – 18.30 E. Fiordilino, High-order harmonic generation from molecules: classical versusquantum effects.Friday 1 st MayMorning session: Ultrafast Dynamics <strong>of</strong> Molecules II (Chair: C. D. Lin)9.00 – 9.30 P. Salières, Experimental tomographic reconstruction <strong>of</strong> molecular orbitals usingHHG.9.30 – 10.00 H. Stapelfeldt, Quantum state selection <strong>of</strong> polar molecules: Alignment, orientationand conformational control.10.00 – 10.30 D. Villeneuve, Following molecular dynamics using high harmonic generation.10.30 – 11.00 C<strong>of</strong>fee break11.00 – 11.30 K. Ueda, Momentum imaging for ultrafast molecular imaging: from synchrotronradiation to femtosecond laser to XFEL.11.30 – 11.45 C. Pellegrini, X-ray Free-electron Lasers.11.45 – 12.00 J. Marangos, UK New Light Source (NLS).12.30 - 13.30 Lunch13.30 – 15.00 Poster sessionAfternoon session: Attosecond Electron Dynamics II (Chair: P. Corkum)15.00 – 15.30 J. Ullrich, Attosecond steering <strong>of</strong> electronic motion in atoms and molecules via ~6 fsCE phase stabilized pulses.15.30 – 16.00 K. L. Ishikawa, Wavelength dependence <strong>of</strong> high-harmonic generation.16.00 – 16.30 A. L’Huillier, Generation and application <strong>of</strong> attosecond pulse trains.4


16.30 – 16.45 V. Tosa, Macroscopic effects in single attosecond pulse generation.16.45 – 17.15 C<strong>of</strong>fee break.Afternoon session: Structural Dynamics <strong>of</strong> Complex Systems I (Chair: M. Chergui)17.15 – 17.45 S. Glenzer, Ultra-fast probing <strong>of</strong> shock-compressed matter with X-ray Thomsonscattering.17.45 – 18.00 D. Boschetto, Ultrafast dynamics and phase transition in photoexcited bismuthcrystal.18.00 – 18.15 P. Wochner, X-ray cross correlation analysis uncovers hidden local symmetries indisordered matter.18.15 – 18.30 B. Mansart, Ultrafast dynamical response <strong>of</strong> <strong>the</strong> prototype Mott compound V 2 O 3 .Saturday 2 nd MayMorning session: Structural Dynamics <strong>of</strong> Complex Systems II (Chair: S. Glenzer)9.00 – 9.30 J. Stohr, Ultrafast manipulation <strong>of</strong> <strong>the</strong> magnetization.9.30 – 10.00 H. Dürr, Ultrafast electron and spin dynamics in ferromagnets.10.00 – 10.30 J. Rost, Ultrafast electronic processes in clusters.10.30 – 11.00 M. Aeschlimann, Time-resolved photoemission electron microscopy -Nanoscale spectroscopy with femtosecond resolution11.00 – 11.30 C<strong>of</strong>fee break.11.30 – 12.00 M. Chergui, Optical and X-ray studies <strong>of</strong> <strong>the</strong> ultrafast dynamics <strong>of</strong> molecularsystems in liquids.12.00 – 12.30 D. Miller, “Making <strong>the</strong> Molecular Movie”: Quest for <strong>the</strong> structure-functioncorrelation <strong>of</strong> biology.12.30 – 13.00 I. P. Mercer, Quantum dimension <strong>of</strong> photosyn<strong>the</strong>sis revealed by powerful new lasertechnique.13.00 – 14.30 Lunch16.00 Boat trip around <strong>the</strong> island20.00 Social diner5


Sunday 3 rd MayMorning session: New Methods and Sources (Chair: J. Rossbach)9.00 – 9.30 K. Midorikawa, Water window X-ray generation by phase-matched high harmonicswith neutral media.9.30 – 10.00 S. Boutet, Linac coherent light source and single molecule imaging.10.00 – 10.30 J. Costello, Two colour and two photon ionization processes in intense EUV andoptical fields at “FLASH”.10.30 – 11.00 C<strong>of</strong>fee break.11.00 – 11.30 T. Tschentscher, Investigation <strong>of</strong> ultrafast structural changes in complex chemicalsystems using X-ray FELs.11.30 – 12.30 Round table discussion (coordinator: J. Marangos): Future Challenges andProspects for Ultra-Fast Dynamics Imaging.12.30 – 13.30 Lunch.6


Abstracts7


Thursday 30 th April9:00 – 12:00Morning session:Attosecond Electron Dynamics IChair: R. Velotta8


IMAGING ATTOSECOND ELECTRON DYNAMICS IN GRAPHITE ANDGRAPHENE WITH INELASTIC X-RAY SCATTERINGJames P. Reed 1 , Young Il Joe 1 , Bruno Uchoa 1 , Diego Casa 2 , Thomas Gog 2 , Yong Cai 3 ,and Peter Abbamonte 11 Frederick Seitz Materials Research Laboratory, University <strong>of</strong> Illinois, Urbana, IL, USA2 Advanced Photon Source, Argonne National Laboratory, Argonne, IL, USA3 NSLS II, Brookhaven National Laboratory, Upton, NY, USAX-ray scattering is a static imaging technique that has been widely applied to both periodicand non-periodic objects. The key technical challenge in x-ray imaging is to overcome <strong>the</strong> “phaseproblem”, i.e. to recover <strong>the</strong> missing phases that are lost because x-ray experiments measure anintensity, E 2 , ra<strong>the</strong>r than <strong>the</strong> electric field itself.In this talk I will describe a solution to <strong>the</strong> phase problem for inelastic x-ray scattering, thatallows dynamical imaging <strong>of</strong> charge propagation in a material 1,2 . The method is a four-stepprocedure involving i. symmetrization <strong>of</strong> <strong>the</strong> data, ii. analytic continuation, iii. a temporal sinetransform, and finally iv. a spatial Fourier transform. This technique yields <strong>the</strong> density propagator,χ( x, t) = −i / h 0 ˆ ρ( x, t), ˆ ρ(0,0) 0 θ ( t), which is a general measure <strong>of</strong> how charge propagates[ ]around a system.Our most recent use <strong>of</strong> this technique has been to image background screening processes ingraphite, with a time resolution <strong>of</strong> ∆t = 26 attoseconds and spatial resolution <strong>of</strong> ∆r = 0.53 Å. Thescreening is found to be extremely anisotropic, due to <strong>the</strong> existence <strong>of</strong> van Hove singularities near Land M points in Brillouin zone. From <strong>the</strong>se results we can extract <strong>the</strong> individual screeningproperties <strong>of</strong> <strong>the</strong> graphene layers. We have determined, among o<strong>the</strong>r things, a backgrounddielectric constant <strong>of</strong> ε graphene ~14, which potentially explains <strong>the</strong> absence <strong>of</strong> a divergence in <strong>the</strong>Fermi velocity near <strong>the</strong> Dirac points in graphene.1 P. Abbamonte, K. D. Finkelstein, M. D. Collins, and S. M. Gruner, Imaging density disturbances in water with a 41.3attosecond time resolution. Phys. Rev. Lett. 92, 237401 (2004).2 P. Abbamonte, et. al., Dynamical reconstruction <strong>of</strong> <strong>the</strong> exciton in LiF with inelastic x-ray scattering. Proc. Natl. Acad.Sci. 105, 12159 (2008).9


INTERFERENCE AND ELECTRON ENTANGLEMENT INPHOTOIONIZATION OF H 2 AND N 2M. Schöffler 1,2 , D. Akoury 1 , K. Kreidi 1 , T. Jahnke 1 , Th.Weber 2 , N. Neumann 1 , J. Titze 1 , L. Ph. H.Schmidt 1 , A. Czasch 1 , O. Jagutzki 1 , R.A. Costa Fraga 1 , R.E. Grisenti 1 , R. Diez Muino 3 , N.A.Cherepkov 4 , S.K. Semenov 4 , P. Ranitovic 5 , C.L. Cocke 5 , T. Osipov 2 , H. Adaniya 6 , J.C. Thompson 6 ,M.H. Prior 2 , A. Belkacem 2 , A. Landers 6 , H. Schmidt- Böcking 1R. Dörner 11 Institut ür Kernphysik, University Frankfurt,Max von Laue Str 1, D-60438 Frankfurt Germany2 Lawrence Berkeley National Lab., Berkeley CA 947203 Centro de Física de Materiales and Donostia InternationalPhysics Center, 20018 San Sebasian, Spain4 State University <strong>of</strong> Aerospace Instrumentation,190000 St. Petersburg, Russia5 Dept <strong>of</strong> Physics, Kansas State Univ, Cardwell Hall, Manhattan KS 66506\\5 Department <strong>of</strong> Physics, Auburn University Auburn AL 36849The talk will report on many particle coincident imaging experiments on direct double ionization <strong>of</strong>H 2 and innershell ionization followed by Auger decay <strong>of</strong> N 2 . Both electrons and both ions aremeasured in coincidence.For H 2 we show Thomas Young type double slit interference and how it is lost by electron-.electron correlations. This simple 4 body systems shows <strong>the</strong> first onset <strong>of</strong> <strong>the</strong> transition from <strong>the</strong>quantum to <strong>the</strong> classical world 1,2 .For innershell ionization <strong>of</strong> N 2 we find a surprising solution for <strong>the</strong> 30 year old puzzle <strong>of</strong> core holelocalization. We use <strong>the</strong> Auger electron as a ultrafast probe for <strong>the</strong> localized or delocalizedcharacter <strong>of</strong> <strong>the</strong> innershell hole. We show that and how localization arises from quantumentanglement <strong>of</strong> <strong>the</strong> photo and Auger electron. Depending on photon energy and direction <strong>of</strong> <strong>the</strong>photoelectron <strong>the</strong> Auger angular distribution shows broken or restored symmetry which directlyreflects <strong>the</strong> character <strong>of</strong> <strong>the</strong> innershell hole 3 .___________________________________1 Akoury et al. Science 318, 949 (2007)2 Kreidi at al. Phys.Rev.Lett. 100, 133005 (2008)3 Schöffler et al. Science 320, 920 (2008)10


ATTOSECOND PHYSICSR. KienbergerMax-Planck-Institut für Quantenoptik, Garching,Ludwig-Maximilians-Universität München, GermanyFundamental processes in atoms, molecules, as well as condensed matter are triggered or mediatedby <strong>the</strong> motion <strong>of</strong> electrons inside or between atoms. Electronic dynamics on atomic length scalestends to unfold within tens to thousands <strong>of</strong> attoseconds (1 attosecond [as] = 10 -18 s). Recentbreakthroughs in laser science are now opening <strong>the</strong> door to watching and controlling <strong>the</strong>se hi<strong>the</strong>rtoinaccessible microscopic dynamics.The key to accessing <strong>the</strong> attosecond time domain is <strong>the</strong> control <strong>of</strong> <strong>the</strong> electric field <strong>of</strong> (visible) light,which varies its strength and direction within less than a femtosecond (1 femtosecond = 1000attoseconds). Atoms exposed to a few oscillations cycles <strong>of</strong> intense laser light are able to emit asingle extreme ultraviolet (xuv) burst lasting less than one femtosecond 1,2 . Full control <strong>of</strong> <strong>the</strong>evolution <strong>of</strong> <strong>the</strong> electromagnetic field in laser pulses comprising a few wave cycles 3 have recentlyallowed <strong>the</strong> reproducible generation and measurement <strong>of</strong> isolated sub-femtosecond xuv pulses 4 ,demonstrating <strong>the</strong> control <strong>of</strong> microscopic processes (electron motion and photon emission) on anattosecond time scale. These tools have enabled us to visualize <strong>the</strong> oscillating electric field <strong>of</strong>visible light with an attosecond “oscilloscope” 5 , to control and probe single- and multi-electrondynamics in atoms 6,7 , molecules 8 and solids 9 . Recent experiments indicate <strong>the</strong> feasibility <strong>of</strong>extending to frontiers <strong>of</strong> attosecond metrology towards kiloelectronvolt photon energies 10 ,Megaelectronvolt electron energies 11 , and a temporal resolution approaching <strong>the</strong> atomic unit <strong>of</strong> time(~ 24 as) 12 .1 M. Hentschel et al., Nature 414, 509 (2001).2 R. Kienberger et al., Science 291, 1923 (2002).3 A. Baltuska et al., Nature 421, 611 (2003).4 R. Kienberger et al., Nature 427, 817 (2004).5 E. Goulielmakis et al., Science 305, 1267 (2004);6 M. Drescher et al., Nature 419, 803 (2002).7 M. Uiberacker et al., Nature 446, 627 (2007).8 M. Kling et al., Science 312, 246 (2006).9 A. Cavalieri et al., Nature 449, 1029 (2007).10 J. Seres et al, Nature 433, 596 (2005).11 L. Veisz et al., zur Veröffentlichung eingereicht (2008).12 E. Goulielmakis et al., Science 320, 1614 (2008).11


ATTOSECOND DYNAMICS OF ELECTRON WAVEPACKETSIN ATOMS AND MOLECULES.G. Sansone 1 , F. Kelkensberg 2 , M.F. Kling 3 , E. Benedetti 1 , F. Ferrari 1 ,W. Siu 2 , O. Ghafur 2 , P.Johnsson 2 , M. Swoboda 4 , T. Remetter 4 , F. Lépine 5 , S. Zherebtsov 3 , I. Znakovskaya 3 , M.Yu.Ivanov 6 , J.F. Pérez 7 , F. Morales 7 , J.L. Sanz-Vicario 8 , A. L'Huillier 4 , F. Martín 7 , M. Nisoli 2 andM.J.J. Vrakking 2 .1 National Laboratory for Ultrafast and Ultraintense Optical Science, Department <strong>of</strong> Physics,Politecnico <strong>of</strong> Milan, Piazza Leonardo da Vinci 32, 20133 Milano, Italy2 FOM-Institute AMOLF, Kruislaan 407, 1098 SJ Amsterdam, The Ne<strong>the</strong>rlands3 Max-Planck Institut für Quantenoptik, Hans-Kopfermann-Strasse 1, Garching, Germany4 Department <strong>of</strong> Physics, Lund University, P.O. Box 118, SE-221 00 Lund, Sweden5 Universit Lyon 1;CNRS;LASIM, UMR 5579, Villeurbane, France6 National Research Council <strong>of</strong> Canada, 100 Sussex Drive, Ontario K1A 0R6 Ottawa, Canada7 Departamento de Química, Universidad Autonoma de Madrid, 28049 Madrid, Spain8 GFAM, Instituto de Física, Universidad de Antioquia, AA1226 Medellín, ColombiaSingle attosecond pulses (SAP) are opening new perspectives in <strong>the</strong> control <strong>of</strong> chemical reaction as<strong>the</strong>y allow to steer <strong>the</strong> motion <strong>of</strong> electronic wave packets on <strong>the</strong>ir natural timescale 1 . In thiscontribution we report experimental evidences for <strong>the</strong> control <strong>of</strong> electron localization on H 2 and D 2molecules. In <strong>the</strong> experiment, SAP, with a bandwidth extending between 20 and 40 eV, wereproduced by carrier-envelope phase stabilized few-cycle pulse with a time dependent ellipticity.The pulses were used to initiate an ultrafast dynamics in H 2 and D 2 . Several states <strong>of</strong> <strong>the</strong> neutralmolecule (autoionizing states) or <strong>of</strong> <strong>the</strong> molecular ion (1sσ g and 2pσ u ) can be accessed due to <strong>the</strong>large bandwidth <strong>of</strong> <strong>the</strong> SAP. The subsequent electron dynamics was probed and controlled using asynchronized infrared few-cycle pulse with an intensity <strong>of</strong> I=3x10 12 W/cm 2 .The energy E and angular distribution <strong>of</strong> <strong>the</strong> D + and H + ions was measured using a velocity mapimaging spectrometer as a function <strong>of</strong> <strong>the</strong> delay τ between <strong>the</strong> pump and probe pulses. Thesignature <strong>of</strong> <strong>the</strong> different excitation mechanisms can be identified in <strong>the</strong> energy distribution <strong>of</strong> <strong>the</strong>ions. By changing <strong>the</strong> delay τ, <strong>the</strong> relative number <strong>of</strong> ions emitted in opposite direction can bevaried, indicating that electron dynamics can be steered by <strong>the</strong> probe beam during <strong>the</strong> moleculardissociation.1 F. Krausz and M. Ivanov Attosecond Physics Rev. Mod. Phys. 81, 163 (2009).12


TIME AND SPACE RESOLVED HIGH HARMONIC IMAGING OFELECTRON TUNNELING FROM MOLECULESOlga Smirnova 1,2 , Serguei Patchkovskii 2 , YannMairesse 2,4 , Nirit Dudovich 2,5 David Villeneuve 2 ,Paul Corkum 2 , and Misha Yu. Ivanov 2,31 Max-Born-Institute, Max-Born-Str. 2A, 12489 Berlin, Germany2 National Research Council, 100 Sussex Drive, Ottawa,Ontario K1A 0R6, Canada3 Imperial College <strong>of</strong> Science, Technology and Medicine, London SW7 2BW, United Kingdom4 CELIA, Universite Bordeaux I, UMR 5107 (CNRS, Bordeaux 1, CEA), 351 Cours de laLiberation, 33405 Talence Cedex, France5 Department <strong>of</strong> Physics <strong>of</strong> Complex Systems, Weizmann Institute <strong>of</strong> Science, Rehovot 76100,IsraelHigh harmonic generation in intense laser fields carries <strong>the</strong> promise <strong>of</strong> combining sub-Angstromspatial and attosecond temporal resolution <strong>of</strong> electronic structures and dynamics in molecules, seee.g 1,2,3 . High harmonic emission occurs when an electron detached from a molecule by an intenselaser field recombines with <strong>the</strong> parent ion 4 . Similar to Young's double-slit experiment,recombination to several 'lobes' <strong>of</strong> <strong>the</strong>same molecular orbital can produce interference minima and maxima in harmonic intensities 1 .These minima (maxima) carry structural information -- <strong>the</strong>y occur when <strong>the</strong> de-Broglie wavelength<strong>of</strong> <strong>the</strong> recombining electron matches distances between <strong>the</strong> centers. We demonstrate both<strong>the</strong>oretically and experimentally that amplitude minima (maxima) in <strong>the</strong> harmonic spectra can alsohave dynamical origin, reflecting multi-electron dynamics in <strong>the</strong> molecule. We use high harmonicspectra to record this dynamics and reconstruct <strong>the</strong> position <strong>of</strong> <strong>the</strong> hole left in <strong>the</strong> molecule afterionization. Experimental data are consistent with <strong>the</strong> hole starting in different places as <strong>the</strong>ionization dynamics changes from tunnelling to <strong>the</strong> multi-photon regime. Importantly, holelocalization and subsequent attosecond dynamics are induced even in <strong>the</strong> tunnelling limit. Thus,even 'static' tunnelling induced by a tip <strong>of</strong> a tunnelling microscope will generate similar attoseconddynamics in a sample. We anticipate that our approach will become standard in disentanglingspatial and temporal information from high harmonic spectra <strong>of</strong> molecules.1 M. Lein et al. Phys. Rev. Lett. 88, 183903 (2002).2 J. Itatani et al Nature 432 , 834 (2004).3 S. Baker et al Science 312 , 424 (2006).4 P.B. Corkum Phys. Rev. Lett. 71, 994 (1993).13


Thursday 30 th April14:00 – 18:45Afternoon session:Ultrafast Dynamics <strong>of</strong> Molecules IChair: A. L’Huillier14


A LASER STM FOR MOLECULESA. Staudte 1 , H. Akagi 2 , M Meckel 3 , L. Arissian 1,4 , C. Smeenk 1 ,F. Turner 1,5 , and P. B. Corkum 11 Joint Laboratory for Attosecond ScienceUniversity <strong>of</strong> Ottawa and National Research Council, Ottawa, ON. K1A 0R6 Canada;2 Japan Atomic Energy Agency,Tokai-mura, Naka-gun, Ibaraki 319-1195, Japan;3 Johann Wolfgang Goe<strong>the</strong> Universität, Max-von-Laue Straße 1, Frankfurt, Germany;4 Department <strong>of</strong> Physics, Texas A and M University, College Station, Texas, USA;5 Department <strong>of</strong> Physics, University <strong>of</strong> Waterloo, Waterloo, ON, CanadaTunnelling, one <strong>of</strong> <strong>the</strong> most fundamental manifestations <strong>of</strong> quantum mechanics, is apowerful platform from which technologies can be launched. Tunnelling allows surfaces to beimaged atom by atom and is <strong>of</strong>ten present in strong field science. In both solids and gases electronsescape from <strong>the</strong> outer regions <strong>of</strong> <strong>the</strong> orbital to <strong>the</strong> continuum, i.e. to <strong>the</strong> vacuum for multiphotonionization <strong>of</strong> gas phase molecules and to <strong>the</strong> conduction band <strong>of</strong> <strong>the</strong> metal-tip in STM. In an STM,a sharp tip is scanned across a metal surface to trace out <strong>the</strong> band structure <strong>of</strong> <strong>the</strong> solid. By analogy,rotating <strong>the</strong> molecule will trace out <strong>the</strong> structure <strong>of</strong> <strong>the</strong> highest occupied molecular orbital.Using O 2 and N 2 as examples, we show that <strong>the</strong> momentum distribution <strong>of</strong> <strong>the</strong> electron thatemerges from <strong>the</strong> tunnel is a filtered projection <strong>of</strong> <strong>the</strong> orbital from which it tunnelled.There is mounting evidence to suggest that lower lying levels contribute significantly to <strong>the</strong>total tunnelling probability in strong field experiments. The evidence arises from <strong>the</strong> structure <strong>of</strong>high harmonic spectrum, but <strong>the</strong> interpretation is debated. Using <strong>the</strong> “molecular STM”, we resolvethis debate. We study HCl since it <strong>of</strong>fers a second unique opportunity to isolate <strong>the</strong> tunnellingcontribution <strong>of</strong> <strong>the</strong> highest occupied molecular orbital (HOMO) from <strong>the</strong> one below (HOMO-1).Tunnelling from HOMO-1 s<strong>of</strong>tens <strong>the</strong> bond and, in <strong>the</strong> laser field, leads to fragmentation <strong>of</strong> <strong>the</strong>molecular ion. Hence, <strong>the</strong> break-up <strong>of</strong> an HCl molecule after ionization is a direct signature fortunnelling from a lower lying orbital.Our results show <strong>the</strong> asymmetry in tunnelling from hetero-nuclear molecules and confirmthat tunnelling naturally induces electron wave packet dynamics in <strong>the</strong> residual ion. They imply thatattosecond hole dynamics 1 , created by tunnelling, will be ubiquitous -- in atoms, molecules andsolids 2 .1 O. Smirnova, S. Patchkovskii, Y. Mairesse, N. Dudovich, D. Villeneuve, P. Corkum, and M. Y. Ivanov, “Time andSpace Resolved High Harmonic Imaging <strong>of</strong> Electron Tunnelling from Molecules”, submitted to Nature.2 M. Gertsvolf, H. Jean-Ruel, P. P. Rajeev, D. D. Klug, D. M. Rayner, and P. B. Corkum, “Orientation-DependentMultiphoton Ionization in Wide Band Gap Crystals”, PRL 101, 243001 (2008).15


CONTROLLING THE MOLECULAR ORIENTATIONIN THE LASER-FIELD-FREE CONDITIONHir<strong>of</strong>umi SakaiDepartment <strong>of</strong> Physics, Graduate School <strong>of</strong> Science, The University <strong>of</strong> Tokyo,7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, JapanWe have already realized both one- and three-dimensional molecular orientation with <strong>the</strong>combination <strong>of</strong> a weak electrostatic field and an intense, nonresonant laser field. 1,2,3 I will reportrecent progress in <strong>the</strong> control <strong>of</strong> molecular orientation.We propose an approach to achieve laser-field-free molecular orientation with <strong>the</strong> combination <strong>of</strong> aweak electrostatic field and an intense, nonresonant laser field with a rapid turn <strong>of</strong>f. 4 It is found that<strong>the</strong> adiabatically created pendular state is effectively transferred to <strong>the</strong> rotational wave packet in <strong>the</strong>nonadiabatic regime after <strong>the</strong> rapid turn <strong>of</strong> <strong>the</strong> laser pulse and that <strong>the</strong> orientation achieved at <strong>the</strong>peak <strong>of</strong> <strong>the</strong> laser pulse is revived at <strong>the</strong> rotational period <strong>of</strong> <strong>the</strong> molecule with <strong>the</strong> same degree <strong>of</strong>orientation. Based on this approach, we demonstrate laser-field-free orientation <strong>of</strong> OCS moleculeswith <strong>the</strong> combination <strong>of</strong> an electrostatic field <strong>of</strong> 800 V/cm and an intense, nonresonant rapidlyturned-<strong>of</strong>f laser field, which can be shaped with <strong>the</strong> plasma shutter technique. 5 As was expectedfrom <strong>the</strong>oretical simulations, molecular orientation is adiabatically created in <strong>the</strong> rising part <strong>of</strong> <strong>the</strong>laser pulse, and it is found to revive at around <strong>the</strong> rotational period <strong>of</strong> an OCS molecule with <strong>the</strong>same degree <strong>of</strong> orientation as that at <strong>the</strong> peak <strong>of</strong> <strong>the</strong> laser pulse in <strong>the</strong> virtually laser-field-freecondition. We fur<strong>the</strong>r propose a technique to achieve completely field-free molecular orientationwith an intense, nonresonant, two-colour laser field with a slow turn on and rapid turn <strong>of</strong>f. 6 Thetechnique is based on <strong>the</strong> combined effects <strong>of</strong> anisotropic hyperpolarizability interaction as well asanisotropic polarizability interaction. 71 H. Sakai, S. Minemoto, H. Nanjo, H. Tanji, and T. Suzuki, Phys. Rev. Lett. 90, 083001 (2003).2 S. Minemoto, H. Nanjo, H. Tanji, T. Suzuki, and H. Sakai, J. Chem. Phys. 118, 4052 (2003).3 H. Tanji, S. Minemoto, and H. Sakai, Phys. Rev. A 72, 063401 (2005).4 Y. Sugawara, A. Goban, S. Minemoto, and H. Sakai, Phys. Rev. A 77, 031403(R) (2008).5 A. Goban, S. Minemoto, and H. Sakai, Phys. Rev. Lett. 101, 013001 (2008).6 M. Muramatsu, M. Hita, S. Minemoto, and H. Sakai, Phys. Rev. A 79, 011403(R) (2009).7 T. Kanai and H. Sakai, J. Chem. Phys. 115, 5492 (2001).16


PROBING MOLECULAR STRUCTURE AND DYNAMICS USING LASERDRIVEN ELECTRON RECOLLISIONSS. Baker 1 , T. Siegel 1 , L. Brugnera 1 , R. Torres 1 , L. E. Chipperfield 1 , I. Procino 2 ,J. G. Underwood 2 , J. W. G. Tisch 1 , and J. P. Marangos 11 Quantum Optics and Laser Science, Department <strong>of</strong> Physics, Imperial College London, UK.2 Department <strong>of</strong> Physics and Astronomy, University College London, UK.The sub-cycle nature <strong>of</strong> high-harmonic generation (HHG) is <strong>of</strong> great interest due its potential toreveal correspondingly fast molecular dynamics. HHG has also been very successfully used as aprobe <strong>of</strong> molecular structure. It now seems possible that <strong>the</strong> nature <strong>of</strong> <strong>the</strong> electron collision mayalso be manipulated to enable more complete structural information to be obtained. Our group hasrecently conducted a number <strong>of</strong> experiments working towards <strong>the</strong> use <strong>of</strong> HHG to elucidatemolecular structure and attosecond dynamics.The PACER (probing attosecond dynamics by chirp-encoded recollision) technique, firstdemonstrated in 2006 1,2 , allowed <strong>the</strong> nuclear dynamics <strong>of</strong> H 2 , D 2 , CH 4 , and CD 4 followingionisation to be studied with a temporal resolution <strong>of</strong> 100as. More recently this technique has alsoallowed details <strong>of</strong> <strong>the</strong> electronic structure <strong>of</strong> <strong>the</strong> molecules used to be revealed 3 , through <strong>the</strong>observation <strong>of</strong> a dynamic interference effect in <strong>the</strong> recombination event. We have also beenworking towards to goal <strong>of</strong> using HHG to image <strong>the</strong> electronic structure <strong>of</strong> larger, organicmolecules 4 . Recent results investigating HHG in a range <strong>of</strong> molecules using a driving field at 1300nm will be presented. The use <strong>of</strong> a longer wavelength driving field is beneficial as <strong>the</strong> recollidingelectron wavepacket contains higher energy components, and can thus probe <strong>the</strong> molecule withgreater spatial resolution.This work will be presented here and <strong>the</strong> potential <strong>of</strong> <strong>the</strong>se techniques for fur<strong>the</strong>r developmentdiscussed.1 S. Baker et al. Probing proton dynamics in molecules on an attosecond timescale, Science 312, 424 (2006).2 M. Lein. Attosecond probing <strong>of</strong> vibrational dynamics with high-harmonic generation, Phys. Rev. Lett. 94, 053004(2005).3 S. Baker et al. Dynamic two-centre interference in High-order harmonic generation from molecules with attosecondnuclear motion, Phys. Rev. Lett. 101, 053901 (2008).4 R. Torres et al. Probing orbital structure <strong>of</strong> polyatomic molecules by High-order harmonic generation, Phys. Rev.Lett. 98, 203007 (2007).17


THE PHASE IN MOLECULAR HIGH-HARMONIC GENERATIONM. Lein 1,2 , E. V. van der Zwan 2 , C.C.Chirilă 1,21 Institute for Theoretical Physics, Leibniz Universität Hannover, 30167 Hannover, Germany2 Institute <strong>of</strong> Physics, Universität Kassel, 34132 Kassel, GermanyIn high-harmonic generation from molecules, <strong>the</strong> shape <strong>of</strong> <strong>the</strong> active electronic orbital plays acrucial role in determining <strong>the</strong> emission spectra as well as <strong>the</strong> orientation dependence <strong>of</strong> <strong>the</strong>harmonics from aligned molecules. In simple molecules, minima in <strong>the</strong> harmonic emission can beapproximately understood as a signature <strong>of</strong> destructive interference. At such minima, <strong>the</strong> phaseundergoes a measurable phase jump 1 . The details <strong>of</strong> <strong>the</strong> phase jump are important for <strong>the</strong> shape <strong>of</strong><strong>the</strong> produced attosecond pulses. It has been found <strong>the</strong>oretically and experimentally 2 that <strong>the</strong> jump isnot abrupt and <strong>the</strong> size <strong>of</strong> <strong>the</strong> jump differs from π. This cannot be explained in terms <strong>of</strong> a harmonicsignal passing exactly through zero. We investigate <strong>the</strong> phase jump using two different approaches:(i) <strong>the</strong> strong-field approximation for H 2 + using plane-wave matrix elements and (ii) numericalsolution <strong>of</strong> <strong>the</strong> time-dependent Schrödinger equation for 2D model systems. Both calculationssupport <strong>the</strong> conclusion that <strong>the</strong> width <strong>of</strong> <strong>the</strong> phase jump is due to a breakdown <strong>of</strong> <strong>the</strong> various saddlepointapproximations that are <strong>of</strong>ten adopted in <strong>the</strong> strong-field approximation. This effect is<strong>the</strong>refore related to <strong>the</strong> laser pulse parameters ra<strong>the</strong>r than to <strong>the</strong> molecular structure. Deviations <strong>of</strong><strong>the</strong> continuum electron states from plane waves, on <strong>the</strong> o<strong>the</strong>r hand, appear to be relevant mainly for<strong>the</strong> size <strong>of</strong> <strong>the</strong> phase jump. We discuss <strong>the</strong> implications for <strong>the</strong> Cooper minimum in <strong>the</strong> highharmonicemission spectrum from Argon atoms, where a phase jump appears as a consequence <strong>of</strong>destructive interference between different partial waves <strong>of</strong> <strong>the</strong> continuum electron.1 M. Lein et al., Role <strong>of</strong> <strong>the</strong> Intramolecular Phase in High-Harmonic Generation, Phys. Rev. Lett. 88, 183903 (2002).2 W. Boutu et al., Nature Phys. 4, 545 (2008).18


QUANTITATIVE RESCATTERING THEORY OF DYNAMIC CHEMICALIMAGING WITH INFRARED LASERSC. D. LinDepartment <strong>of</strong> Physics, Kansas State University, Manhattan, Kansas 66506, USABased on <strong>the</strong> rescattering concept, we have recently established 1-4 a quantitative rescattering <strong>the</strong>ory(QRS) where HATI (or HHG) spectra are expressed as a product <strong>of</strong> <strong>the</strong> returning electron wavepacket with <strong>the</strong> elastic differential cross sections (DCS) between <strong>the</strong> target ion with free electrons(or photo-recombination cross section). The QRS has been established for atomic targets based onaccurate results obtained from solving <strong>the</strong> time-dependent Schrödinger equation (TDSE). It has alsobeen fur<strong>the</strong>r established that <strong>the</strong> momentum distribution <strong>of</strong> <strong>the</strong> returning electron wave packet canbe obtained from <strong>the</strong> well-known Strong Field Approximation (SFA). According to <strong>the</strong> QRS, <strong>the</strong>structure is contained in <strong>the</strong> DCS or PRCS, <strong>the</strong> laser information is contained in <strong>the</strong> wave packet,i.e., <strong>the</strong>y are decoupled.The QRS has now been extended to calculate HHG spectra from aligned molecules to compare wi<strong>the</strong>xperiments. For atomic targets <strong>the</strong> QRS has been used to extract <strong>the</strong> DCS from <strong>the</strong> experimentalHATI spectra 5 , to predict and explain why <strong>the</strong> ATI spectra in <strong>the</strong> plateau region is flat or not 2 , andhow <strong>the</strong>y depend on laser parameters. We have also shown that <strong>the</strong> electron wave packet extractedfrom <strong>the</strong> QRS can be used to retrieve laser parameters 5 , such as <strong>the</strong> peak intensity, pulse durationand carrier-envelope phase, and to obtain nonsequential double ionization yield <strong>of</strong> atoms 6 . The QRSallows calculations <strong>of</strong> HATI and HHG spectra with accuracy comparable to that from TDSE, butwith computer time comparable to that <strong>of</strong> <strong>the</strong> SFA. Thus laser focus volume effect on <strong>the</strong> HATIspectra and macroscopic propagation effect on <strong>the</strong> HHG spectra can also be investigated<strong>the</strong>oretically.1 T. Morishita et al. Accurate retrieval <strong>of</strong> structural information from laser-induced photoelectron and high- orderharmonic spectra by few-cycle laser pulse. Phys. Rev. Lett. 100, 013902 (2008).2Z. J. Chen et al. Origin <strong>of</strong> species dependence <strong>of</strong> high-energy plateau photoelectron spectra. J. Phys. B 42, 061001(2009).3A. T. Le et al. Extraction <strong>of</strong> <strong>the</strong> species-dependent dipole ampitude and phase from high-order harmonic spectra inrare gas atoms. Phys. Rev. A 78, 023814 (2008).4A. T. Le et al. Theory <strong>of</strong> high-order harmonic generation from molecules with intense laser pulses. J. Phys. B 41,081002 (2008).5S. Micheau et al. Accurate retrieval <strong>of</strong> target structure and laser parameters <strong>of</strong> few-cycle pulses from photoelectronmomentum spectra. Phys. Rev. Lett. 102, 073001 (2009).6S. Micheau et al. Quantitative rescattering <strong>the</strong>ory for non-sequential double ionization <strong>of</strong> atoms by intense laserpulse. Phys. Rev. A 79, 013417 (2009).19


HIGH ORDER HARMONICS DRIVEN BY IR PARAMETRIC SOURCEC. Vozzi 1 , F. Calegari 1 , M. Nisoli 1 , G. Sansone 1 , S. De Silvestri 1 ,F. Frassetto 2 , L. Poletto 2 , P.Villoresi 2 , E. Balogh 3 , V. Tosa 3 , and S. Stagira 11 ULTRAS, CNR-INFM, Department <strong>of</strong> Physics, Politecnico di Milano, Italy2 LUXOR, CNR-INFM, Università di Padova, Italy3 Natl. Inst. RD Isotop & Mol. Technol, Cluj Napoca 400293, RomaniaWe investigated high-order harmonic generation (HHG) by carrier-envelope-phase stabilized fewcyclenear-IR parametric source in noble gases and simple molecules. This source is characterizedby 1500 nm central wavelength, almost transform limited pulse duration <strong>of</strong> about 20 fs and pulseenergy up to 1.2 mJ 1 . We observed a significant cut<strong>of</strong>f extension as compared to a standard 800 nmTi:Sapphire driving source for all <strong>the</strong>se generating media.We studied <strong>the</strong> dependence <strong>of</strong> spectral features on phase-matching condition in harmonicsgenerated in argon and krypton. These features are well reproduced by HH calculation 2 , taking intoaccount macroscopic effects.We also investigated HHG driven by two color laser field, obtained by mixing our parametricsource with a small portion <strong>of</strong> <strong>the</strong> fundamental 800 nm laser field. Exploiting <strong>the</strong> tunability <strong>of</strong> <strong>the</strong>parametric amplification process, we were able to change <strong>the</strong> carrier wavelength <strong>of</strong> <strong>the</strong> parametricsource. When harmonics are generated by two electric field components at 1600 and 800 nm, weobserved even and odd harmonic due to <strong>the</strong> break in <strong>the</strong> generation process symmetry. We observeda broad continuum extending above 100 eV when <strong>the</strong> parametric source is tuned at a carrierwavelength <strong>of</strong> 1500 nm which is not exactly double with respect to <strong>the</strong> 800-nm laser source,thus demonstrating <strong>the</strong> approach <strong>of</strong> Merdji et al. 3 for isolated attosecond pulse generation andextending this approach to <strong>the</strong> spectral region above 100 eV.1 C. Vozzi et al. “Millijoule-level phase-stabilized few-optical-cycle infrared parametric source” Opt. Lett. 32, 2957(2007).2 V. Tosa et al. “High-order harmonic generation by chirped and self-guided femtosecond laser pulses. I. Spatial andspectral analysis” Phys. Rev. A 71, 063807 (2005).3 H. Merdji et al. “Isolated attosecond pulses using a detuned second-harmonic field” Opt. Lett. 32, 3134 (2007).20


NONSEQUENTIAL DOUBLE IONIZATION IN DIATOMIC MOLECULES:ONE AND TWO-CENTRE RESCATTERING 1Figueira de Morisson FariaDepartment <strong>of</strong> Physics and Astronomy, University College London,Gower Street, London WC1E 6BT, United KingdomWe investigate laser-induced nonsequential double ionization from aligned diatomic molecules,using <strong>the</strong> strong-field approximation (SFA) in its length and velocity gauge formulations. Weconsider that <strong>the</strong> first electron dislodges <strong>the</strong> second by electron-impact ionization. Employingmodified saddle-point equations, we single out <strong>the</strong> contributions <strong>of</strong> different scattering scenarios to<strong>the</strong> maxima and minima observed in <strong>the</strong> differential electron momentum distributions. We showthat <strong>the</strong> quantum interference between <strong>the</strong> electron orbits starting and ending at a specific centre C jand those starting at C j and ending at a different centre C ν leads to <strong>the</strong> same maxima as minima as ifall possible scenarios are taken.There exist, however, quantitative differences as far as <strong>the</strong> gauge choice is concerned. Indeed, while<strong>the</strong> velocity-gauge distributions obtained employing only <strong>the</strong> above-mentioned processes arepractically identical to <strong>the</strong> overall distributions, <strong>the</strong>ir length-gauge counterparts exhibit anasymmetry in <strong>the</strong> positive and negative momentum regions. This asymmetry is due to additionalpotential-energy shifts, which are only present in <strong>the</strong> length-gauge formulation <strong>of</strong> <strong>the</strong> SFA.Depending on <strong>the</strong> centre, <strong>the</strong>se shifts sink or increase <strong>the</strong> potential barrier through which <strong>the</strong> firstelectron tunnels. In contrast, <strong>the</strong> interference between topologically similar scenarios leads at mostto patterns whose positions, in momentum space, do not agree with <strong>the</strong> overall interferencecondition, nei<strong>the</strong>r in <strong>the</strong> length nor in <strong>the</strong> velocity gauge.It is ra<strong>the</strong>r interesting that, in <strong>the</strong> length gauge, <strong>the</strong> influence <strong>of</strong> <strong>the</strong> potential energy shifts can bedirectly mapped into <strong>the</strong> electron momentum distributions for <strong>the</strong> processes starting at <strong>the</strong> samecentre. In fact, different potential energy shifts lead to an enhancement or a suppression <strong>of</strong> <strong>the</strong>distributions in distinct momentum regions. Hence, if <strong>the</strong>se processes could be isolated in a realisticscenario, one could in principle determine from which side <strong>of</strong> <strong>the</strong> molecule <strong>the</strong> first electronreached <strong>the</strong> continuum. If no asymmetry is observed, <strong>the</strong> existence <strong>of</strong> <strong>the</strong> potential-energy shifts and<strong>the</strong> validity <strong>of</strong> <strong>the</strong> length-gauge SFA electron momentum distributions could be ruled out fordiatomic molecules.1 C. Figueira de Morisson Faria, Laser-induced nonsequential double ionization in diatomic molecules: one and twocenterrescattering scenarios, arXiv: 0807.276321


LASER-INDUCED ELECTRON TNNELING AND DIFFRACTIONM. Meckel 1,2 , D. Comtois 3 , D. Zeidler 2,4 , A. Staudte 1,2 , D. Pavičić 2 , H. C. Bandulet 3 , H. Pépin 3 , J. C.Kieffer 3 , D. Dörner 1 , D. M. Villeneuve 2 , P. B. Corkum 21 Institut für Kernphysik, Johann Wolfgang Goe<strong>the</strong>-Universität, Frankfurt am Main, Germany2 Steacie Institute for Molecular Sciences, National Research Council, Ottawa, ON, Canada3 Institut National de la Recherche Scientifique – Énergie, Matériaux et Télécommunications,Varennes, QC, Canada4 Carl Zeiss SMT AG, Oberkochen, GermanyWe use a laser field to extract electrons from <strong>the</strong> molecule itself, accelerate <strong>the</strong>m, and in some casesforce <strong>the</strong>m to recollide with and diffract from <strong>the</strong> parent ion, all within a fraction <strong>of</strong> a laser period.The momentum distribution <strong>of</strong> <strong>the</strong> extracted electron carries <strong>the</strong> fingerprint <strong>of</strong> <strong>the</strong> highest occupiedmolecular orbital, whereas <strong>the</strong> elastically scattered electrons transmit <strong>the</strong> position <strong>of</strong> <strong>the</strong> nuclearcomponents <strong>of</strong> <strong>the</strong> molecule. 1We control <strong>the</strong> angular distributions <strong>of</strong> molecular axes at <strong>the</strong> instant <strong>of</strong> ionization by usingimpulsive molecular alignment 2 . The three-dimensional momentum vectors <strong>of</strong> emerging electronsand ions are recorded by a COLTRIMS reaction microscope 3 . A comparison <strong>of</strong> <strong>the</strong> electronmomentum distributions from aligned and anti-aligned molecules makes <strong>the</strong> above-mentionedeffects visible.Thus, in one comprehensive technology, <strong>the</strong> photoelectrons can give information about <strong>the</strong>electronic orbital and <strong>the</strong> position <strong>of</strong> <strong>the</strong> nuclei.1 M. Meckel et al., Laser-Induced Electron Tunneling and Diffraction, Science 320, 1478 (2008).2 E.g.: P. W. Dooley at al., Direct imaging <strong>of</strong> rotational wave-packet dynamics <strong>of</strong> diatomic molecules, Phys. Rev. A 68,023406 (2003).3 E.g.: J. Ullrich et al., Recoil-ion and electron momentum spectroscopy: reaction-microscopes, Rep. Prog. Phys. 66,1463 (2003).22


IMAGING REAL TIME BOND BREAKING IN MOLECULES ANDCLUSTERSR. de Nalda 1 , J. Durá 2 , J. G. Izquierdo 3 , G. Amaral 3 , L. Bañares 31 Instituto de Química Física Rocasolano, CSIC, C/ Serrano 119, 28006 Madrid, Spain2 Unidad Asociada Departamento de Química Física I, Facultad de Ciencias Químicas, UniversidadComplutense de Madrid. 28040 Madrid, Spain and Instituto de Estructura de la Materia, CSIC, C/Serrano, 123. 28006 Madrid, Spain3 Departamento de Química Física I, Facultad de Ciencias Químicas, Universidad Complutense deMadrid, 28040 Madrid, SpainIn this contribution, we show direct measurements <strong>of</strong> dissociation times <strong>of</strong> molecular bonds inpolyatomic molecules and clusters. The bond chosen is C⎯I in <strong>the</strong> CH 3 I molecule (or <strong>the</strong> (CH 3 I) ncluster), which presents rich dynamics when excited to its A-band in <strong>the</strong> ultraviolet. The dynamicsinvolves non-adiabatic crossings between electronic surfaces, and different degrees <strong>of</strong>vibrational/rotational excitation in <strong>the</strong> CH 3 fragment, with <strong>the</strong> result <strong>of</strong> a broad variety <strong>of</strong> channelsaccessed upon UV absorption. Those different channels are resolved by time-delayed ionization <strong>of</strong><strong>the</strong> fragments and spatially resolved detection in velocity-map configuration (i.e. complete map <strong>of</strong>velocity vectors resulting from <strong>the</strong> bond breaking process). We will show a dual use <strong>of</strong> thistechnique: a) combined with resonant, ultrafast probing, it works as a stopwatch, and it has allowedus to follow <strong>the</strong> rupture <strong>of</strong> this benchmark molecular bond in unprecedented detail, since <strong>the</strong>reaction times found for <strong>the</strong> different channels are directly related with <strong>the</strong> non-adiabatic dynamics<strong>of</strong> this multidimensional photodissociation reaction 1 ; b) combined with nonresonant, ultrafastprobing, it yields information on <strong>the</strong> transient species (and its potential surface) as it proceedstowards dissociation 2 . Additionally, we will show very recent results concerning <strong>the</strong> measurement<strong>of</strong> bond dissociation in (CH 3 I) 2 clusters. The study <strong>of</strong> <strong>the</strong> cluster introduces two types <strong>of</strong> novelties: asubtle one related to <strong>the</strong> bare molecule A-band being modified by <strong>the</strong> presence <strong>of</strong> a nearbymolecule, and novel dynamic channels related to new chemical rearrangements in <strong>the</strong> clusteredspecies. Evidence for both effects will be presented in this communication.________________________1 R. de Nalda, J. Durá, A. García-Vela, J. G. Izquierdo, J. González-Vázquez, and L. Bañares. J. Chem. Phys. 128,244309 (2008).2 J. Durá, R. de Nalda, J. Álvarez, J. G. Izquierdo, G. A. Amaral and L. Bañares. ChemPhysChem 9, 1245 (2008).23


IMAGING ELECTRON DYNAMICS IN C 60 FROM FS TO MICROSECONDTIMESCALE.Y. Huismans 1 , C. Cauchy 2 , E. Cormier 3 , P-A. Hervieux 4 , C. Bordas 2 , G. Gademann 1 , A.Gijsbertsen 1 , P. Logman 1 , F. Lépine 2 and M. Vrakking 1 ,1 AMOLF, FOM Amsterdam, The Ne<strong>the</strong>rlands2 LASIM, CNRS/Université Lyon 1, 69622 Villeurbanne, France3 CELIA, CEA Bordeaux, France4 IPCMS, CNRS/Université de Strasbourg, Strasbourg, Francelepine@lasim.univ-lyon1.frWe have used velocity map imaging spectrometry to study <strong>the</strong> influence <strong>of</strong> electronic andvibrational degrees <strong>of</strong> freedom on <strong>the</strong> ionization <strong>of</strong> photoexcited C 60 molecules. Thiscommunication presents experimental and <strong>the</strong>oretical results on <strong>the</strong> ionization processes <strong>of</strong> C 60occurring from femtosecond to microsecond timescale. The velocity distribution <strong>of</strong> <strong>the</strong> electronscarries direct information on <strong>the</strong> nature <strong>of</strong> <strong>the</strong> ionization process and <strong>the</strong>refore on <strong>the</strong> electrondynamics responsible for <strong>the</strong> ejection <strong>of</strong> <strong>the</strong> electron.When a short (30 fs) laser pulse ionizes C 60 , <strong>the</strong> electron spectrum is dominated by ATI peakswhich can be described by solving <strong>the</strong> Schrödinger equation. These measurements permit us to test<strong>the</strong> single active electron picture in <strong>the</strong> case <strong>of</strong> molecular strong field ionization and to look formolecular effects. Moreover, angle resolved photoelectron measurements allow us to disentanglecoherent ionization (ATI) from fast statistical electronic emission (<strong>the</strong>rmoelectronic). From thispoint <strong>of</strong> view velocity map imaging allows a clear distinction between coherent processes leading tohighly aligned electron emission, and statistical emission leading to isotropic emission. Aquantification <strong>of</strong> <strong>the</strong> loss <strong>of</strong> coherent can be obtained.When <strong>the</strong> laser pulse becomes much longer than <strong>the</strong> timescale <strong>of</strong> <strong>the</strong> vibronic couplings, <strong>the</strong>molecule can be considered as a reservoir <strong>of</strong> vibrationnal energy. The use <strong>of</strong> statistical <strong>the</strong>ory is<strong>the</strong>n fully justified. In that case, time-resolved imaging demonstrates <strong>the</strong> purely <strong>the</strong>rmionic nature<strong>of</strong> <strong>the</strong> process.Future experiments performed in <strong>the</strong> attosecond regime in order to access to <strong>the</strong> ultrafast electrondynamics will be discussed at <strong>the</strong> conference.24


HIGH-ORDER HARMONIC GENERATION FROM MOLECULES:CLASSICAL VERSUS QUANTUM EFFECTSE. Fiordilino, G. Castiglia, P.P. Corso, G. Orlando, F. PersicoDipartimento di Scienze Fisiche ed Astronomiche, Università <strong>degli</strong> Studi di Palermo, Via Archirafi36, 90123 Palermo and CNISMWe investigate High-Order Harmonic Generation from simple molecules and molecular ions; inparticular we are mainly interested on <strong>the</strong> effects <strong>of</strong> <strong>the</strong> nuclei dynamics on <strong>the</strong> emitted spectra.These effects are mainly related to both <strong>the</strong> appearance <strong>of</strong> satellite peaks around <strong>the</strong> usual oddharmonics and to an evident isotopic effect which allows to relate <strong>the</strong> intensity <strong>of</strong> <strong>the</strong> emitted linesto <strong>the</strong> mass <strong>of</strong> <strong>the</strong> isotopes. Fur<strong>the</strong>rmore we show that <strong>the</strong> presence <strong>of</strong> <strong>the</strong> satellite peaks isexplainable in terms <strong>of</strong> just a classical model <strong>of</strong> nuclei dynamics; on <strong>the</strong> contrary, <strong>the</strong> isotopic effectis only observable if we describe <strong>the</strong> nuclei as quantum objects. All <strong>the</strong> discussed results have beenobtained by numerically solving <strong>the</strong> time-dependent Schroedinger equations <strong>of</strong> <strong>the</strong> investigatedsystems.25


Friday 1 st May9:00 – 12:00Morning session:Ultrafast Dynamics <strong>of</strong> Molecules IIChair: C.D. Lin26


EXPERIMENTAL TOMOGRAPHIC RECONSTRUCTION OFMOLECULAR ORBITALS USING HHGS. Haessler 1 , W. Boutu 1 , P. Breger 1 , M. Stankiewicz 2 , L.J. Frasinski 2 , R. Taieb 3 , J. Caillat 3 , A.Maquet 3 , T. Ruchon 1 , B. Carré 1 and P. Salières 11 CEA-Saclay, Service des Photons, Atomes et Molécules, 91191 Gif sur Yvette, France2 J.J. Thomson Physical Laboratory, Univ. <strong>of</strong> Reading, Whiteknights, Reading RG6 6AF, UK3 UPMC Univ. Paris 06, UMR 7614, Laboratoire de Chimie Physique-Matière et Rayonnement, 11rue Pierre et Marie Curie, 75231 Paris Cedex 05, France.A strong laser field interacting with atoms or molecules drives ultrafast intra-atomic/molecularelectron wavepackets on a subfemtosecond timescale, resulting in <strong>the</strong> emission <strong>of</strong> attosecond bursts<strong>of</strong> XUV light. In linear molecules, <strong>the</strong> interaction <strong>of</strong> <strong>the</strong> laser-driven electron wavepacket with <strong>the</strong>core may lead to quantum interferences during <strong>the</strong> recombination step, as first proposed by Lein 1 . InBoutu 2 , we have characterized <strong>the</strong> attosecond emission from transiently-aligned CO 2 molecules andwe demonstrated that <strong>the</strong>se interferences can be finely controlled by turning <strong>the</strong> molecular axis withrespect to <strong>the</strong> laser polarization, i.e. changing <strong>the</strong> electron recollision angle. Our control <strong>of</strong> <strong>the</strong>interference results in an attosecond pulse shaping, useful for future applications in ultrafastcoherent control <strong>of</strong> atomic and molecular processes. Moreover our measurements give direct accessto <strong>the</strong> transition dipole matrix elements between <strong>the</strong> continuum states and <strong>the</strong> molecular orbitalsinvolved in <strong>the</strong> emission process. When <strong>the</strong> HOMO orbital gives <strong>the</strong> dominant contribution, Itatani 3proposed a tomographic reconstruction <strong>of</strong> <strong>the</strong> orbital within a plane wave approximation for <strong>the</strong>recolliding electron. We have performed a fully experimental reconstruction <strong>of</strong> <strong>the</strong> N 2 HOMO,where <strong>the</strong> polarization-resolved harmonic emission was characterized in amplitude and phase. Thisreconstruction exhibits Angström spatial resolution, mainly limited by <strong>the</strong> accessible spectral range.It also reveals <strong>the</strong> Coulombic character <strong>of</strong> <strong>the</strong> continuum waves (Haessler 4 ).1 M. Lein et al. Role <strong>of</strong> <strong>the</strong> intramolecular phase in high-harmonic generation. Phys. Rev. Lett. 88, 183903 (2002).2 W. Boutu et al. Coherent control <strong>of</strong> attosecond emission from aligned molecules. Nature Physics 4, 545 (2008).3 J. Itatani et al. Tomographic imaging <strong>of</strong> molecular orbitals. Nature 432, 867 (2004).4 S. Haessler et al. In preparation.27


QUANTUM STATE SELECTION OF POLAR MOLECULES:ALIGNMENT, ORIENTATION AND CONFORMATIONAL CONTROLHenrik Stapelfeldt 1 ,1 Department <strong>of</strong> Chemistry, University <strong>of</strong> Aarhus, DenmarkBuilding on ideas that go back to Stern in <strong>the</strong> 1920s we use an inhomogeneous static electric field todeflect a cold beam <strong>of</strong> polar molecules. The deflection spatially disperses <strong>the</strong> rotational quantumstates <strong>of</strong> <strong>the</strong> molecules. We show that <strong>the</strong> molecules residing in <strong>the</strong> lowest-lying rotational statescan be selected and used as targets for fur<strong>the</strong>r experiments 1 . In particular, <strong>the</strong> quantum-stateselectedmolecules enable unprecedented strong alignment, induced by a moderately intense laserpulse, as well as strong orientation induced by a mixed laser and static electric field. Here,alignment refers to confinement <strong>of</strong> one or more molecule-fixed axes along laboratory-fixed axes,and orientation refers to <strong>the</strong> molecular dipole moments pointing in a specific direction. Also, it isshown that <strong>the</strong> deflection enables separation <strong>of</strong> <strong>the</strong> different conformers <strong>of</strong> a single molecule. Theexample <strong>of</strong> 3-aminophenol will be discussed.We discuss new opportunities <strong>of</strong>fered by <strong>the</strong> enhanced degree <strong>of</strong> orientational control, madepossibly by quantum state selection, including time resolved studies <strong>of</strong> torsion, and eventuallyenantiomeric conversion, <strong>of</strong> axially chiral molecules.The work presented is done in collaboration with Jochen Küpper and Gerard Meijer, Fritz HaberInstitute, Berlin and Lars Bojer Madsen, Dept. <strong>of</strong> Physics, University <strong>of</strong> Aarhus.1 L. Holmegaard, J. H. Nielsen, I. Nevo, H. Stapelfeldt, F. Filsinger, J. Küpper, and G. Meijer Laser-Induced Alignmentand Orientation <strong>of</strong> Quantum-State-Selected Large Molecules, Phys. Rev. Lett. 102. 023001 (2009).28


FOLLOWING MOLECULAR DYNAMICSUSING HIGH HARMONIC GENERATIONDavid Villeneuve, Julien Bertrand, Paul Corkum and Hans Jakob WörnerNational Research Council <strong>of</strong> Canada, Ottawa ON CanadaHigh harmonic generation from molecules is known to be sensitive to <strong>the</strong> electronic structure <strong>of</strong> <strong>the</strong>molecule. We show that we can follow a unimolecular reaction in systems such as Br 2 and NO 2 . Asingle-photon pump pulse promotes <strong>the</strong> molecule to an excited electronic state, leading todissociation. The delayed probe pulse ionizes <strong>the</strong> molecule and creates high harmonic emission.By first aligning <strong>the</strong> molecule, it is possible to make <strong>the</strong> measurements in <strong>the</strong> molecular frame.Using a homodyne technique, we can determine both <strong>the</strong> amplitude and phase <strong>of</strong> <strong>the</strong> recombinationdipole matrix elements <strong>of</strong> <strong>the</strong> products along <strong>the</strong> complete reaction coordinate.High harmonic generation has many similarities to photoelectron spectroscopy since both involve atransition between a bound state and <strong>the</strong> continuum. We will compare <strong>the</strong> two approaches. HHG isa highly parallel measurement in which <strong>the</strong> photon energy, phase and polarization containinformation in <strong>the</strong> molecular frame, but has <strong>the</strong> disadvantage that <strong>the</strong> measurement takes place in astrong laser field.29


MOMENTUM IMAGING FOR ULTRAFAST MOLECULAR IMAGING:FROM SYNCHROTRON RADIATION TOFEMTOSECOND LASER TO XFELKiyoshi UedaIMRAM, Tohoku University, Sendai 8577, JAPANUsing position sensitive detectors in <strong>the</strong> ion time <strong>of</strong> flight (TOF) spectrometry, hit position on <strong>the</strong>detector allows one to determine <strong>the</strong> momentum particle by particle. In particular, <strong>the</strong> use <strong>of</strong> delayline detectors is a well-established method for multi-particle momentum imaging. This method hasbeen successfully applied to synchrotron radiation (SR) experiments to probe ultrafast deformation<strong>of</strong> <strong>the</strong> core excited Molecules. 1 A combination between ion momentum imaging and electronmomentum imaging, <strong>of</strong>ten called as reaction microscope, 2 has also been used for SR experimentsas a powerful tool for photoelectron diffraction measurements <strong>of</strong> free molecules, again as ultrafastprobing for <strong>the</strong> transient shape <strong>of</strong> <strong>the</strong> molecule. 3 These momentum imaging techniques are nowcommonly used also for femto-second laser experiments. Especially, one can probe electronic andmolecular structure <strong>of</strong> <strong>the</strong> target ion using rescattering electrons, 4 which may be called ultrafastlaser induced electron microscope (LIEM). In near future, X-ray free electron lasers (XFELs) willbe in operation for user experiments. These new light sources will provide us with newopportunities for ultrafast coherent X-ray imaging <strong>of</strong> a single large-scale molecule. The number <strong>of</strong>diffracted photons from a single molecule is, however, limited and additional information such as<strong>the</strong> orientation <strong>of</strong> <strong>the</strong> molecule is indispensable for retrieving <strong>the</strong> three dimensional structure <strong>of</strong> <strong>the</strong>molecule. Recently, we have developed a dead-time free detection system for ion momentumimaging and successfully used it to investigate multiple ionization <strong>of</strong> rare-gas clusters irradiated byextreme-ultraviolet FEL pulses from <strong>the</strong> SCSS test accelerator, 5 demonstrating that momentum foreach <strong>of</strong> more than one hundred ions produced by a single shot <strong>of</strong> FEL can be determined. 6,7 Webelieve that retrieval <strong>of</strong> <strong>the</strong> structure information from a coherent X-ray imaging <strong>of</strong> a singlemolecule become feasible if <strong>the</strong> dead-time detection system is used for determining <strong>the</strong> orientation<strong>of</strong> <strong>the</strong> molecule.1 K Ueda and J.H.D. Eland, J. Phys. B: At. Mol. Opt. Phys. 38, S839 (2005).2 J. Ullrich et al., Rep. Prog. Phys. 66, 1463 (2003).3 X,-J. Liu et al., Phys. Rev. Lett. 101, 109901 (2008).4 M. Okunishi et al., Phys. Rev. Lett. 100, 143001 (2008); D. Ray et al., Phys. Rev. Lett. 100, 143002 (2008).5 T. Shintake et al., Nature Photon. 2, 555 (2008).6 H. Fukuzwa et al., Phys. Rev. A Rap. Com. (in press).7 H. Iwayama et al., J. Phys. B: At. Mol. Opt. Phys. (accepted).30


X-RAY FREE-ELECTRON LASERSClaudio PellegriniDepartment <strong>of</strong> Physics and Astronomy, UCLA, 405 Hilgard Avenue, Los Angeles, California 90077.We review <strong>the</strong> present status and properties <strong>of</strong> X-ray free-electron lasers in operation or underconstruction in <strong>the</strong> nanometer and sub-nanometer wavelength range, and <strong>the</strong> novel possibilities <strong>the</strong>y<strong>of</strong>fer for <strong>the</strong> study <strong>of</strong> atomic and molecular processes. We also discuss recent developments inrelativistic electron beam physics, that give us <strong>the</strong> possibility <strong>of</strong> designing a new generation <strong>of</strong> X-ray free-electron lasers that: a. are more compact; b. reduce <strong>the</strong> radiation pulse duration to onefemtosecond or below; c. extend <strong>the</strong> photon energy to <strong>the</strong> 50 keV region. These results are obtainedby reducing <strong>the</strong> electron bunch charge while at same time maximizing <strong>the</strong> beam brightness andreducing <strong>the</strong> bunch length to a value near or smaller than <strong>the</strong> free-electron laser cooperation length.In <strong>the</strong> last case <strong>the</strong> radiation pulse is fully coherent in <strong>the</strong> longitudinal and transverse space. Theincrease in beam brightness can also be used to reduce <strong>the</strong> beam energy needed for a given radiationwavelength, when, at <strong>the</strong> same time, <strong>the</strong> undulator period is reduced. The simultaneous decrease inbeam energy and undulator period lead to a more compact free-electron laser, while <strong>the</strong> high beambrightness reduces <strong>the</strong> gain length and increases <strong>the</strong> coherent radiation intensity.31


UK NEW LIGHT SOUCESJon MarangosBlackett Laboratory, Imperial College <strong>of</strong> London, London SW7 2BW, United KingdomI will present a status report for <strong>the</strong> UK New Light Source (NLS) Project, based on advancedconventional and free electron lasers, with unique and world leading capabilities. The key sciencedrivers have been identified for this facility are:IMAGING NANOSCALE STRUCTURES.Instantaneous images <strong>of</strong> nanoscale objects can be recorded at any desired instant allowing,for example, nanometer scale resolution <strong>of</strong> sub-cellular structures in living systems.CAPTURING FLUCTUATING AND RAPIDLY EVOLVING SYSTEMS.Rapid intrinsic evolution and fluctuations in <strong>the</strong> positions <strong>of</strong> <strong>the</strong> constituents within mattercan be characterized.STRUCTURAL DYNAMICS UNDERLYING PHYSICAL AND CHEMICAL CHANGES.The structural dynamics governing physical, chemical and biochemical processes can befollowed by using laser pump- X-ray probe techniques.ULTRA-FAST DYNAMICS IN MULTI-ELECTRON SYSTEMS.New approaches to measuring <strong>the</strong> multi-electron quantum dynamics, that are present in allcomplex matter, will become possible.To address this science <strong>the</strong> following baseline specification has emerged for <strong>the</strong> facility:• High brightness (up to 10 12 photons/pulse) pulsed coherent light source coverage from THzto ~1keV (with harmonics to ~5 keV)• ~1kHz repetition rate with even pulse spacing• Photon source capable <strong>of</strong> smooth tuning across most <strong>of</strong> <strong>the</strong> spectral range• Pulse durations down to ~20 fs• Two-colour capability for pump probe experiments with synchronistaion jitter better than10fs. For example, Colour 1: THz- IR (pump)/ Colour 2: 100 eV-5 keV (probe)• High degree <strong>of</strong> transverse coherence• High degree <strong>of</strong> temporal coherence up to 400 eV, extending to >1 keV as seeding sourcesimprove• Synchronised to short pulsed lasers32


Friday 1 st May13:30 – 15:00Poster session33


P1AMPLITUDE AND PHASE OF THE HIGH HARMONIC RADIATIONIN ALIGNED MOLECULESJ. B. Bertrand, H. J. Wörner, D. M. Villeneuve, P. B. CorkumJoint Laboratory for Attosecond Science,National Research Council <strong>of</strong> Canada and University <strong>of</strong> Ottawa,100 Sussex Drive, Ottawa, ON, Canada K1A 0R6We use field-free alignment to generate harmonics in <strong>the</strong> molecular frame. In <strong>the</strong> same experiment,we perform a parallel measurement <strong>of</strong> <strong>the</strong> harmonic yield intensity and <strong>the</strong> ionization probability asa function <strong>of</strong> molecular alignment. The latter allows us to deconvolve <strong>the</strong> contribution <strong>of</strong> <strong>the</strong>ionization step in <strong>the</strong> high harmonic generation process, in <strong>the</strong> molecular frame. This is madepossible given <strong>the</strong> known degree <strong>of</strong> alignment achieved in <strong>the</strong> experiment 1 . Respectively, for N 2 andBr 2 molecules, we observe that <strong>the</strong> angular-dependent ionization probability reflects <strong>the</strong> σ g and π gcharacter <strong>of</strong> <strong>the</strong> highest occupied molecular orbital (HOMO). In a complimentary two-sourceinterferometry 2 experiment, we retrieve <strong>the</strong> phase <strong>of</strong> <strong>the</strong> harmonic radiation coming from alignedmolecules with respect to unaligned molecules. Particularly, a phase-shift around harmonic number17 is observed in Br 2 . By removing <strong>the</strong> measured contribution <strong>of</strong> <strong>the</strong> ionization step, we obtain acomplete map <strong>of</strong> <strong>the</strong> dipole amplitude and phase in <strong>the</strong> molecular frame. 11 D. Pavicic et al, Phys. Rev. Lett. 98, 243001 (2007).2C. Corsi et al, Phys. Rev. Lett. 97, 023901 (2006).34


P2SCALING OF HIGH HARMONIC GENERATION EFFICIENCYWITH WAVELENGTHAndrew D. Shiner 1 , Carlos Trallero-Herrero 1 , Nathaniel Kajumba 1 ,Heidi-C Bandulet 2 , Daniel Comtois 2 , François Légaré 2 , and Jean-Claude Kieffer 2 ,Paul B. Corkum 1 and David M. Villeneuve 11 National Research Council <strong>of</strong> Canada, Ottawa, Canada2 INRS- Energie, Materiaux et Telecommunications, Varennes, QC, CanadaHigh Harmonic Generation (HHG) is an efficient process for producing radiation at XUVwavelengths. Higher XUV photon energies can be reached through this process by increasing <strong>the</strong>driving laser wavelength; however, this comes at <strong>the</strong> expense <strong>of</strong> harmonic yield. The scaling <strong>of</strong>XUV yield with laser wavelength remains an active area <strong>of</strong> investigation both <strong>the</strong>oretically 1,2 andexperimentally 3 .We present measurements <strong>of</strong> <strong>the</strong> scaling <strong>of</strong> XUV yield on laser wavelength for wavelengths from800 nm to 1.8 um. We operate with a thin (0.5 mm), low-density gas sample so that phase matchingis not influenced by plasma or material dispersion. The observed quadratic increase in harmonicyield with increasing pressure confirms that our measurement is not influenced phase mismatch. Inall cases we maintain a constant focal volume as we change wavelength by imaging <strong>the</strong> output <strong>of</strong> aspatial filter into <strong>the</strong> gas jet. The harmonic yield is measured with an XUV spectrometer. An iondetector located below <strong>the</strong> jet simultaneously records <strong>the</strong> ionization current. The linear dependence<strong>of</strong> <strong>the</strong> ionization current on jet backing pressure proves that this signal is proportional to <strong>the</strong> number<strong>of</strong> ions produced in <strong>the</strong> sample. We determine <strong>the</strong> harmonic yield per emitter by dividing <strong>the</strong> HHGspectrum by <strong>the</strong> square <strong>of</strong> <strong>the</strong> ion current. This measurement allows us to extract <strong>the</strong> single atomresponse. The resulting scaling laws for Kr and Xe will be presented which are found to be in goodagreement with current <strong>the</strong>ories 50 .1 J. Tate et al. Scaling <strong>of</strong> Wave-Packet Dynamics in an Intense Midinfrared Field. Phys. Rev. Lett., 98, 13901 (2007).2 K. Schiessl et al. Quantum Path Interference in <strong>the</strong> Wavelength Dependence <strong>of</strong> High-Harmonic Generation. Phys.Rev. Lett. 99, 253903 (2007).3 P. Colosimo et al. Scaling strong-field interactions towards <strong>the</strong> classical limit. Nature Phys, 4, 386-389 (2008).35


P3ATTOSECOND HOMODYNE INTERFEROMETRY OF A CHEMICALREACTIONH. J. Wörner, J. B. Bertrand, P. B. Corkum and D. M. VilleneuveJoint laboratory for attosecond science,National Research Council <strong>of</strong> Canada and University <strong>of</strong> Ottawa,100, Sussex Drive, Ottawa, ON, Canada K1A0R6High-harmonic generation in aligned molecules provides information about <strong>the</strong>ir electronicstructure and ionization continuum within a fraction <strong>of</strong> a laser cycle. We exploit <strong>the</strong> ultrahigh timeresolution to observe a chemical reaction <strong>of</strong> fixed-in-space molecules. The experiment proceeds inthree steps: non-adiabatic alignment, impulsive excitation and high harmonic generation. We use<strong>the</strong> photodissociation <strong>of</strong> Br 2 in a pro<strong>of</strong>-<strong>of</strong>-principle experiment. The transient interference <strong>of</strong> highharmonics generated by <strong>the</strong> ground and <strong>the</strong> excited states results in a high visibilty <strong>of</strong> <strong>the</strong>photodissociation process on <strong>the</strong> femtosecond time scale. The variation <strong>of</strong> <strong>the</strong> observed signal withharmonic order provides dynamic information on <strong>the</strong> attosecond time scale. We develop ahomodyne technique that enables us to extract <strong>the</strong> harmonic amplitude and phase <strong>of</strong> <strong>the</strong> excitedstate undergoing dynamics. Molecular frame information on <strong>the</strong> evolution <strong>of</strong> <strong>the</strong> electronic structurealong <strong>the</strong> dissociation coordinate and <strong>the</strong> associated ionization continuum is <strong>the</strong>reby obtained. Theresults indicate that <strong>the</strong> coherence <strong>of</strong> <strong>the</strong> atomic fragments manifests itself for very largeinternuclear separations. These experiments pave <strong>the</strong> way towards dynamic orbital tomography - amovie <strong>of</strong> <strong>the</strong> orbitals undergoing a chemical reaction.36


P4THE DEVELOPMENT OF AN ULTRAFAST LABORATORY AT DCU:A PROGRESS REPORTT. J. Kelly, P. Hayden and J. T. Costello1 National Centre for Plasma Science and TechnologySchool <strong>of</strong> Physical SciencesDublin City UniversityGlasnevinDublin 9The field <strong>of</strong> ultrafast science has been revolutionised in recent years by <strong>the</strong> developmentsurge in femtosecond laser technology which now permits unprecedented control over keyparameters such as amplitude, polarisation, frequency, phase and carrier envelope phase 1,2 . Thegeneration <strong>of</strong> coherent EUV radiation via <strong>the</strong> process <strong>of</strong> high harmonic generation or HHG 3 hasalso developed rapidly in parallel over <strong>the</strong> last three decades and even attosecond pulses may beproduced 4 . Hence it is now possible to prepare and probe atoms, molecules and o<strong>the</strong>r smallquantum systems in variously intense and/or coherent multicolour fields stretching from <strong>the</strong> NIR to<strong>the</strong> EUV.An ultrafast laboratory is nearing completion at DCU with a laser capable <strong>of</strong> producingpulses with widths as short as 30 fs in a wavelength range from 267 nm to 2 µm. A multiplicity <strong>of</strong>electron, ion and photon detection techniques will be employed in coherent time resolved EUV +optical laser ionization and fragmentation <strong>of</strong> atoms and molecules. A report <strong>of</strong> <strong>the</strong> progress to dateand planned experiments will be presented.________________________1 Cavalieri AL, Goulielmakis E, Horvath B, Intense 1.5-cycle near infrared laser waveforms and <strong>the</strong>ir use for <strong>the</strong>generation <strong>of</strong> ultra-broadband s<strong>of</strong>t-x-ray harmonic continua New Journal <strong>of</strong> Physics, Vol: 9, 242(2007)2 Brixner T, Krampert G, Pfeifer T, Selle R, Gerber G, Wollenhaupt M, Graefe O, Horn C, Liese D, Baumert T,Quantum control by ultrafast polarization shaping, Physical Review Letters, Vol: 92, 20(2004)3 M Ferray et al, Multiple Harmonic Conversion <strong>of</strong> 1064 nm radiation in rare- gases J. Phys. B: At. Mol. Opt. Phys.21(1988)4 Corkum PB, Krausz F, Attosecond Science, Nature Physics, Vol: 3, 381(2007)37


P5PROBING THE MOLECULAR ROTO-VIBRATIONALDYNAMICS EXCITED IN OPTICAL FILAMENTATIONF. Calegari, C. Vozzi, S. De Silvestri, S. StagiraNational Laboratory for Ultrafast and Ultraintense Optical Science, CNR – INFM ,Dipartimento di Fisica, Politecnico di Milano, I-20133, Milano, ItalyOptical filamentation in molecular gases shows peculiar features with respect to analogousphenomena in atomic media, owing to <strong>the</strong> occurrence <strong>of</strong> rotational and vibrational molecularexcitation. Indeed spatio-temporal effects, ascribed to <strong>the</strong> rotational Raman response, have beenrecently demonstrated in <strong>the</strong> wake <strong>of</strong> an optical filament excited in N 2 1 . The study <strong>of</strong> vibrationaleffects in filamentation is, on <strong>the</strong> o<strong>the</strong>r hand, at an early stage 2 .In this work we investigate <strong>the</strong> roto-vibrational excitation <strong>of</strong> a molecular medium induced byfilamentation <strong>of</strong> an ultrashort laser pulse. A first pump pulse (10 fs) was focused in a gas cellgenerating a filament which induced <strong>the</strong> roto-vibrational excitation in <strong>the</strong> molecular sample. Asecond pulse (10 fs) was used to probe <strong>the</strong> effects occurring in <strong>the</strong> filament wake. The central part<strong>of</strong> <strong>the</strong> two beams was sent to a spectrometer, which was used to record <strong>the</strong> UV tail <strong>of</strong> <strong>the</strong> spectrumas a function <strong>of</strong> <strong>the</strong> pump-probe delay.A first set <strong>of</strong> experiments was performed in CO 2 . The acquired pump-probe trace shows a beatbetween two modes at 1285.4 cm -1 and 1388.15 cm -1 . This beat demonstrates <strong>the</strong> excitation <strong>of</strong> <strong>the</strong>so-called Fermi doublet. Moreover, <strong>the</strong> Fourier analysis reveals <strong>the</strong> presence <strong>of</strong> hot bands aroundthis two modes, which suggests that overtone excitation must also be considered in ourexperimental conditions. Similar experiments have been performed also in H 2 . The acquired signalpresents a complex evolution indicating <strong>the</strong> roto-vibrational excitation <strong>of</strong> <strong>the</strong> molecules. Theexcitation <strong>of</strong> <strong>the</strong> very fast stretching mode <strong>of</strong> H 2 (4152 cm -1 ) demonstrates that during opticalfilamentation <strong>the</strong> pump pulse becomes self-compressed down to a pulse duration which enablesISRS <strong>of</strong> this Raman active mode.1 F. Calegari et al. Rotational Raman effects in <strong>the</strong> wake <strong>of</strong> optical filamentation Phys. Rev. Lett. 100, 123006 (2008).2 F. Calegari et al. Molecular rotovibrational dynamics excited in optical filamentation, Opt. Lett. 33, 2922 (2008).38


P6FEMTOSECOND STUDIES OF THE PHOTODISSOCIATION OF CH 3 I VIATHE B-BANDG. Gitzinger 1 , M.E. Corrales 2 , J. Durá 3 , G.A. Amaral 2 , R. de Nalda 1 , L. Bañares 21 Instituto de Química Física Rocasolano, CSIC, C/ Serrano, 119. 28006 Madrid, Spain2 Departamento de Química Fisica I, Facultad de Ciencias Químicas, Universidad Complutense deMadrid. 28040 Madrid, Spain3 Unidad Asociada Departamento de Química Física I, Facultad de Ciencias Químicas,Universidad Complutense de Madrid. 28040 Madrid, Spain and Instituto de Estructura de laMateria, CSIC, C/ Serrano, 123. 28006 Madrid. SpainFemtosecond CH 3 I photodissociation experiments via <strong>the</strong> B-band were carried out by <strong>the</strong> velocitymap imaging (VMI) technique using one photon excitation (“pump” laser centered at 200 nm) andion detection <strong>of</strong> CH 3 fragments by resonance enhanced multiphoton ionization (REMPI) with atime-delayed “probe” laser beam in <strong>the</strong> wavelength range 325-334 nm. The initial excitation leaves<strong>the</strong> parent CH 3 I molecule in an excited 6s[1] Rydberg state with one vibrational quantum in <strong>the</strong> ν 6mode (CH 3 “rocking”) 1 . It is well known that at this wavelength two photodissociation channels arepossible. After predissociation from <strong>the</strong> Rydberg state, both channels lead to <strong>the</strong> formation <strong>of</strong>ground state CH 3 , but one <strong>of</strong> <strong>the</strong>m produces I in its ground state ( 2 P 3/2 ) while <strong>the</strong> second oneproduces I in <strong>the</strong> spin orbit excited state ( 2 P 1/2 ). Some controversy has arisen at <strong>the</strong>se excitationwavelengths with some authors claiming that <strong>the</strong> photodissociation proceeds entirely via <strong>the</strong> secondchannel 2 , while o<strong>the</strong>rs have also detected <strong>the</strong> first channel with a quantum yield <strong>of</strong> up to 0.32 3 .In this work, we have been able to detect <strong>the</strong> formation <strong>of</strong> vibrationless CH 3 (ν=0) fragments as wellas vibrationally excited CH 3 in <strong>the</strong> ν 1 (CH stretch) and ν 2 (umbrella) modes. In all cases <strong>the</strong>dissociation proceeds entirely via <strong>the</strong> CH 3 +I( 2 P 1/2 ) channel. Our technique is sensitive to <strong>the</strong> spatialdistribution <strong>of</strong> <strong>the</strong> fragments; thus we have measured <strong>the</strong> anisotropy parameter for all types <strong>of</strong> CH 3 ,which corresponds in all cases to a perpendicular transition with β ∼ -0.8. Finally, our time resolvedexperiments have shown that <strong>the</strong> formation <strong>of</strong> ground state CH 3 as well as vibrationally excited CH 3occurs within similar subpicosend timescales.1 A.P. Baronvaski and J.C. Owrutksy. Vibronic dependence <strong>of</strong> <strong>the</strong> B State lifetimes <strong>of</strong> CH 3 I and CD 3 I usingfemtosecond photoionization spectroscopy. J. Chem. Phys. 108, 3445 (1998).2 G.N.A Van Veen et al. Predissociation <strong>of</strong> specific vibrational states in CH 3 I upon excitation around 193.3 nm.Chem. Phys. 97, 179 (1985).3 A. Gilchrist et al. Methyl Iodide photodissociation at 193 nm: The I(P) quantum yield. J. Phys. Chem. A. 112,4531 (2008).39


P7ULTRAFAST TABLETOP EXAFS: THE WAY TOWARDS DIRECTOBSERVATION OF MOLECULAR STRUCTURAL CHANGESJens Uhlig, Niklas Gador, Wilfred Fullagar and Villy SundströmDepartment <strong>of</strong> Chemical Physics, Lund University, Box 124, 22100 Lund, SwedenJens.Uhlig@chemphys.lu.sePhotochemistry and dynamics <strong>of</strong> molecules in nature and artificial systems is <strong>of</strong> enormouscontemporary interest. A small selection <strong>of</strong> applications includes solar cells, artificialphotosyn<strong>the</strong>sis, photosensors, photostimulated chemistry and organic light emitting diodes (OLED).Direct real-time observation <strong>of</strong> molecular structural changes in <strong>the</strong>se systems is highly desirable.Massive efforts are underway at large scale accelerator and laser facilities to generate and detectsuitably short bursts <strong>of</strong> X-rays for this purpose. This poster presents a novel table-top arrangementfor subpicosecond time resolved X-ray absorption measurements in a conventional laser laboratory.Our laser plasma X-ray generator produces isotropic bremsstrahlung bursts with detectable energiesin <strong>the</strong> range 3 – 15 keV from a simply constructed water jet target. Measurements suggest an X-raypulse duration <strong>of</strong> 400 fs or shorter. The spectrum is free from detectable emission lines, importantfor temporal and detection reasons.Moderate power ultrafast kHz repetition lasers in modern laboratories yield enough X-ray flux toenable resolution <strong>of</strong> local molecular structures within practical timeframes using <strong>the</strong> EXAFStechnique, when coupled to suitable detection systems. A helium or rough vacuum environmentallows a variety <strong>of</strong> liquid or solid samples without <strong>the</strong> constraints <strong>of</strong> high vacuum systems.We suggested and are poised to pioneer <strong>the</strong> use <strong>of</strong> a novel single photon mode micro calorimeterdetector array with sufficient energy resolution to allow EXAFS measurements directly. Thisdevelopment arises from extensive work with direct detection CCDs, bent crystal (focusing vonHamos) spectrometers, synchrotron EXAFS experiments and laser/X-ray characterisations. Themicro calorimeters <strong>of</strong>fer energy resolution <strong>of</strong> ~4eV @ 6keV in a compact setup that does notmotivate higher fluxes than are already observed. The development is expected to enable EXAFSin widespread laser laboratories, with particular applications in <strong>the</strong> context <strong>of</strong> ultrafast structuraldynamics.40


P8VELOCITY MAP IMAGING OF HIGH ENERGY ELECTRONSD. C. Darios 1 , I. Procino 2 , M. Siano 1 , S. Baker 1 , R. Torres 1 , J.G. Underwood 2 and J. P. Marangos 11 Blackett Laboratory, Imperial College <strong>of</strong> London, London SW7 2BW, United Kingdom2 Department <strong>of</strong> Physics and Astronomy, University College London, London WC1E 6BT, UKVelocity Map Imaging (VMI) is a powerful experimental technique that allows directmeasurement <strong>of</strong> a two-dimensional (2D) projection <strong>of</strong> <strong>the</strong> velocity distribution <strong>of</strong> a phot<strong>of</strong>ragment.The VMI technique 1 is widely used because <strong>of</strong> its ease <strong>of</strong> use and excellent collection efficiency.We have developed a VMI spectrometer to study (high energy, up to 600 eV) electron rescatteringprocesses that occur when an atom/molecule is subjected to a strong laser field. The sameinstrument can also characterize <strong>the</strong> degree <strong>of</strong> laser induced alignment by observing <strong>the</strong> momentumdistribution <strong>of</strong> Coulomb exploded fragments.Our VMI spectrometer is equipped with three high voltage (up to 15 kV) electrostatic lensesthat direct <strong>the</strong> electrons/ions trajectories into a 15 cm long field-free time <strong>of</strong> flight tube towards amicrochannel plate detector followed by a phosphor screen. We use a commercial Titanium-Sapphire chirp-pulsed amplified (CPA) laser system operating at 1 kHz and producing pulses wi<strong>the</strong>nergy <strong>of</strong> 2.5 mJ and durations <strong>of</strong> ~45±5 fs. Intense and ultrashort laser pulses with duration <strong>of</strong>12.5±0.5 fs and energy up to 500 µJ are generated in a hollow-fibre pulse compression system thatis implemented at <strong>the</strong> output <strong>of</strong> our laser system.The pump beam aligns <strong>the</strong> molecules and <strong>the</strong>n <strong>the</strong> intense and short probe pulse causesCoulomb explosion <strong>of</strong> <strong>the</strong> molecules. A pump-probe experiment in ion VMI configuration is firstused to characterize <strong>the</strong> degree <strong>of</strong> alignment in <strong>the</strong> molecules. The ion image contains informationon both <strong>the</strong> angular distribution and <strong>the</strong> kinetic energy <strong>of</strong> <strong>the</strong> fragments through <strong>the</strong> radialdistribution. We are also implementing <strong>the</strong> experimental observation <strong>of</strong> high energy electronsrescattering in atoms and/or diatomic molecules. If <strong>the</strong> momentum distribution <strong>of</strong> <strong>the</strong> rescatteredelectrons resulting from ionisation by <strong>the</strong> 12.5 fs pulse can be resolved with <strong>the</strong> VMI spectrometer,information <strong>of</strong> <strong>the</strong> molecular structure is gained without <strong>the</strong> need for numerical reconstruction.Finally, VMI spectrometers are easier to implement compared to COLTRIMS 2 apparatus andprovide high quality data.1 A. T. J. B. Eppink et al., Velocity map imaging <strong>of</strong> ions and electrons using electrostatic lenses: Application inphotoelectron and phot<strong>of</strong>ragment ion imaging <strong>of</strong> molecular oxygen, Review <strong>of</strong> scientific Instruments 68, 3477-3484(1997)2 M. Meckel, Laser-Induced Electron Tunneling and Diffraction, Science 320, 1478-1482 (2008)41


P9DEVELOPMENT OF AN ALGORITHM TO RETRIEVE 3DDISTRIBUTIONS IN A NON-CYLINDICAL SYMMETRIC VELOCITY MAPIMAGING SYSTEMI. Procino 1 , D. Darios 2 , S. Baker 2 , J. Underwood 1 , J. Marangos 21 Department <strong>of</strong> Physics and Astronomy, University College London, London WC1E 6BT, UK2 Blackett Laboratory, Imperial College London, London SW7 2BW, UKMeasurements on gas phase molecules performed on an isotropic sample suffer an averaging overall molecular orientations resulting in a loss <strong>of</strong> information. To gain information about <strong>the</strong>molecules it is necessary to define <strong>the</strong> molecular orientation at <strong>the</strong> point <strong>of</strong> making a measurement.This can be achieved by using a strong non-resonant linearly polarized laser field 1 . The molecularaxis alignment distribution induced from such a laser pulse can be measured by using CoulombExplosion Imaging technique 2 .We are developing an experiment for creating molecular axis alignment, and measuring it usingtime-resolved femtosecond laser Coulomb explosion in conjunction with velocity map imaging(VMI). Two laser beams are thus necessary: a linearly polarized pump laser beam aligns <strong>the</strong>molecules, and a circularly polarized laser beam Coulomb explodes <strong>the</strong>m. We have chosen acircular polarization <strong>of</strong> <strong>the</strong> probe laser beam in order to obtain a uniform efficiency <strong>of</strong> <strong>the</strong> detectionfunction for each possible direction <strong>of</strong> <strong>the</strong> molecular axis in <strong>the</strong> polarization plane. However, such apolarization breaks <strong>the</strong> cylindrical symmetry <strong>of</strong> <strong>the</strong> exploded ions cloud. As a consequence an Abelinversion algorithm (a necessary step to obtain 3D distribution from 2D projection recorded withVMI) cannot be used to invert <strong>the</strong> acquired images.We present <strong>the</strong> development <strong>of</strong> a new algorithm that inverts <strong>the</strong> images obtained in ourexperimental configuration allowing <strong>the</strong> reconstruction <strong>of</strong> <strong>the</strong> angular and energy distributions <strong>of</strong><strong>the</strong> ions. The angular distribution <strong>of</strong> <strong>the</strong> ions permits recovery <strong>of</strong> <strong>the</strong> degree <strong>of</strong> alignment <strong>of</strong> <strong>the</strong>molecules before <strong>the</strong> explosion.1 J. B. Fredrich and D. Herschbach, Alignment and Trapping <strong>of</strong> Molecules in Intense Laser Fields, Phys. Rev. Lett. 74,4623 (1995).2 J. J. Larsen et al., Three Dimensional Alignment <strong>of</strong> Molecules Using Elliptically Polarized Laser Fields, Phys. Rev.Lett. 85, 2470 (2000).42


P10A BRIEF SUMMARY OF EXPERIMENTS AT FLASH – IONISATION ININTENSE LASER FIELDSV Richardson 1 J. Dardis 1 , P. Hayden 1 , P. Hough 1 , E. T. Kennedy 1 , J. T. Costello 1 , S. Düsterer 2 , W.Li 2 , A. Azima 2 , H. Redlin 2 , K. Tiedke 2 , P. Juranic 2 , J. Feldhaus 2 , D. Cubaynes 3 , D. Glijer 3 , M.Meyer 3 , A.A. Sorokin 4 , M. Richter 4 , H. van der Hart 5 , N. Grum-Grzhimailo 6 E.V. Gryzlova 6 and S.I. Strakhova 6 , R. Taïeb 7 and A. Maquet 7 .1 School <strong>of</strong> Physical Sciences, National Centre for Plasma Science and Technology,Dublin City University, Dublin 9, Ireland, 2 HASYLAB, DESY, Notkestr. 85, D-22607 Hamburg,Germany, 3 LIXAM/ CNRS, UMR 8624 Centre Universitaire Paris-Sud, Bâtiment 350, F-91405Orsay Cedex, France, 4 Physikalisch-Technische Bundesanstalt, Abbestrasse 2-12, D-10587 Berlin,Germany, 5 Dept. Of Applied Ma<strong>the</strong>matics and Theoretical Physics, David Bates Building, Queen’sUniversity Belfast, Belfast, BT7 1NN, Nor<strong>the</strong>rn Ireland, 6 Institute <strong>of</strong> Nuclear Physics, MoscowState University, Moscow 119991, Russia, 7 UPMC, Université Paris 06, CNRS, UMR 7614,LCPMR, 11 Rue Pierre et Marie Curie, 75231 Paris Cedex 05, FranceFLASH (Free electron LASer in Hamburg) operates on <strong>the</strong> principle <strong>of</strong> Self Amplified SpontaneousEmission (SASE) and produces coherent, bright and ultrashort eXtreme- UV (XUV) pulses 1 . Bysynchronizing FLASH with an independent optical laser, it is possible to induce and controlcoherent processes in superimposed, intense XUV and NIR fields. One such process isphotoelectron sideband generation 2 . In this class <strong>of</strong> experiment, photoelectrons are ejected by XUVradiation and simultaneously subjected to <strong>the</strong> intense field <strong>of</strong> an optical laser with which <strong>the</strong>y canexchange photons. In effect, <strong>the</strong>y absorb/emit photons with energy corresponding to ħω i.e. thatenergy <strong>of</strong> <strong>the</strong> optical laser photons 3,4 . As a consequence <strong>the</strong> photoelectron spectrum is no longercomprised <strong>of</strong> a single feature corresponding to <strong>the</strong> main photoline but is straddled by additionalphotoelectron lines separated by ħω - <strong>the</strong>se are referred to as sidebands.The use <strong>of</strong> a highly developed EUVL Si-Mo multilayer mirror allows one to focus <strong>the</strong> FEL beam,resulting in ultrahigh intensities on <strong>the</strong> order <strong>of</strong> 10 -16 Wcm -2 5 . This intensity, coupled with a lowFEL wavelength (13nm) makes it possible to induce non-linear inner shell ionisation processes. For<strong>the</strong> first time using photoelectron spectroscopy, a signal has been detected resulting from <strong>the</strong> directtwo photon inner shell ionisation <strong>of</strong> an atom, in this case <strong>of</strong> <strong>the</strong> 4d subshell <strong>of</strong> xenon._______________________1 W. Ackermann et al, Nature Photonics 1 336 (2007).2 T.E. Glover et al., Phys Rev Lett. 76, 2468 (1996).3 P. Radcliffe et al, App Phys Lett, 90, 121109 (2007),.4 M. Meyer et al, Phys. Rev. Lett, 101 193002 (2008).5 A.A. Sorokin et al, Phys Rev Lett, 99, 213002 (2007).43


P11TIME-RESOLVED STIMULATED EMISSION SPECTROSCOPY IN THESUBPICOSECOND DOMAIN THROUGH PUMP–PROBE EXPERIMENTSS. Orlando 1 , A. Paladini 1 , L. Guidoni 2 , A. Santagata 1 , G.P. Parisi 1 , P. Villani 1,3 ,R. Teghil 3 , A. Galasso 3 , A. Giardini 11 CNR, Istituto di Metodologie Inorganiche e dei Plasmi, Sede di Potenza, I-85050, Tito Scalo (PZ),Italy2 CNRS, Materiaux et Phenomenes Quantiques UMR 7162, Universite Denis Diderot, Paris 7,Paris, France3 Dipartimento di Chimica, Universita` <strong>degli</strong> Studi della Basilicata, I-85100 Potenza, ItalyThe photoemission properties <strong>of</strong> fluorescent chromophores have a widespread application in manyfields ranging from chemical-physics and biology to organic light emitting devices. These systemsusually display high fluorescence conversion efficiency, which makes <strong>the</strong>m suitable fortransient/gain experiments also in liquid solutions, thin films and eventually in proteinenvironments.Pump and probe methods have been widely employed for wavelength-resolved spectroscopy in <strong>the</strong>subpicosecond time scale. In our group, we have recently assembled a new experimental setup forpump and probe spectroscopy: preliminary tests on <strong>the</strong> Rhodamine B dye in ethanol have beenperformed in order to optimize <strong>the</strong> setup. The dynamic response <strong>of</strong> photoinduced changes <strong>of</strong> <strong>the</strong>chromophore dispersed into a suitable solvent has been studied with a subpicosecond timeresolution.The optically prepared initial state <strong>of</strong> <strong>the</strong> Rhodamine B in ethanol solution appears to evolve on atimescale <strong>of</strong> few picoseconds into a successive state, which could be attributed to an intramolecularcharge transfer state.44


P12HIGH-ORDER HARMONIC GENERATION FROM MOLECULES:CLASSICAL VERSUS QUANTUM EFFECTSE. Fiordilino, G. Castiglia, P.P. Corso, G. Orlando, F. PersicoDipartimento di Scienze Fisiche ed Astronomiche, Università <strong>degli</strong> Studi di Palermo, Via Archirafi36, 90123 Palermo and CNISMWe investigate High-Order Harmonic Generation from simple molecules and molecular ions; inparticular we are mainly interested on <strong>the</strong> effects <strong>of</strong> <strong>the</strong> nuclei dynamics on <strong>the</strong> emitted spectra.These effects are mainly related to both <strong>the</strong> appearance <strong>of</strong> satellite peaks around <strong>the</strong> usual oddharmonics and to an evident isotopic effect which allows to relate <strong>the</strong> intensity <strong>of</strong> <strong>the</strong> emitted linesto <strong>the</strong> mass <strong>of</strong> <strong>the</strong> isotopes. Fur<strong>the</strong>rmore we show that <strong>the</strong> presence <strong>of</strong> <strong>the</strong> satellite peaks isexplainable in terms <strong>of</strong> just a classical model <strong>of</strong> nuclei dynamics; on <strong>the</strong> contrary, <strong>the</strong> isotopic effectis only observable if we describe <strong>the</strong> nuclei as quantum objects. All <strong>the</strong> discussed results have beenobtained by numerically solving <strong>the</strong> time-dependent Schroedinger equations <strong>of</strong> <strong>the</strong> investigatedsystems.45


P13CONCEPTUAL IDEAS FOR THE TEMPORAL OVERLAP OF THEELECTRON BEAM AND THE SEED LASER FOR SFLASHJ.Bödewadt 1 , J. Rossbach 1 , R.Tarkeshian* ,1 , V. Milchev 1H. Schlarb 2 , S. Schreiber 2R. Ischebeck 31 University <strong>of</strong> Hamburg, Germany2 DESY, Hamburg3 PSI, SwitzerlandsFLASH is a seeding FEL experiment at FLASH/DESY, to introduce a 30nm high harmonic gain(HHG)-based XUV-beam laser to <strong>the</strong> electron bunches <strong>of</strong> FLASH at <strong>the</strong> entrance <strong>of</strong> a 10mvariable-gap undulator. The temporal overlap between <strong>the</strong> electron beam and HHG is important for<strong>the</strong> seeding process. The installation <strong>of</strong> a 3rd harmonic cavity at FLASH will provide a long highcurrent electron beam (at kA level) over ~ 600 fs Full-Width at Half- Maximum (FWHM) bunchduration. The duration <strong>of</strong> <strong>the</strong> HHG laser pulse will be about 30fs (FWHM). The desired overlap canbe achieved in steps. One approach will be to synchronize <strong>the</strong> drive laser (Ti: Sapphire, 800nm) <strong>of</strong>HHG and <strong>the</strong> incoherent spontaneous synchrotron radiation <strong>of</strong> <strong>the</strong> undulator at a sub-picosecondprecision. In a following step <strong>the</strong> overlap can be improved by scanning within <strong>the</strong> sub-picoseconduncertainty. The possibility <strong>of</strong> using a streak camera to detect both <strong>the</strong> 800nm laser and <strong>the</strong>spontaneous undulator radiation pulses without perturbing FLASH user operation is investigated.To match <strong>the</strong> power levels, <strong>the</strong> laser beam has to be attenuated by several orders in magnitude. Thelayout <strong>of</strong> <strong>the</strong> experiment and preliminary simulation results <strong>of</strong> generation and transport <strong>of</strong> both lightpulses are presented.46


P14CONTROL OF THE POLARIZATION OF ATTOSECOND PULSES USINGA TWO-COLOR FIELDCamilo Ruiz 1,2 , David H<strong>of</strong>fmann 1 , Ricardo Torres 1 , Luke Chipperfield 1and Jonathan P Marangos 11 Blackett Laboratory, Imperial College London, London SW7 2BW, UK1 Centro de Laseres Pulsados ultraintensos, Plaza de la Merced s/n 37006 ,Salamanca, SpainControl over <strong>the</strong> polarization <strong>of</strong> an attosecond pulse train is demonstrated <strong>the</strong>oretically by usingorthogonally polarized two-color fields. The carrier envelope phase (CEP) <strong>of</strong> <strong>the</strong> two pulses is usedas a control parameter to switch from linear polarization in two planes to elliptical polarization. Thecontrol mechanism is explained in terms <strong>of</strong> classical trajectories.In this paper we will address <strong>the</strong> control <strong>of</strong> <strong>the</strong> polarization and temporal structure <strong>of</strong> <strong>the</strong> attosecondpulses and APT by using two perpendicular fields <strong>of</strong> different frequencies overlapped in time. Theadvantage <strong>of</strong> <strong>the</strong> proposed scheme is its flexibility. Several distinct control scenarios can beobtained: a good degree <strong>of</strong> control over <strong>the</strong> polarization – from linear to elliptical – by adjusting <strong>the</strong>CEP <strong>of</strong> <strong>the</strong> two fields and, in <strong>the</strong> case <strong>of</strong> linear polarization, a simple way to change <strong>the</strong> temporalstructure <strong>of</strong> <strong>the</strong> APT obtained. Such pulses, and <strong>the</strong> required control over <strong>the</strong> CEP are nowavailable from state-<strong>of</strong>-<strong>the</strong>-art ultra intense few-cycle laser systems 1,2.________________________________________1 E. Goulielmakis et al., Single-Cycle Nonlinear Optics, Science 320, 1614 (2008).2 G. Cirmi, et al., Carrier-envelope phase stable, few-optical-cycle pulses tunable from visible tonear IR, J. Opt. Soc. Am. B 25, B62 (2008).47


Friday 1 st May15:00 – 16:45Afternoon session:Attosecond Electron Dynamics IIChair: P. Corkum48


ATTOSECOND STEERING OF ELECTRONIC MOTION IN ATOMS ANDMOLECULES VIA ~6 FS CE PHASE STABILIZED PULSESR. Gopal 1 , A. Rudenko 2 , M. Kremer 1 , B. Fischer 1 , K. Simeonidis 1 , R. Moshammer 1 , Th. Ergler 1 , M.Kurka 1 , K.U. Kühnel 1 , C. D. Schröter 1 , D. Bauer 1 , B. Feuerstein 1 , V. L. B. de Jesus 4 , O. Herrwerth 3 ,Th. Uphues 3 , M. Schultze 3 , E. Goulielmakis 3 , M. Uiberacker 3 , M. Lezius 3 , M. F. Kling 3 , J.Ullrich 1,21 Max-Planck-Institut für Kernphysik (MPIK) , Saupfercheckweg 1, D-69117 Heidelberg2 Max Planck Advanced Study Group at CFEL, D-22607 Hamburg3 Max-Planck-Institut für Quantenoptik (MPQ), Hans-Kopfermann-Str. 1, D-85748 Garching4 CFET de Química de Nilópolis, Rua Lucio Tavares 1045, Rio de Janeiro, BrazilUsing a reaction-microscope, three-dimensional electron and ion momentum ( P r ) spectra have beenrecorded for carrier-envelope-phase (CEP) stabilized few-cycle (~ 5-6 fs), intense (4⋅10 14 W/cm 2 )laser pulses (740 nm) interacting with atoms and molecules. In a collaborative effort experiments onHe atoms have been performed at <strong>the</strong> MPQ whereas <strong>the</strong> fragmentation <strong>of</strong> H 2 molecules wasinvestigated at <strong>the</strong> new CEP stabilized pump-probe facility at <strong>the</strong> MPIK.For He atoms preferential emission <strong>of</strong> low-energy electrons (E e < 15 eV) to ei<strong>the</strong>r hemisphere isobserved as a function <strong>of</strong> <strong>the</strong> CEP. Clear interference patterns emerge in P r -space at CEPs withmaximum asymmetry, interpreted as attosecond holographic “self”-images <strong>of</strong> re-scattered electronwave-packets by means <strong>of</strong> a simple model and in line with previous <strong>the</strong>oretical predictions 1 . ForH 2 + molecules we do observe, for <strong>the</strong> first time and different from earlier measurements 2 , electronlocalisation in <strong>the</strong> 1ω and effective 2ω fragmentation channels depending on <strong>the</strong> kinetic energyrelease (KER) in general agreement with but at better significantly better contrast than predicted by<strong>the</strong>ory 3 . Moreover, we find <strong>the</strong> asymmetry varying as a function <strong>of</strong> <strong>the</strong> orientation <strong>of</strong> <strong>the</strong> moleculesand inspect CEP dependent coincident electron emission from <strong>the</strong> first step, i.e. ionizing <strong>the</strong> H 2molecule and starting <strong>the</strong> bound-state dynamics in H 2 + . Finally, we present results <strong>of</strong> wave-packetdynamic calculations, show data for more complicated molecules and envision future directions.1 D.G. Arbó et al. Phys. Rev. A 74, 063407 (2006).2M.F. Kling et al., Science 312 246 (2006).3V. Roudnev and B. D. Esry, PRA 76, 023403 (2007).49


WAVELENGTH DEPENDENCE OF HIGH-HARMONIC GENERATIONK. L. Ishikawa 1,2 , K. Schiessl 3 , E. Persson 3 , J. Burgdörfer 3 , E. J. Takahashi 4 , K. Midorikawa 4 ,1 RIKEN Computational Science Research Program, Saitama, Japan2 PRESTO, Japan Science and Technology Agency, Saitama, Japan3 Institute for Theoretical Physics, Vienna University <strong>of</strong> Technology, Vienna, Austria, EU4 Extreme Photonics Research Group, RIKEN Advanced Science Institute, Saitama, JapanWe investigate <strong>the</strong> dependence <strong>of</strong> <strong>the</strong> yield <strong>of</strong> <strong>the</strong> high-harmonic generation (HHG) on wavelengthλ <strong>of</strong> a few-cycle laser pulse. Superimposed on a smooth power-law dependence observedpreviously, we find surprisingly strong and rapid fluctuations on a fine λ scale 1 . Using <strong>the</strong>Lewenstein model <strong>of</strong> HHG, we identify <strong>the</strong> origin <strong>of</strong> <strong>the</strong>se fluctuations in terms <strong>of</strong> quantum pathinterferences with many returning orbits significantly contributing.We also investigate <strong>the</strong> connection <strong>of</strong> <strong>the</strong> fine-scale oscillations to <strong>the</strong> well-known channel closing(CC) effect. By studying <strong>the</strong> simultaneous variations with intensity and wavelength, differentmodels for <strong>the</strong> interference <strong>of</strong> channel closing peaks can be tested. Contrary to <strong>the</strong>oreticalpredictions for short-range potentials, <strong>the</strong> peaks are located nei<strong>the</strong>r at nor just below <strong>the</strong> CCcondition, but a significant shift is observed 2 . The long Coulomb tail <strong>of</strong> <strong>the</strong> atomic potential isidentified as <strong>the</strong> origin <strong>of</strong> <strong>the</strong> shift 3 .In addition, we study <strong>the</strong> scaling with λ <strong>of</strong> HHG, under <strong>the</strong> simultaneous irradiation <strong>of</strong> <strong>the</strong> boosterXUV pulse. Surprisingly, at fixed ponderomotive energy and ionization, <strong>the</strong> harmonic yield isnearly independent <strong>of</strong> λ. We identify one <strong>of</strong> its origins as <strong>the</strong> initial spatial width <strong>of</strong> <strong>the</strong> statesexcited by <strong>the</strong> booster pulse, making <strong>the</strong> wavepacket spreading less prominent. We also establishthat <strong>the</strong> distribution <strong>of</strong> <strong>the</strong> harmonic energy up to <strong>the</strong> cut<strong>of</strong>f has a contribution proportional to λ -2 .1 K. Schiessl et al. Quantum path interference in <strong>the</strong> wavelength dependence <strong>of</strong> high-harmonic generation. Phys. Rev.Lett. 99, 253903 (2007).2 K. Schiessl et al. Wavelength dependence <strong>of</strong> high-harmonic generation from ultrashort pulses. J. Mod. Opt. 55, 2617-2630 (2008).3 K. L. Ishikawa et al. Fine-scale oscillations in <strong>the</strong> wavelength- and intensity-dependence <strong>of</strong> high-harmonicgeneration: connection with channel closings. Phys. Rev. A, in press (2009).50


GENERATION AND APPLICATIONS OF ATTOSECONDPULSE TRAINSE. Mansten, J. M. Dahlström, K. Klünder, M. Swoboda, Xinkui He, J. Schwenke,P. Johnsson, J. Mauritsson, A. L’HuillierDepartment <strong>of</strong> PhysicsLund UniversityWhen an intense laser field interacts with an atomic gas, nonlinear processes take place, leading to<strong>the</strong> emission <strong>of</strong> a sequence <strong>of</strong> extremely short pulses <strong>of</strong> light, <strong>of</strong> attosecond duration. We willdiscuss in this talk a few techniques to frequency shape and tune attosecond pulses, as well as tomanipulate and characterize attosecond pulse trains in different conditions. Examples <strong>of</strong>applications <strong>of</strong> attosecond pulses and pulse trains will be presented.51


MACROSCOPIC EFFECTS IN SINGLE ATTOSECOND PULSEGENERATIONValer Tosa 1 , Carlo Altucci 2 and Raffaele Velotta 21 Natl. Inst. R&D Isotopic Molecular Technologies, Cluj-Napoca, Romania2 CNISM-Dipartimento di Scienze Fisiche, Università di Napoli “Federico II”, Napoli, ItaliaThe generation <strong>of</strong> a single isolated attosecond pulse (SAP) have been mainly achieved by means <strong>of</strong>High Harmonic Generation (HHG) in gas. Usually SAP can only be obtained if one is able to select<strong>the</strong> HHG emission within half a cycle <strong>of</strong> <strong>the</strong> laser field. We discuss here some <strong>of</strong> <strong>the</strong> macroscopiceffects which are responsible for producing clean isolated pulses lasting few hundreds <strong>of</strong>attoseconds. In particular we consider <strong>the</strong> polarisation gating scheme 1 and show that <strong>the</strong> gating and<strong>the</strong> ionization induced depletion usually producemore attosecond pulses <strong>of</strong> radiation at single dipolelevel. We show that non-homogeneous HHG in <strong>the</strong>interaction region as well as phase matchedharmonic field propagation, contribute to <strong>the</strong> SAPgeneration at macroscopic level.Non-adiabatic, three dimensional (3D) propagation<strong>of</strong> fundamental and harmonic fields through to <strong>the</strong>gas target has been accounted for by extending aprevious model to <strong>the</strong> case <strong>of</strong> two fields, and bynumerically integrating <strong>the</strong> correspondingpropagation equations for both fundamental andharmonic fields.The proposed experimental configurations areanalysed against <strong>the</strong> variation <strong>of</strong> various-4 -2 4t/T 0Fig. 1. The temporal SAP structure for±30% intensity variation1C. Altucci, V. Tosa, R. Velotta, Phys Rev A 75, 061401R (2007)2 C. Altucci, R. Esposito, V. Tosa, R. Velotta, Opt. Lett. 33, 2943 (2008)experimental parameters in view <strong>of</strong> <strong>the</strong>ir applicability to commercially available laser systems. Thedata in Fig. 1 demonstrate that in <strong>the</strong> polarization gating scheme recently 2 proposed <strong>the</strong> laserintensity may vary as much as 30% without altering <strong>the</strong> SAP structure. In <strong>the</strong> same schemehowever, <strong>the</strong> radial variation <strong>of</strong> <strong>the</strong> frequency modulation parameter (chirp) is limited to a 3-5%range.765432100.7 I 0I 01.3 I 052


Friday 1 st May15:00 – 16:45Afternoon session:Structural Dynamics <strong>of</strong> Complex Systems IChair: M. Chergui53


ULTRA-FAST PROBING OF SHOCK-COMPRESSED MATTER WITH X-RAY THOMSON SCATTERINGSiegfried GlenzerLawrence Livermore National Laboratory, P.O. Box 808, Livermore, CA 94551, USA,E-mail: glenzer1@llnl.govWe have developed accurate x-ray scattering techniques to measure <strong>the</strong> physical properties <strong>of</strong> denseplasmas. One future challenge is <strong>the</strong> application <strong>of</strong> this technique to characterize compressed mattersuch as produced in inertial confinement fusion experiments on <strong>the</strong> National Ignition Facility (NIF)where hydrogen and beryllium will approach extremely dense states <strong>of</strong> matter <strong>of</strong> up to 1000 g/cc.In this regime, present experiments 1,2 show that density and compressibility can be directlymeasured from <strong>the</strong> spectral broadening <strong>of</strong> <strong>the</strong> Compton scattered spectrum <strong>of</strong> a high-energy x-raysource. This technique is model-independent and based on first principles allowing us to determine<strong>the</strong> density from <strong>the</strong> spectral shape <strong>of</strong> <strong>the</strong> scattering spectrum that is directly reflecting <strong>the</strong> electronvelocity distribution. For Fermi-degenerate plasmas, <strong>the</strong> spectrum thus provides <strong>the</strong> Fermi energy.In this talk, Compton scattering 3 and Plasmon scattering 4 experiments on shock-compressed matterwill be presented. Besides extracting <strong>the</strong> standard plasma parameters, density and temperature,forward scattering is shown to yield new observables such as a direct measure <strong>of</strong> collisions,structure factors, and <strong>the</strong> dispersion <strong>of</strong> plasma waves in quantum plasmas.*This work performed under <strong>the</strong> auspices <strong>of</strong> <strong>the</strong> U.S. Department <strong>of</strong> Energy by LawrenceLivermore National Laboratory under Contract DE-AC52-07NA27344.1 A. L. Kritcher et al., Science, 322,69 (2008).2 H. J. Lee et al., Phys. Rev. Letters, in print (2008).3 S. H. Glenzer et al., Phys. Rev. Letters 90, 175002 (2003).4 S. H. Glenzer et al., Phys. Rev. Letters 98, 065002 (2007).54


ULTRAFAST DYNAMICS AND PHASE TRANSITION IN PHOTOEXCITEDBISMUTH CRYSTALDavide Boschetto 1 , Denis Morineau 2 , Antoine Rousse 1 , Eugene Gamaly 3 , Andrei V. Rode 31 Laboratoire d’Optique Appliquée, ENSTA/Ecole Polytechnique,Chemin de la Hunière, 91761 Palaiseau, France2 Institut de Physique de Rennes, Université de Rennes 1, Campus de Beaulieu, 35042 Rennes,France3 Laser Physics Centre, The Australian National University,Canberra, ACT 0200, AustraliaThe ability to modify and control <strong>the</strong> physical properties <strong>of</strong> matter by using any external excitationis a very exciting challenge from both scientific and technological point <strong>of</strong> view. When usingfemtosecond laser pulse for excitation, <strong>the</strong> system is set in a highly non-equilibrium state, in which<strong>the</strong> interaction between all <strong>the</strong> degrees <strong>of</strong> freedoms <strong>of</strong> <strong>the</strong> crystal can produce transitions into newphases different from equilibrium ones. Following <strong>the</strong> relaxation dynamics with <strong>the</strong> required timeresolution <strong>of</strong> few tens <strong>of</strong> femtoseconds is a key step in order to understand <strong>the</strong> pathway <strong>of</strong> any <strong>of</strong>those transitions. However, <strong>the</strong> characterization <strong>of</strong> any transient state requires <strong>the</strong> measurement <strong>of</strong><strong>the</strong> dielectric function dynamics, which has <strong>the</strong> signature <strong>of</strong> <strong>the</strong> band structure modifications.We applied two-probes set-up for recovering <strong>the</strong> dynamics <strong>of</strong> dielectric function at 800 nm <strong>of</strong>photo-excited bismuth, in order to characterize <strong>the</strong> transient state following both <strong>the</strong> coherentphonon oscillation mode and <strong>the</strong> electron-phonon <strong>the</strong>rmalization process [1]. The results arecompared with those from static ellipsometry measurement as function <strong>of</strong> <strong>the</strong> crystal temperature.Just after <strong>the</strong> photo-excitation, <strong>the</strong> crystal is driven into a more metallic state, as expected by <strong>the</strong>injection <strong>of</strong> electrons into <strong>the</strong> conduction band, and coherent phonon mode starts. However, after<strong>the</strong> electron-phonon <strong>the</strong>rmalization that occurs in around 20 ps, <strong>the</strong> results suggest that bismuthcrystal undergoes a photo-induced phase transition toward a new transient metastable phase.____________________________________________1 D. Boschetto et al., Small Atomic Displacements Recorded in Bismuth by <strong>the</strong> Optical Reflectivity <strong>of</strong> FemtosecondLaser-Pulse Excitations, Physical Review Letters 100, 027404 (2008).55


X-RAY CROSS CORRELATION ANALYSIS UNCOVERS HIDDEN LOCALSYMMETRIES IN DISORDERED MATTERP. Wochner 1 , C. Gutt 2 , T. Autenrieth 2 , T. Demmer 1 , V. Bugaev 1 , A. Díaz Ortiz 1 , A. Duri 2 , F.Zontone 3 , G. Grübel 2 , H. Dosch 1,21 Max-Planck-Institut für Metallforschung, Heisenbergstrasse 3, D-70569 Stuttgart, Germany2 DESY, Notkestrasse 85, D-22607 Hamburg, Germany3 ESRF, 6 rue Jules Horowitz BP 220, 38043 Grenoble Cedex 09, FranceDisordered matter, such as glasses and liquids, does not exhibit translational symmetry and in turnis able to accommodate different local symmetries in <strong>the</strong> same system, among <strong>the</strong>m <strong>the</strong> icosahedrallocal order, which belongs to <strong>the</strong> forbidden motifs in periodic structures.To explore <strong>the</strong> different local symmetries in disordered matter we need to go beyond <strong>the</strong> standardpair correlation analysis. Using our newly developed 4-point x-ray cross correlation analysis(XCCA) concept toge<strong>the</strong>r with brilliant coherent x-ray sources, we have been able to access andclassify <strong>the</strong> o<strong>the</strong>rwise hidden local order within disorder in colloidal glasses 1 . The emerging localsymmetries are coupled to distinct momentum transfer (Q) values, which do not coincide with <strong>the</strong>maxima <strong>of</strong> <strong>the</strong> amorphous structure factor. Four-, six-, ten- and, most prevailing, five-foldsymmetries are observed. The observation <strong>of</strong> dynamical evolution <strong>of</strong> <strong>the</strong>se symmetries forms aconnection to dynamical heterogeneities in glasses, which is far beyond conventional diffractionanalysis.The XCCA concept opens up a fascinating view into <strong>the</strong> world <strong>of</strong> disorder and will definitely allow,with <strong>the</strong> advent <strong>of</strong> free electron x-ray lasers, an accurate and systematic experimentalcharacterization <strong>of</strong> <strong>the</strong> structure <strong>of</strong> <strong>the</strong> liquid and glass states. By analyzing single laser shot specklediffraction patterns <strong>the</strong> detailed structural dynamics can be studied on a shot by shot basis or viapump-probe technique. The combination <strong>of</strong> short-pulse XFEL radiation and large 2D-detectorarrays will also open up <strong>the</strong> window for <strong>the</strong> study <strong>of</strong> nano-powders and transient complex molecularstructures in solution.1 P. Wochner et al. X-ray Cross Correlation Analysis Uncovers Hidden Local Symmetries in Disordered Matter.Manuscript submitted.56


ULTRAFAST DYNAMICAL RESPONSE OF THE PROTOTYPE MOTTCOMPOUND V 2 O 3B. Mansart 1 , D. Boschetto 2 and M. Marsi 11 Laboratoire de Physique des Solides, UMR 8502, Université Paris-Sud, 91405 Orsay, France2 Laboratoire d’Optique Appliquée, ENSTA, CNRS, Ecole Polytechnique, 91761 Palaiseau, FranceCr-doped V 2 O 3 is considered as a prototype Mott-Hubbard system, presenting a first order metalinsulatorMott transition.. In this work, we used femtosecond time-resolved pump-probe reflectivityto study this complex material, extending for <strong>the</strong> first time <strong>the</strong> use <strong>of</strong> this technique to <strong>the</strong> study <strong>of</strong>several points <strong>of</strong> its phase diagram. In particular, we explored <strong>the</strong> difference between <strong>the</strong>paramagnetic metallic and paramagnetic insulating phases, which have been <strong>the</strong> subject <strong>of</strong>numerous <strong>the</strong>oretical and experimental studies, including some recent ones in our laboratory 1 .Our results show that <strong>the</strong> transient reflectivity <strong>of</strong> Cr-doped V 2 O 3 presents a complexphenomenology, characterized by an ultrafast electronic excitation followed by coherentoscillations corresponding to optical and acoustic lattice vibrations. These features depend onsurface crystallographic orientation, light polarization and on Cr doping <strong>of</strong> <strong>the</strong> specimen - i.e. on itsphase across <strong>the</strong> Mott transition - as we found after an extensive and systematic series <strong>of</strong>measurements.We will discuss <strong>the</strong>se results and <strong>the</strong>ir implications for our understanding <strong>of</strong> this model Mott-Hubbard system, also in <strong>the</strong> light <strong>of</strong> some recent and parallel synchrotron radiation basedexperiments which indicate that in some portions <strong>of</strong> <strong>the</strong> phase diagram <strong>the</strong> metallic and insulatingstate can coexist on a microscopic scale, thus affecting <strong>the</strong> dynamical evolution <strong>of</strong> <strong>the</strong> system.1 P. Limelette et al. Universality and critical behavior at <strong>the</strong> Mott transition. Science 302, 89 (2003).57


Saturday 2 nd May15:00 – 16:45Morning session:Structural Dynamics <strong>of</strong> Complex Systems IIChair: S. Glenzer58


ULTRAFAST MANIPULATION OF MAGNETIZATIONJoachim StöhrStanford Synchrotron Radiation Lightsource and PULSE CenterStanford University, Stanford, California, USASwitching <strong>of</strong> <strong>the</strong> magnetization <strong>of</strong> a ferromagnet between two opposite directions can be initiatedby an external magnetic field generated by current flow through wires or by injecting a spinpolarized current directly into <strong>the</strong> magnetic material. In <strong>the</strong> pursuit <strong>of</strong> smaller and faster switchingdevices, currentless reversal <strong>of</strong> <strong>the</strong> magnetization would be highly desirable. This would avoidenergy dissipation by current flow and overcome impedance induced speed limitations. It may <strong>the</strong>nbe possible to extend <strong>the</strong> present switching speed <strong>of</strong> about 100 ps into <strong>the</strong> femtosecond regime.In this talk I will discuss schemes <strong>of</strong> reversing <strong>the</strong> magnetization <strong>of</strong> a ferromagnet by electric fieldsalone, without charge or spin currents or external magnetic fields. The concept is based on using astrong (eV/atom) and short (femtoseconds) electric field pulse to distort <strong>the</strong> atomic charge densityalong <strong>the</strong> direction <strong>of</strong> <strong>the</strong> linearly polarized E field. The charge distortion in conjunction with <strong>the</strong>spin-orbit interaction can <strong>the</strong>n lead to a transient magneto-electronic anisotropy which can beutilized to redirect <strong>the</strong> magnetization. The switching process is initiated and predetermined by <strong>the</strong>orientation, magnitude, and temporal length <strong>of</strong> <strong>the</strong> E-field writing pulse.I will also present experimental data that support <strong>the</strong> proposed concept. In particular, we usedultrashort (70 fs) and ultrastrong (up to 20 GV/m) fields generated by a compressed relativisticelectron bunch to manipulate <strong>the</strong> magnetization in a magnetic thin film sample 1 . Such pulsesgenerate true half-cycle THz fields that imprint a characteristic magnetization pattern into <strong>the</strong>sample. Analysis <strong>of</strong> <strong>the</strong> pattern clearly reveals <strong>the</strong> existence <strong>of</strong> a magneto-electronic anisotropygenerated by <strong>the</strong> E field, superimposed on that due to <strong>the</strong> B field. Since <strong>the</strong> switching torque on <strong>the</strong>magnetization is quadratic in E but linear in B, we propose that a full cycle THz pulse, where <strong>the</strong> Bfield contribution cancels, could be employed for E field only switching.1 J. Stöhr and H. C. Siegmann, Magnetism: From Fundamentals to Nanoscale Dynamics, Springer 2006.59


ULTRAFAST ELECTRON AND SPIN DYNAMICS IN FERROMAGNETSH.A. DürrHelmholtz Zentrum Berlin, BESSY,Albert Einstein-Str. 15, 12489 Berlin, GermanyThe interplay between electronic, spin and lattice degrees <strong>of</strong> freedom <strong>of</strong>ten determines <strong>the</strong> function<strong>of</strong> complex materials such as ferromagnets, high T C superconductors, colossal magnetoresistive andmultiferroic oxides. Charge and orbital ordering phenomena can lead to metal-insulator transitionswith temperature or chemical doping. These phenomena can ideally be studied using s<strong>of</strong>t x-rayswhich probe directly <strong>the</strong> valence orbitals responsible for electronic and spin order. Time resolvedoptical pump – x-ray probe studies <strong>of</strong>fer <strong>the</strong> exciting prospect <strong>of</strong> observing <strong>the</strong> flow <strong>of</strong> energy andangular momentum in real time 1 . Here I will concentrate on ferromagnetic materials where x-raydichroism is a unique probe <strong>of</strong> <strong>the</strong> spin order while x-ray resonant scattering provides direct accessto orbital and charge order. Examples <strong>of</strong> ultrafast laser induced demagnetization <strong>of</strong> Gd and laserinduced melting <strong>of</strong> charge order in magnetite will be described.1 C. Samm et al. Femtosecond modification <strong>of</strong> electron localization and exchange <strong>of</strong> angular momentum in Ni, NatureMaterials 6, 740 (2007).60


ULTRAFAST ELECTRONIC PROCESSES IN CLUSTERSJ. RostMax-Planck-Institut fuer Physik komplexer SystemeNoethnitzer Str. 38, D-01187 DresdenAttosecond pulses extend our capabilities to excited electrons in various ways. Simultaneous(within <strong>the</strong> length <strong>of</strong> an attosecond pulse) excitation <strong>of</strong> several electrons becomes in principlepossible but requires also roughly equivalent bound electrons. This is <strong>the</strong> case in rare gas clusters.The resulting, unusual, excitation dynamics will be discussed. In <strong>the</strong> second part <strong>of</strong> <strong>the</strong> talk a newmechanism <strong>of</strong> ultrafast formation <strong>of</strong> an electronic nanoplasma will be introduced, which does notrequire attosecond pulses. It relies on a substantial breaking <strong>of</strong> <strong>the</strong> spherical plasma symmetrywhich can be easily induced by seed atoms (molecules) 1 .1A. Mikaberidze, U. Saalmann, J. M. Rost, Phys. Rev. Lett 102, 128102 (2009).61


TR-PHOTOEMISSION ELECTRON MICROSCOPY - NANOSCALESPECTROSCOPY WITH FEMTOSECOND RESOLUTIONMartin AeschlimannDepartment <strong>of</strong> Physics and Research Center OPTIMAS, University <strong>of</strong> Kaiserslautern, GermanyIn this contribution I will present an experimental scheme capable <strong>of</strong> monitoring ultrafast dynamicson nanoscale dimensions. Over <strong>the</strong> last decade <strong>the</strong>re have been numerous attempts to combinescanning probe microscopy and femtosecond pump-probe techniques to realize an ultrafastmicroscope with nanometer resolution. So far, no satisfactory solution has been presented. Ourapproach applies <strong>the</strong> technique <strong>of</strong> time-resolved 2PPE to a conventional photoemission electronmicroscope (PEEM) 1 . In this configuration <strong>the</strong> photoemission signal collected by <strong>the</strong> PEEMdetector is related to <strong>the</strong> lifetime <strong>of</strong> excited (hot) electrons at <strong>the</strong> sample surface.The potential <strong>of</strong> this technique will be illustrated by two examples: In a first study <strong>the</strong> time-resolvedPEEM technique is used to map <strong>the</strong> dynamical response <strong>of</strong> supported metal clusters (


OPTICAL AND X-RAY STUDIES OF THE ULTRAFAST DYNAMICS OFMOLECULAR SYSTEMS IN LIQUIDSM. CherguiLaboratoire de Spectroscopie Ultrarapide (LSU), Ecole Polytechnique Fédérale de Lausanne,CH-1015 Lausanne SwitzerlandThe details <strong>of</strong> <strong>the</strong> photoinduced dynamics <strong>of</strong> molecular systems in liquids has been investigated bya combination <strong>of</strong> different ultrafast spectroscopic techniques, which include transient absorption in<strong>the</strong> visible and UV (down to 300 nm), polychromatic femtosecond fluorescence measurements in<strong>the</strong> range from 300 to 800 nm, and picosecond and femtosecond hard X-ray absorptionspectroscopy. These approaches allow us to probe both <strong>the</strong> molecular structure <strong>of</strong> <strong>the</strong> systems, butalso <strong>the</strong> underlying electronic structure changes that trigger <strong>the</strong>m. We will present examples on <strong>the</strong>spin and structural dynamics in Fe(II)-based molecular complexes, 1,2 on <strong>the</strong> dynamics <strong>of</strong> electronicsolvation 3,4 and on <strong>the</strong> bond formation in bimetallic complexes 5 .1 W. Gawelda et al. Structural determination <strong>of</strong> a short-lived Iron(II) Complex by Picosecond X-ray AbsorptionSpectroscopy. Phys. Rev. Lett. 98 (2007) 057401.2 C. Bressler et al. Femtosecond XANES <strong>of</strong> <strong>the</strong> light-induced spin crossover dynamics in an Iron(II)-complex Science323 (2009) 489.3 Van Thai Pham et al. Observation <strong>of</strong> <strong>the</strong> solvent shell reorganisation around electronically excited atomic solutes bypicosecond X-ray absorption spectroscopy. J. Am. Chem. Soc. 129 (2007) 1530.4 C. Bressler et al. Exploiting EXAFS and XANES for Time-Resolved Molecular Structures in Liquids. Z. für Kristall.223 (2008) 307.5 R. M. van der Veen et al. Structural determination <strong>of</strong> photochemically active diplatinum molecule by time-resolvedEXAFS spectroscopy. Ang. Chem. Int. Ed. (in press).63


“MAKING THE MOLECULAR MOVIE”: QUEST FOR THE STRUCTURE-FUNCTION CORRELATION OF BIOLOGYR.J. Dwane MillerDepartments <strong>of</strong> Chemistry and Physics,Institute for Optical SciencesUniversity <strong>of</strong> Toronto,Toronto, Ontario, Canada, M5S 3H6dmiller@lphys.chem.utoronto.caFemtosecond Electron Diffraction harbours great potential for providing atomic resolution tostructural changes as <strong>the</strong>y occur, essentially watching atoms move in real time ― directly observetransition states. This experiment has been referred to as "making <strong>the</strong> molecular movie" and hasbeen previously discussed in <strong>the</strong> context <strong>of</strong> a classic gedanken experiment, outside <strong>the</strong> realm <strong>of</strong>direct observation. With <strong>the</strong> recent development <strong>of</strong> femtosecond electron pulses with sufficientnumber density to execute nearly single shot structure determinations, this experiment has beenfinally realized. A new concept in electron pulse generation was developed based on a solution to<strong>the</strong> N-body electron propagation problem involving up to 10,000 interacting electrons that has ledto a new generation <strong>of</strong> extremely “bright” electron pulsed sources that minimizes space chargebroadening effects. Previously thought intractable problems <strong>of</strong> determining t=0 and fullycharacterizing electron pulses on <strong>the</strong> femtosecond time scale have now been solved through <strong>the</strong>use <strong>of</strong> <strong>the</strong> laser pondermotive potential to provide a time dependent scattering source.Synchronization <strong>of</strong> electron probe and laser excitation pulses is now possible with an accuracy <strong>of</strong>10 femtoseconds to follow even <strong>the</strong> fastest nuclear motions. The camera for <strong>the</strong> “molecular movie”is now in hand with electron based sources. Atomic level views <strong>of</strong> <strong>the</strong> simplest possible structuraltransition have been obtained under strongly driven conditions (up to warm dense matterconditions) as well as electronically driven atomic motions as a direct probe <strong>of</strong> <strong>the</strong> many bodyelectron correlation effects on <strong>the</strong> forces related to bonding. The overall objective is to extend thisapproach to biological systems to directly observe <strong>the</strong> structure-function correlation ⎯ <strong>the</strong>fundamental underpinnings <strong>of</strong> biology.64


QUANTUM DIMENSION OF PHOTOSYNTHESISREVEALED BY POWERFUL NEW LASER TECHNIQUEIan P. Mercer 1 , Yasin C. El-Taha 2 , Nathaniel Kajumba 2 , Jonathan P. Marangos 2 , John W. G. Tisch 2 ,Mads Gabrielsen 3 , Richard J. Cogdell 3 , Emma Springate 4 & Edmund Turcu 41School <strong>of</strong> Physics, Centre for Syn<strong>the</strong>sis and Chemical Biology,University College Dublin, Dublin 4, Ireland.2 Quantum Optics and Laser Science Group, Blackett Laboratory,Imperial College, London, UK.3 Biochemistry and Molecular Biology, Faculty <strong>of</strong> Biomedical and Life Sciences,University <strong>of</strong> Glasgow, Glasgow, UK.4Central Laser Facility, STFC Ru<strong>the</strong>rford Appleton Laboratory, Didcot, UK.Coherent electronic motion may play a role in <strong>the</strong> remarkably efficient energy transfer inphotosyn<strong>the</strong>tic macromolecules. Coherent optical four wave mixing has been used widely to obtaininformation on <strong>the</strong> timescales <strong>of</strong> energy transfer in complex molecular systems. However, <strong>the</strong>interpretation <strong>of</strong> such measurements is difficult in particular where chromophores are stronglycoupled, such as in photosyn<strong>the</strong>tic systems, and new methods are required for an improvedfeedback to simulation.We present a novel non-linear optical method, Angle-Resolved Coherent (ARC) wave mixing, thatseparates out coherent electronic couplings from energy transfers in an instantaneous twodimensionalmapping 1 . For this we use a high energy, ultra-broadband hollow fibre laser source 2 .The power <strong>of</strong> <strong>the</strong> new method is demonstrated with <strong>the</strong> light harvesting complex II (LH2) <strong>of</strong> purplebacteria at ambient temperature. We reveal a coherent quantum electronic beating with a timeorderedmatter-selection <strong>of</strong> transition energies. We show that <strong>the</strong> position <strong>of</strong> a feature can mapuniquely to each <strong>of</strong> <strong>the</strong> four laser beam interaction energies that produce <strong>the</strong> signal and we observea correlation between excitation and emission energies in <strong>the</strong> protein.1 I.P. Mercer et al., Phys. Rev. Lett. 102, 57402 (2009).2 J. S. Robinson et al., Appl. Phys. B 85, 525 (2006).65


Sunday 3 rd May9:00 – 11:30Morning session:New Methods and SourcesChair: J. Rossbach66


WATER WINDOW X-RAY GENERATION BY PHASE-MATCHED HIGHHARMONICS WITH NEUTRAL MEDIAKatsumi MidorikawaExtreme Photonics Research Group, RIKEN2-1 Hirosawa, Wako, Saitama 351-0198, Japankmidori@riken.jpHigh-order harmonics generation (HHG) provides highly coherent ultrafast s<strong>of</strong>t x-ray pulses from atabletop laser system. HHG has been attracting much attention due to <strong>the</strong>ir unique properties, suchas ultrashort pulse duration, high peak intensity and brightness, wide tunability, and low equipmentcost. Although <strong>the</strong> harmonics photon energy attained within <strong>the</strong> ”water window” region by usingsub-10 fs Ti:sapphire laser as a driving source, <strong>the</strong> generation efficiency <strong>of</strong> <strong>the</strong> water windowwavelength harmonics was limited by <strong>the</strong> dephasing <strong>of</strong> <strong>the</strong> atomic dipoles and <strong>the</strong> plasmadefocusing <strong>of</strong> <strong>the</strong> laser pulse due to free electrons, because <strong>the</strong> laser intensity exceeds <strong>the</strong> ionizationthreshold <strong>of</strong> <strong>the</strong> target gases for 800 nm driving lasers.Here we report on <strong>the</strong> generation <strong>of</strong> coherent water-window x-ray by phase-matched highharmonics in neutral media. The spectral cut<strong>of</strong>f <strong>of</strong> HHG is approximately given by Ip + 3.17Up,where Ip is <strong>the</strong> ionization potential and Up is <strong>the</strong> ponderomotive energy. Since <strong>the</strong> ponderomotiveenergy is proportional to not only <strong>the</strong> pump laser intensity but also <strong>the</strong> square <strong>of</strong> <strong>the</strong> driving laserwavelength, a longer-wavelength intense infrared laser allows generating higher-energy harmonicphotons without ionization. We have demonstrated <strong>the</strong> efficient generation <strong>of</strong> a coherent x-ray highorderharmonics in <strong>the</strong> water window region using an IR driving laser and a neutral rare-gasmedium. Our proposed procedure for generating <strong>the</strong> water window x-ray is efficient and scalable inoutput yield, which provides us with <strong>the</strong> HHG parameters required for <strong>the</strong> imaging <strong>of</strong> live cells.67


LINAC COHERENT LIGHT SOURCE AND SINGLE MOLECULEIMAGINGSébastien BoutetLinac Coherent Light Source, SLAC National Accelerator LaboratoryThe Linac Coherent Light Source (LCLS), coming on-line in <strong>the</strong> Summer <strong>of</strong> 2009, will become <strong>the</strong>first ever hard x-ray Free-Electron Laser (FEL). It will utilize <strong>the</strong> 13 GeV electron beam from <strong>the</strong>last km <strong>of</strong> <strong>the</strong> 3 km long linear accelerator on <strong>the</strong> site <strong>of</strong> <strong>the</strong> SLAC National Accelerator Laboratoryto produce hard x-ray pulses containing 10 12 photons or more in less than 100 femtoseconds. Theincredible brightness <strong>of</strong> this new source will make it a unique tool with unexplored discoverypotential. Among <strong>the</strong> novel scientific opportunities hard x-ray FELs <strong>of</strong>fer, <strong>the</strong> possibility <strong>of</strong>obtaining snapshot images <strong>of</strong> single non-periodic objects, especially biological samples, hasgenerated a tremendous level <strong>of</strong> excitement. The extremely short duration and high intensity <strong>of</strong> <strong>the</strong>x-ray beam promises to minimize radiation damage to biological samples during <strong>the</strong> pulse and toallow high resolution imaging <strong>of</strong> non-crystalline objects.In this talk, I will discuss <strong>the</strong> LCLS and <strong>the</strong> status <strong>of</strong> its commissioning as <strong>the</strong> start <strong>of</strong> operationsrapidly approaches. I will briefly introduce <strong>the</strong> experimental instruments being built for LCLS thatwill utilize to its fullest <strong>the</strong> unique properties <strong>of</strong> <strong>the</strong> beam in areas <strong>of</strong> ultra-fast science. Finally, Iwill discuss in greater detail <strong>the</strong> plans for <strong>the</strong> single molecule imaging instrument along with some<strong>of</strong> <strong>the</strong> recent results validating <strong>the</strong> techniques required for such experiments.68


TWO COLOUR AND TWO PHOTON IONIZATION PROCESSES ININTENSE EUV AND OPTICAL FIELDS AT ‘FLASH’J. T. Costello 1 , J. Dardis 1 , P. Hayden 1 , P. Hough 1 , T. J. Kelly 1 , E. T. Kennedy 1 ,V. Richardson 1 , A. A. Sorokin 2 , M. Richter 2 , S. Duesterer 3 , W. B. Lee 3 , K. Tiedke 3 ,J. Feldhaus 3 , R. Taieb 4 , A. Maquet 4 , H. van der Hart 5 , A. N. Grum-Grzhimailo 6 ,E. V. Gryzlova 6 , S. I. Strakhova 6 , D. Cubaynnes 7 and M. Meyer 71 School <strong>of</strong> Physical Sciences & NCPST, Dublin City University, Dublin 9, Ireland2 Physikalisch-Technische Bundesanstalt, Abbestrasse 2-12, D-10587 Berlin, German3 HASYLAB at DESY, Notkestr. 85, D-22607 Hamburg, Germany4 UPMC, Universite Paris 06, CNRS, UMR 7614, LCPMR, 75231 Paris Cedex 05, France5 Dept. Of Applied Ma<strong>the</strong>matics and Theoretical Physics, QUB, Belfast, BT7 1NN, N. Ireland6 Institute <strong>of</strong> Nuclear Physics, Moscow State University, Moscow 119991, Russia7 LIXAM, UMR 8624, Universite Paris Sud, Batiment 350, 91405 Orsay Cedex, FranceThe EUV research domain is undergoing a period <strong>of</strong> unprecedented growth, motivated not just by adesire to educidate <strong>the</strong> fundamental light-matter interaction on atomic time and spatial scales butalso by <strong>the</strong> prospects that <strong>the</strong> field <strong>of</strong>fers to address impending bottlenecks in semiconductormanufacturing on <strong>the</strong> nanoscale and improve molecular scale imaging with its unfolding benefits in<strong>the</strong> health and biomedial sciences. The key outcome <strong>of</strong> <strong>the</strong> EUV photon-matter interaction isphotoionization and, in <strong>the</strong> case <strong>of</strong> weak EUV fields, <strong>the</strong>ory and experiment have developedsymbiotically to provide a deep understanding <strong>of</strong> <strong>the</strong> underlying photon-electron processes even inhighly correlated systems. The complementary field <strong>of</strong> ionization in intense optical laser fields hasrevealed many new dynamical processes such as multi-photon, above-threshold and optical-fieldionization as well as high harmonic generation [1]. Now <strong>the</strong> development <strong>of</strong> EUV Free ElectronLaser facilities such FLASH [2] signals a new era for <strong>the</strong> study atomistic systems in not just intensebut also in ultrahigh frequency fields [3,4]. In this talk I will provide an update on <strong>the</strong> FLASHfacility and briefly summarise its current performance parameters. Experimental topics will includea demonstration experiment on dissociation <strong>of</strong> H 2 and photoionization <strong>of</strong> rare gas atoms in intenseEUV and superposed EUV/optical fields. The talk will wrap up with some perspectives onexperiments following <strong>the</strong> imminent FLASH upgrade (2010) and to be carried out at LCLS (2009).__________________________1 Corkum PB, Krausz F, Attosecond Science, Nature Physics, Vol: 3, 381 (2007).2 Ackermann W et al, Operation <strong>of</strong> FLASH in <strong>the</strong> Water Window, Nature Photonics, Vol: 1, 336 (2007).3 Costello J T Photoionization Experiments with FLASH, J. Phys. Conf. Ser. Vol: 88 012057 (2007).4 Bostedt C et al., Experiments at FLASH, Nucl. Inst. Meth. in Res. A doi:10.1016/j.nima.2008.12.202 (2009).69


INVESTIGATION OF ULTRAFAST STRUCTURAL CHANGES INCOMPLEX CHEMICAL SYSTEMS USING X-RAY FELSTh. Tschentscher 1 , M. Messerschmidt 2 , S. Techert 33 European XFEL, c/o DESY, Notkestraße 85, 22603 Hamburg, Germany2 DESY, Notkestraße 85, 22603 Hamburg, Germany3 MPI Biophysical Chemistry, Am Faßberg 11, 37070 Göttingen, GermanyResearch using ultrashort, intense and coherent x-ray pulses providing by forth-coming x-ray freeelectronlaser (FEL) facilities enables new insight into <strong>the</strong> structural and dynamic behaviour <strong>of</strong>molecules, clusters, plasmas or solid state matter. A time resolution in <strong>the</strong> regime <strong>of</strong> 100femtoseconds and below is well suited to investigate ultrafast electronic and structural dynamics <strong>of</strong>very different origin. As an example for one area <strong>of</strong> research <strong>the</strong> application to small moleculechemical systems will be discussed in this presentation. X-ray diffraction, scattering and imagingtechniques provide <strong>the</strong> necessary spatial resolution to study structural properties at <strong>the</strong> relevantatomic length scale, e.g. to investigate <strong>the</strong> time evolution <strong>of</strong> <strong>the</strong> geometrical structure <strong>of</strong> moleculesduring <strong>the</strong> course <strong>of</strong> transitions. Spectroscopic techniques can fur<strong>the</strong>r be used to study electronicexcitations. Using hard x-rays and investigating crystalline samples will enable to exploit x-raystructure determination techniques achieving very high sensitivity and spatial resolution. Currentlythis research is limited by <strong>the</strong> availability <strong>of</strong> x-ray sources providing at <strong>the</strong> same time femtosecondtime-resolution, adequate resolution and significant photon flux. Hard x-ray FELs will change thissituation dramatically.Results <strong>of</strong> pre-cursor experiments investigating ultrafast dynamics in small molecules using hard x-ray synchrotron radiation with reduced time resolution and s<strong>of</strong>t x-ray FEL radiation with reducedspatial resolution will be presented. Issues to be addressed in terms <strong>of</strong> instrumentation using FELswill be discussed. In this context also concepts for applying <strong>the</strong> high repetition rate <strong>of</strong> <strong>the</strong> EuropeanXFEL to a variety <strong>of</strong> challenging scientific problems and to operating many experiments in parallelwill be introduced.70


Sunday 3 rd May, 11.30 – 12.30Round table discussion (coordinator: J. Marangos):Future Challenges and Prospects forUltra-Fast Dynamics Imaging.71


List <strong>of</strong> ParticipantsPeter Abbamonte University <strong>of</strong> Illinois abbamonte@mrl.uiuc.eduMartin Aeschlimann University <strong>of</strong> Kaiserslautern ma@physik.uni-kl.deCarlo Altucci University <strong>of</strong> Naples "Federico II" caltucci@unina.itMuhammadTanveerBaig University <strong>of</strong> Siegen tanveer_pucit@yahoo.comSarah Baker Imperial College London sarah.baker@imperial.ac.ukLuis Banares Universidad Complutense de Madrid banares@quim.ucm.esDavid Bartram Imperial College London david.bartram@gmail.comJulienBeaudoinBertrandUniversity <strong>of</strong> Ottawajulien.bertrand@nrc.caDavideBoschettoLaboratoire d'Optique Appliquée, ENSTA/EcolePolytechniquedavide.boschetto@ensta.frSebastien Boutet SLAC National Accelerator Laboratory sboutet@slac.stanford.eduFrancesca Calegari Politecnico di Milano francesca.calegari@polimi.itMajed Chergui EPFL - LSU majed.chergui@epfl.chPaul Corkum University <strong>of</strong> Ottawa Paul.Corkum@nrc.caPietro Paolo Corso Università di Palermo corso@fisica.unipa.itJohn Costello Dublin City University john.costello@dcu.ieDelphine Darios Imperial College London delphine.darios@imperial.ac.ukRebeca de Nalda Instituto de Quimica Fisica Rocasolano (CSIC) r.nalda@quim.ucm.esZsolt Diveki CEA-Saclay zsolt.diveki@cea.frReinhard Dörner Institut für Kernphysik, University <strong>of</strong> Frankfurt doerner@atom.uni-frankfurt.deHermann Dürr Helmholtz Zentrum Berlin hermann.duerr@bessy.deFederico Ferrari Politecnico di Milano federico.ferrari@mail.polimi.itCarla F. M. Faria University College London c.faria@ucl.ac.ukEmilio Fiordilino Università di Palermo fiordili@fisica.unipa.it72


Gregory Gitzinger Consejo Superior de Investigaciones Cientificas coach_gg83@hotmail.comSiegfried Glenzer Lawrence Livermore National Laboratory glenzer1@llnl.govKenichi Ishikawa RIKEN ishiken@riken.jpMisha Ivanov Imperial College London m.ivanov@imperial.ac.ukMossy Kelly Dublin City University mossy.kelly@gmail.comReinhard Kienberger Max Planck Institute <strong>of</strong> Quantum Optics reinhard.kienberger@mpq.mpg.deJoukoKorppi-TommolaUniversity <strong>of</strong> Jyväskyläktommola@jyu.fiManfred Lein University <strong>of</strong> Kassel lein@physik.uni-kassel.deFranck Lépine LASIM/CNRS lepine@lasim.univ-lyon1.frAnne L'Huillier Lund University Anne.LHuillier@fysik.lth.seChii-Dong Lin Kansas State University cdlin@phys.ksu.eduMatteo Lucchini Politecnico di Milano matteo.lucchini@mail.polimi.itBarbara Mansart Laboratoire de Physique des Solides mansart@lps.u-psud.frJon Marangos Imperial College London j.marangos@imperial.ac.ukMoritz Meckel Institut fuer Kernphysik, Univ. Frankfurt meckel@atom.uni-frankfurt.deIan Mercer University College Dublin ian.mercer@ucd.ieMarco Micciarelli University <strong>of</strong> Naples "Federico II" marco.miccia@libero.itKatsumi Midorikawa RIKEN kmidori@riken.jpDwayne Miller University <strong>of</strong> Toronto dmiller@lphys.chem.utoronto.caStefano Orlando CNR - IMIP stefano.orlando@imip.cnr.itClaudio Pellegrino Department <strong>of</strong> Physics and Astronomy, UCLA cpellegrini@roadrunner.comImmacolata Procino University College London i.procino@ucl.ac.ukVincent Richardson Dublin City University vincent.richardson2@mail.dcu.ieJoerg Rossbach University <strong>of</strong> Hamburg & DESY joerg.rossbach@desy.deValerio Rossi Albertini National Research Council valerio.rossi@artov.ism.cnr.it73


Jan Michael Rost MPI for <strong>the</strong> Physics <strong>of</strong> Complex Systems rost@pks.mpg.deCamilo Ruiz University <strong>of</strong> Salamanca camilo@usal.esHir<strong>of</strong>umi Sakai University <strong>of</strong> Tokyo hsakai@phys.s.u-tokyo.ac.jpPascal Salieres CEA-Saclay pascal.salieres@cea.frGiuseppe Sansone Politecnico di Milano giuseppe.sansone@polimi.itAndrew Shiner National Research Council andrew.shiner@nrc.caOlgaSmirnovaMax-Born-Institute for Nonlinear Optics andShort pulse Spectroscopyolga.smirnova@mbi-berlin.deEmma Springate STFC Ru<strong>the</strong>rford Appleton Lab emma.springate@stfc.ac.ukHenrik Stapelfeldt University <strong>of</strong> Aarhus henriks@chem.au.dkJoachim Stohr Stanford University and SLAC stohr@slac.stanford.eduRoxana Tarkeshian Desy roxana.tarkeshian@desy.deJohn Tisch Imperial College London john.tisch@imperial.ac.ukValer Tosa Natl. Inst. R&D Isotopic Molecular Technologies tosa@itim-cj.roThomas Tschentscher European XEL thomas.tschentscher@xfel.euKiyoshi Ueda Tohoku University ueda.kiyoshi@gmail.comJens Uhlig Lund University jens.uhlig@chemphys.lu.seJoachim Ullrich Max-Planck-Institut für Kernphysik c.ries@mpi-hd.mpg.deRaffaele Velotta University <strong>of</strong> Naples "Federico II" rvelotta@unina.itDavid Villeneuve National Research Council david.villeneuve@nrc.caCaterina Vozzi Politecnico di Milano caterina.vozzi@polimi.itPeter Wochner Max-Planck-Institute for Metals Research wochner@mf.mpg.deHans Jakob Wörner National Research Council Hans.Worner@nrc.ca74

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