Körtzinger studies air-sea gas exchange and provides opportunities for large-scale surfacesampling from commercial volunteer observing ships (P4).<strong>The</strong> A6 JRG will apply state-of-the-art spectroscopic techniques to studies of the seawater-airinterface in the context of existing expertise in the areas identified in the diagram.4. ObjectivesA6 will investigate chemical structures and processes at and near the seawater-air interface asrelevant to changing air-sea chemical interactions of the future ocean. Research themes for the A6project team are: (1) halogen speciation/reactivity in the surface ocean, including interactions withorganic material and ozone; (2) photochemical cycling of dust-derived iron and consequences foriron bioavailability; (3) the role of organic films for these processes. Photochemistry and surfacelayerstructures exert strong control on the sea-to-air flux of key organo-iodine compounds (Richterand Wallace 2004), influence inorganic iodine concentrations and speciations (and hence ozoneuptake), are significant for Br chemistry and fluxes. Further, the speciation and reactivity of Br issensitive to future ocean pH change. Photochemically initiated metal-ligand redox reactionsinfluence the rapid dissolution of Fe aerosols in the upper ocean, thus affecting Fe availability tophytoplankton. Within this context, a new Junior Research Group will be established in the Instituteof Physical Chemistry of the University of Kiel. <strong>The</strong> JRG will develop and apply new experimentaltechniques to probe the water-air interface at molecular and supramolecular scales in the presenceof marine solutes, atmospheric gases, and monolayers or thin films of marine-typical organiccompounds. Combined with other gas and liquid-phase spectroscopies supplied by theproponents, time-dependent measurements will allow the JRG to elucidate the mechanisms andrates of surface reactions. <strong>The</strong> research of the JRG will address these overall A6 themes, but thespecific topics will depend on the choices, interests and expertise of the best qualified candidate.Specific work to be undertaken by the A6 project team, including the JRG, includes:• Setting up of laser-based surface-sensitive and liquid phase spectroscopic tools (vibrationalsum frequency spectroscopy (VSFS), second harmonic generation (SHG), evanescent wave(EW) cavity ringdown spectroscopy (CRDS)) for air-water interface studies55
• Field and laboratory investigations into the effects of future forcing changes on speciation andthe reactivity of halogens and iron close to the sea surface (including consideration of pHchange, ozone-iodide reactions, redox and speciation changes, quantum yields, solvent (cage)effects)• Measurements of radical, dimethylsulfide, and ozone reaction kinetics at the liquid surface(including quantitative monitoring of gas and liquid phase products, using quasi steady-stateand time-resolved (laser) photolysis, VSFS, EW-CRDS, LIF)• Structural and photochemical studies at and in organic monolayers and thin organic films onwater (including phospholipid microlayers and release of volatile organic compounds)• <strong>The</strong>oretical studies of the processes outlined above by ab initio quantum chemistry andreactions of (catalytically active) metals in water clusters and supplementary experimentsA6 will provide basic understanding relevant to A4 and A7 and will benefit from cross-fertilization ofexperimental and theoretical approaches with A5. Acidification effects research parallels work inA1, and iron chemistry has relevance for B2. <strong>The</strong>oretical work will use P1 and spectroscopicmethods arising from A6 can be integrated in P4.5. ReferencesAarts IMP, et al. (2005) Quasi-Ice Monolayer on Atomically Smooth Amorphous SiO 2 at RoomTemperature Observed with a High-Finesse Optical Resonator. Phys Rev. Lett. 95, 166104.Bianco R, Hynes JT (2006) Heterogeneous Reactions Important in Atmospheric Ozone Depletion:A <strong>The</strong>oretical Perspective. Acc. Chem. Res. 39, 159-165.Chang W, Heikes BG, Lee M (2004) Ozone deposition to the sea surface: chemical enhancementand wind speed dependence. Atmos. Environ. 38, 1053-1059.Lelieveld J, van Aardenne J, Fischer H, de Reus M, Williams J, Winkler P (2004) Increasing Ozoneover the Atlantic <strong>Ocean</strong>. Science 304, 1483-1487.Mucha M, Frigato T, Levering LM, Allen HC, Tobias DJ, Dang LX, Jungwirth P (2005) UnifiedMolecular Picture of the Surfaces of Aqueous Acid, Base, and Salt Solutions. J. Phys. Chem.B, 109, 7617-7623.von Glasow R, Crutzen PJ (2003) Tropospheric Halogen Chemistry. Chapter 2 in vol. 4 of Treatiseon Geochemistry edited by KK Turekian and HD Holland, p. 21 - 64.Richmond GL (2001) Structure and Bonding of Molecules at Aqueous Surfaces. Annu. Rev. Phys.Chem. 52, 357-389.Richter U, Wallace DWR (2004) Production of methyl iodide in the tropical Atlantic <strong>Ocean</strong>.Geophys. Res. Lett. 31, L23S03.Shen YR (1989) Surface properties probed by second-harmonic and sum-frequency generation.Nature 337, 519-525.Schulz F, Hartke B (2005) A New Proposal for the Reason of Magic Numbers in Alkali CationMicrohydration Clusters. <strong>The</strong>or. Chem. Acc. 114, 357-380.Thomas JL, et al. (2006) Gas-Phase Molecular Halogen Formation from NaCl and NaBr Aerosols:When Are Interface Reactions Important? J. Phys. Chem. A 110, 1859-1867.56
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Suess E, Torres ME, Bohrmann G, Col
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DEKLIMGerman Climate Research Progr
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ITQ’sISAISOSJRGKCMSKitzLALIFLIMSL
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f,rylheonRaytheon Anschütz GmbHPos