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esult, some exciting topics were not covered here, including silicon-basednanostructures, magnetic nanocrystals, and nanocrystals in biology. Canham’sdiscovery of efficient light emission from porous silicon in 1990 hasgenerated a widespread research effort on silicon nanostructures (includingthat on silicon nanocrystals). This effort represents a very large field thatcould not be comprehensively reviewed within the scope of this book. Thesame reasoning applies to magnetic nanostructures and, specifically, tomagnetic nanocrystals. This area has been strongly stimulated by the needsof the magnetic storage industry. It has grown tremendously over the pastseveral years and probably warrants a separate book project. The connectionof nanocrystals to biology is relatively new, however, it already shows greatpromise. Semiconductor and metal nanoparticles have been successfullyapplied to tagging biomolecules. On the other hand, biotemplates have beenused for the assembly of nanoparticles into complex, multiscale structures.Along these lines, a very interesting topic is bio-inspired assemblies of nanoparticlesthat efficiently mimic various biofunctions (e.g., light harvesting andphotosynthesis). ‘‘Nanocrystals in Biology’’ may represent a fascinating topicfor some future review by a group of experts in biology, chemistry, andphysics.I would like to thank all contributors to this book for finding time intheir busy schedules to put together their review chapters. I gratefullyacknowledge M. A. Petruska and Jennifer A. Hollingsworth for help inediting this book. I would like to thank my wife, Tatiana, for her patience,tireless support, and encouragement during my research career and specificallyduring the work on this book.Victor I. KlimovCopyright 2004 by Marcel Dekker, Inc. All Rights Reserved.
ContentsPrefaceContributorsPart I. Semiconductor Nanocrystals (NanocrystalQuantum Dots)1. ‘‘Soft’’ Chemical Synthesis and Manipulationof Semiconductor NanocrystalsJennifer A. Hollingsworth and Victor I. KlimovI. IntroductionII. Colloidal NanosynthesisIII. Inorganic Surface ModificationIV. Shape ControlV. Phase Transitions and Phase ControlVI. Nanocrystal DopingVII. Nanocrystal Assembly and EncapsulationReferences2. Electronic Structure in Semiconductor NanocrystalsDavid J. NorrisI. IntroductionII. Theoretical FrameworkIII.IV.Cadmium Selenide NanocrystalsBeyond CdSeReferencesCopyright 2004 by Marcel Dekker, Inc. All Rights Reserved.
Page 1: Copyright 2004 by Marcel Dekker, In
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Page 6 and 7: Copyright 2004 by Marcel Dekker, In
Page 8 and 9: This book covers several topics of
Page 12 and 13: 3. Fine Structure and Polarization
Page 14 and 15: 9. III-V Quantum Dots and Quantum D
Page 16 and 17: ContributorsUri BaninThe Hebrew Uni
Page 18 and 19: 1‘‘Soft’’ Chemical Synthesi
Page 20 and 21: structure of energy states leads to
Page 22 and 23: growth can proceed by Ostwald ripen
Page 24 and 25: Figure 3 Transmission electron micr
Page 26 and 27: Figure 4 Temporal evolution of the
Page 28 and 29: No. 26, are f85% (Fig. 6) [21]. Alt
Page 30 and 31: tion spectra and broad PL spectra.
Page 32 and 33: ing surface-to-volume ratio with di
Page 34 and 35: Figure 8 Photoluminescence spectra
Page 36 and 37: lattice mismatch. Such a large latt
Page 38 and 39: match between InAs and ZnS of f11%.
Page 40 and 41: successfully repeated for up to thr
Page 42 and 43: Under a different growth regime, on
Page 44 and 45: Figure 14 Atomic model of the CdSe
Page 46 and 47: ‘‘Teardrop-shaped’’ particl
Page 48 and 49: Figure 17 High-resolution TEMs of C
Page 50 and 51: allows isolation of tetrapods in f8
Page 52 and 53: ligand concentrations yield a reduc
Page 54 and 55: een determined and quantitatively c
Page 56 and 57: tion volumes were also shown to be
Page 58 and 59: synthesis temperatures of z400jC ar
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Figure 23 (a) Photoluminescence spe
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levels (fV1 Mn per NQD). Despite in
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Figure 25 X-ray diffraction pattern
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Figure 27 Transmission electron mic
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An additional factor that strongly
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Figure 30 (a,b) Schematics illustra
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Slow, controlled precipitation of h
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Figure 34 Schematic illustrating th
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achieving biological compatibility
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47. Yu H.; Gibbons P.C.; Kelton K.F
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2Electronic Structure inSemiconduct
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Figure 2 (a) Simple model of a nano
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electron and hole to be treated as
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independently, Eq. (13) is commonly
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a better description of the bulk ba
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investigated. For optical experimen
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Figure 4 (a) Absorption (solid line
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Figure 6 Normalized PLE scans for s
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Figure 8 A simplistic model for des
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Figure 10 Theoretically predicted p
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Figure 12 Schematics depicting the
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Figure 14 Calculated band-edge exci
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Figure 15 Absorption (solid line) a
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Figure 18 (a) Calculated band-edge
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IV.BEYOND CdSeA. Indium Arsenide Na
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the six-band Luttinger Hamiltonian.
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11. Norris, D.J.; Efros, Al.L.; Ros
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69. Gaponenko, S.V.; Woggon, U.; Sa
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formation of a long-lived dark exci
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where the constant A is determined
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In crystals for which the function
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The respective wave functions areC
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passive, as was shown in Ref. 12. T
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square of the matrix element of the
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where e F = e F ieV and e F F = e x
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see that for all nanocrystal shapes
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optical recombination of the excito
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B. Recombination of the Dark Excito
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where x = cos h and f = l B g e H/3
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The theory of the polarization memo
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Figure 7 The size dependence of the
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state would have an infinite lifeti
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crystal axis [see Eq. (40)]. As a r
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time of the exciton momentum relaxa
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One must also account for the influ
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observed in one of the first studie
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REFERENCES1. Bawendi, M.G.; Wilson,
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4Intraband Spectroscopyand Dynamics
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The solid line in Fig. 1 shows the
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Figure 2 FTIR spectra of n-type CdS
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of the center frequency. The experi
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limit given by radiative relaxation
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from a long lifetime due to the pho
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are two natural approaches to study
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32. Inoshita, T.; Sakaki, H. Physic
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continuous spectral tunability over
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function and envelope function mome
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ottleneck’’ [14,28]. Further re
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in NQDs is dominated by nonphonon e
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Figure 4 Dynamics of the IR postpum
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Figure 5 (a) Time-resolved PL spect
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Figure 6 (a) The time delay of the
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and due to Auger-type e-h interacti
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Figure 9 Dynamics of the 1S bleachi
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significantly greater than the fast
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Figure 11 (a) Pump-intensity-depend
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NQD size. For small NQD sizes (R =
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Figure 14 Nonlinear absorption/gain
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sorption change associated with a s
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where n h em is the hole ‘‘emit
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ultrafast (subpicosecond to picosec
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Figure 18 Schematic of transitions
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Figure 19 Dynamics of pump-induced
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where n i (i=1, 2 . . . , N ) is th
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Figure 21 (a) Two-e-h-pair (biexcit
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the volume fraction (filling factor
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intensity dependence of this peak (
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Copyright 2004 by Marcel Dekker, In
Page 221 and 222:
can contribute to the saturation of
Page 223 and 224:
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coupling between ‘‘volume’’
Page 227 and 228:
numerous discussions on the photoph
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53. Kang, K.; Kepner, A.; Gaponenko
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the ‘‘on-off ’’ emission in
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parallel form of data acquisition i
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Figure 3 (a) Spectral time trace of
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transition energies. In fact, these
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distribution (dark line) does not d
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exposure to only room light. In our
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statistics for the off times are in
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230Shimizu and BawendiCopyright 200
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Figure 10 (a) Time trace of a CdSe(
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and excited QD core states to fluct
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arrows indicate the on-time truncat
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W. K. Woo and V. C. Sundar for assi
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size allows the electron affinity a
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II.THEORY OF ELECTRON TRANSFER BETW
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For the specific case of charge tra
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dominates, the mobility is often fi
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where the constant A and the temper
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components of modulation which are
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nanocrystals [41], understanding ph
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and ionization potential through tw
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quantum dots. Furthermore, because
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For many applications, a host mater
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form blends with morphologies that
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Figure 11 Photoluminescence efficie
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Figure 12 (a) Room-temperature PIA
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discussed briefly in Section IV. Ch
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dithiolates to thiol-terminated DNA
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Films of passivated CdSe nanocrysta
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Figure 16 Photocurrent action spect
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decay with stretched exponential ki
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siderably larger than might be esti
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dispersing CdSe nanocrystal chromop
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memory and charge storage effects [
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all) of the optically excited elect
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composites of nanocrystals and conj
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55. Asbury, J.B.; Hao, E.C.; Wang,
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108. Morgan, N.Y.; Leatherdale, C.A
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The approaches to fabrication of se
Page 307 and 308:
Figure 1 Experimental realization o
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Due to this voltage division, the m
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Figure 3 Simulated tunneling spectr
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electron charging. In both positive
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Figure 5 shows the typical features
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Figure 7 Map of levels for InAs nan
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Figure 8 Scanning electron microsco
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D CB = 0.31 eV is thus obtained. On
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Figure 11 Correlation of optical an
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atomistic approach based on pseudop
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charging indicated that the tunneli
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capacitance values were also kept t
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could not be detected in the QD/DT/
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Figure 18 Tunneling conductanceF sp
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data in the inset of Fig. 19 repres
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corresponding to the s-like wave fu
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7. Grabert, H.; Devoret, M.H., Eds.
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66. Su, B.; Goldman, V.J.; Cunningh
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dimensional confinement are created
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Figure 1 Transmission electron micr
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The room-temperature absorption and
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narrower in samples with larger mea
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GaInP 2 QDs from a plot of the squa
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crystal, indicating lattice-matched
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Figure 5 Evolution of Stranski-Kras
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Figure 7 Photoluminescence spectra
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Figure 8 Photoluminescence spectra
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C. Efficient Anti-Stokes Photolumin
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Because HF treatment has been shown
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intensity of the PL when it is on a
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eV stems from recombining carriers
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Figure 16 Model to explain two-colo
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although this term is not rigorousl
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10 ps (about an order of magnitude
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electron relaxation is inhibited an
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QDs, the nature of the QD capping s
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QD solution. For an interdot distan
Page 385 and 386:
emission spectra of the two individ
Page 387 and 388:
Figure 23 Change of the PL intensit
Page 389 and 390:
(viz. the absorbed light intensity)
Page 391 and 392:
Figure 25Impact ionization in QDs.m
Page 393 and 394:
prevent electron-hole recombination
Page 395 and 396:
36. Miller, R.D.J.; McLendon, G.; N
Page 397 and 398:
91. Vurgaftman, I.; Singh, J. Appl.
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139. Mićić, O.I.; Ahrenkiel, S.P.
Page 401 and 402:
10Synthesis and Fabrication of Meta
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Figure 2 (A-C) Progression of HR-TE
Page 405 and 406:
Figure 3 Schematic for gold nanocry
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Nanocrystal growth can occur by two
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on the other hand, provide an ensem
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Figure 6 (a) SAXS patterns for disp
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Figure 8 The gold nanocrystal film
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of the stabilizing ligand, and the
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successfully modeled the 2D island
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2. Steric Stabilization and a Soft
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are fully extended. Moving away fro
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Figure 11 High-resolution SEM image
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Figure 13 (A) Transmission electron
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function of the density of localize
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Figure 15 High-resolution SEM image
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thiol-capped nanocrystals [2]. The
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41. Ackerson, B.J. Nature 1993, 365
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with the effect of the particle com
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Figure 1a shows the surface plasmon
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Figure 2 (a) Ultraviolet-visible ab
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agents [34]. The short-wavelength b
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Figure 4 (a) Plot of the plasmon ab
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the framework of traditional Mie’
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show that effects due to the surrou
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is located at the position of the g
Page 451 and 452:
Page 453 and 454:
Figure 8 Ultraviolet-visible absorp
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laser pulses while being mixed in t
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Figure 10 shows HR-TEM images of go
Page 459 and 460:
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final irradiation product. At the s
Page 463 and 464:
following the laser excitation appe
Page 465 and 466:
36. Papavassiliou, G.C. Prog. Solid
Page 467 and 468:
particles to expand. Because the he
Page 469 and 470:
was frequency doubled in a 1-mm B-
Page 471 and 472:
Figure 2 Frequency of the acoustic
Page 473 and 474:
Figure 3 Change in radius (DR/R) ve
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In this model, the electrons couple
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Figure 5 Transient bleach data for
Page 479 and 480:
Figure 7 (a) Transient bleach data
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that the particles with >80% Au hav
Page 483 and 484:
3. Del Fatti, N.; Valle´e, F.; Fly
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