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VII.CONCLUDING REMARKSThe combination of optical spectroscopy and scanning tunneling microscopyis proven to be a highly effective approach for studying the elctronic structureand tunneling transport properties of semiconductor nanocrystal QDs. Theatomiclike nature of the QDs is borne out both from the observation of theAufbau principle for sequential single-electron tunneling through the QDstates as well as from direct imaging of the quantum-confined envelope wavefunctions. Extending the atomic analogy further to include spin correlationeffects (e.g., Hund’s rule) will require the incorporation of magnetic fields inthe tunneling experiments. The methodology of combining optical andtunneling spectroscopy can also be extended to the study of artificial QDsolids such as close-packed superlattices of nanocrystals. Here, the discreteatomiclike QD states could evolve into miniband bulklike structures. Understandingthe level structure and tunneling transport properties is also essentialfor nanocrystal-based-device applications. Of particular relevance is theimplementation of nanocrystals in room-temperature single-electron optoelectronictunneling devices. Due to the small size, these QDs lie well withinthe strong confinement regime, and both the level spacings and the singleelectron charging energies are larger than k B T even at room temperature. Thecontrol of the relative contributions of the level structure and the chargingeffects will be an important ingredient in future QD devices.ACKNOWLEDGMENTSWe would like to thank Y.-W. Cao, S.-H. Kan, and D. Katz for theirimportant contributions to the work presented in this chapter. We also thankO. Agam, U. Landman, Y. Levi, Y.-M. Niquet, A. Sharoni, and A. Zungerfor stimulating discussions and suggestions. The work was supported in partby the Israel Academy of Science and Humanities and by Intel-Israel.REFERENCES1. Alivisatos, A.P. Science 1996, 271, 933.2. Brus, L.E. Appl. Phys. A 1991, 53, 465.3. Weller, H. Angew. Chem. Int. Ed. Engl. 1993, 32, 41.4. Nirmal, M.; Brus, L. Acc. Chem. Res. 1999, 32, 407.5. Collier, C.P.; Vossmeyer, T.; Heath, J.R. Annu Rev. Phys. Chem. 1998, 49, 371.6. Brus, L.E. J. Chem. Phys. 1984, 80, 4403.Copyright 2004 by Marcel Dekker, Inc. All Rights Reserved.
7. Grabert, H.; Devoret, M.H., Eds. In Single Charge Tunneling; Plenum: NewYork, 1992.8. Averin, D.V.; Likharev, K.K. In Mesoscopic Phenomena in Solids; Altshuler,B.L., Lee, P.A., Webb, R.A., Eds.; Elsevier: Amsterdam, 1991; 173 pp.9. Banin, U.; Cao, Y.W.; Katz, D.; Millo, O. Nature 1999, 400, 542.10. Klimov, V.I.; Mikhailovsky, A.A.; Xu, S.; Malko, A.; Hollingsworth, J.A.;Leatherdale, C.A.; Eisler, H.J.; Bawendi, M.G. Science 2000, 290, 314.11. Kazes, M.; Lewis, D.Y.; Ebenstein, Y.; Mokari, T.; Banin, U. Adv. Mater.2002, 14, 317.12. Colvin, V.L.; Schlamp, M.C.; Alivisatos, A.P. Nature 1994, 370, 354.13. Dabboussi, B.O.; Bawendi, M.G.; Onitsuka, O.; Rubner, M.F Appl. Phys.Lett. 1995, 66, 1316.14. Bruchez, M.P.; Moronne, M.; Gin, P.; Weiss, S.; Alivisatos, A.P. Science 1998,281, 2013.15. Chan, W.C.W.; Nie, S. Science 1998, 281, 2016.16. Mitchell, G.P.; Mirkin, C.A.; Letsinger, R.L. J. Am. Chem. Soc. 1999, 121, 8122.17. Brodie, I.; Muray, J.I. The Physics of Nano-Fabrication; Plenum: New York,1992.18. Leon, R.; Petroff, P.M.; Leonard, D.; Fafard, S. Science 1995, 267, 1966.19. Grundmann, M.; Christen, J.; Ledentsov, N.N., et al. Phys. Rev. Lett. 1995, 74,4043.20. Murray, C.B.; Norris, D.J.; Bawendi, M.G. J. Am. Chem. Soc. 1993, 115, 8706.21. Guzelian, A.A.; Banin, U.; Kadavanich, A.V.; Peng, X.; Alivisatos, A.P. Appl.Phys. Lett. 1996, 69, 1432.22. Mews, A.; Eychmu¨ller, A.; Giersig, M.; Schoos, D.; Weller, H. J. Phys. Chem.1994, 98, 934.23. Peng, X.; Wickham, J.; Alivisatos, A.P. J. Am. Chem. Soc. 1998, 120, 5343.24. Cao, Y.W.; Banin, U. Angew. Chem. Int. Ed. Engl. 1999, 38, 3692.25. Katari, J.E.B; Colvin, V.L.; Alivisatos, A.P. J. Phys. Chem. 1994, 98, 4109.26. Murray, C.B., Kagan, C.R., Bawendi, M.G. Science, 270, 1335.27. Collier, C.P.; Vossmeyer, T.; Heath, J.R. Annu. Rev. Phys. Chem. 1998, 49, 371.28. Whetten, R.L.; Khoury, J.T.; Alvarez, M.M.; Murthy, S.; Vezmar, I.; Wang,Z.L.; Stephens, P.W.; Cleveland, C.L.; Luedtke, W.D.; Landman, U. Adv.Mater. 1996, 8, 428.29. Black, C.T.; Murray, C.B.; Sandstrom, R.L.; Sun, S. Science 2000, 260, 1131.30. Pileni, M.P. J. Phys. Chem. B 2001, 105, 3358.31. Alivisatos, A.P.; Johnson, K.P.; Peng, X.; Wilson, T.E.; Loweth, C.J.; Bruchez,M.P.; Schultz, P.G. Nature 1996, 382, 609.32. Hines, M.A.; Guyot-Sionnest, P.J. J. Phys. Chem. 1996, 100, 468.33. Peng, X.; Schlamp, M.C.; Kadavanich, A.V.; Alivisatos, A.P. J. Am. Chem.Soc. 1997, 119, 7019.34. Dabbousi, B.O.; Rodriguez-Viejo, J.; Mikulec, F.V.; Heine, J.R.; Mattoussi,H.; Ober, R.; Jensen, K.F.; Bawendi, M.G. Phys. Chem. B 1997, 101, 9463.35. Tian, Y.; Newton, T.; Kotov, N.A.; Guldi, D.M.; Fendler, J.H. J. Phys. Chem.1996, 100, 8927.Copyright 2004 by Marcel Dekker, Inc. All Rights Reserved.
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Copyright 2004 by Marcel Dekker, In
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This book covers several topics of
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esult, some exciting topics were no
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3. Fine Structure and Polarization
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9. III-V Quantum Dots and Quantum D
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ContributorsUri BaninThe Hebrew Uni
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1‘‘Soft’’ Chemical Synthesi
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structure of energy states leads to
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growth can proceed by Ostwald ripen
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Figure 3 Transmission electron micr
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Figure 4 Temporal evolution of the
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No. 26, are f85% (Fig. 6) [21]. Alt
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tion spectra and broad PL spectra.
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ing surface-to-volume ratio with di
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Figure 8 Photoluminescence spectra
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lattice mismatch. Such a large latt
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match between InAs and ZnS of f11%.
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successfully repeated for up to thr
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Under a different growth regime, on
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Figure 14 Atomic model of the CdSe
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‘‘Teardrop-shaped’’ particl
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Figure 17 High-resolution TEMs of C
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allows isolation of tetrapods in f8
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ligand concentrations yield a reduc
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een determined and quantitatively c
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tion volumes were also shown to be
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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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can contribute to the saturation of
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coupling between ‘‘volume’’
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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
Page 287 and 288: Figure 16 Photocurrent action spect
Page 289 and 290: decay with stretched exponential ki
Page 291 and 292: siderably larger than might be esti
Page 293 and 294: dispersing CdSe nanocrystal chromop
Page 295 and 296: memory and charge storage effects [
Page 297 and 298: all) of the optically excited elect
Page 299 and 300: composites of nanocrystals and conj
Page 301 and 302: 55. Asbury, J.B.; Hao, E.C.; Wang,
Page 303 and 304: 108. Morgan, N.Y.; Leatherdale, C.A
Page 305 and 306: The approaches to fabrication of se
Page 307 and 308: Figure 1 Experimental realization o
Page 309 and 310: Due to this voltage division, the m
Page 311 and 312: Figure 3 Simulated tunneling spectr
Page 313 and 314: electron charging. In both positive
Page 315 and 316: Figure 5 shows the typical features
Page 317 and 318: Figure 7 Map of levels for InAs nan
Page 319 and 320: Figure 8 Scanning electron microsco
Page 321 and 322: D CB = 0.31 eV is thus obtained. On
Page 323 and 324: Figure 11 Correlation of optical an
Page 325 and 326: atomistic approach based on pseudop
Page 327 and 328: charging indicated that the tunneli
Page 329 and 330: capacitance values were also kept t
Page 331 and 332: could not be detected in the QD/DT/
Page 333 and 334: Figure 18 Tunneling conductanceF sp
Page 335 and 336: data in the inset of Fig. 19 repres
Page 337: corresponding to the s-like wave fu
Page 341 and 342: 66. Su, B.; Goldman, V.J.; Cunningh
Page 343 and 344: dimensional confinement are created
Page 345 and 346: Figure 1 Transmission electron micr
Page 347 and 348: The room-temperature absorption and
Page 349 and 350: narrower in samples with larger mea
Page 351 and 352: GaInP 2 QDs from a plot of the squa
Page 353 and 354: crystal, indicating lattice-matched
Page 355 and 356: Figure 5 Evolution of Stranski-Kras
Page 357 and 358: Figure 7 Photoluminescence spectra
Page 359 and 360: Figure 8 Photoluminescence spectra
Page 361 and 362: C. Efficient Anti-Stokes Photolumin
Page 363 and 364: Because HF treatment has been shown
Page 365 and 366: Copyright 2004 by Marcel Dekker, In
Page 367 and 368: intensity of the PL when it is on a
Page 369 and 370: eV stems from recombining carriers
Page 371 and 372: Figure 16 Model to explain two-colo
Page 373 and 374: although this term is not rigorousl
Page 375 and 376: 10 ps (about an order of magnitude
Page 377 and 378: electron relaxation is inhibited an
Page 379 and 380: Figure 18 Transmission electron mic
Page 381 and 382: QDs, the nature of the QD capping s
Page 383 and 384: 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
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(viz. the absorbed light intensity)
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Figure 25Impact ionization in QDs.m
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prevent electron-hole recombination
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36. Miller, R.D.J.; McLendon, G.; N
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91. Vurgaftman, I.; Singh, J. Appl.
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139. Mićić, O.I.; Ahrenkiel, S.P.
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10Synthesis and Fabrication of Meta
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Figure 2 (A-C) Progression of HR-TE
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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
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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
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final irradiation product. At the s
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following the laser excitation appe
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36. Papavassiliou, G.C. Prog. Solid
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particles to expand. Because the he
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was frequency doubled in a 1-mm B-
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Figure 2 Frequency of the acoustic
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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
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Figure 7 (a) Transient bleach data
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that the particles with >80% Au hav
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3. Del Fatti, N.; Valle´e, F.; Fly
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