CHEM01200604009 Sreejith Kaniyankandy - Homi Bhabha ...

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141 samples due to a very weak exciton-phonon coupling in these cases. While the information regarding recombination dynamics have been instructive in ascertaining the role of shell in improving charge separation behaviour, complete understanding on carrier dynamics is not obtained just from radiative recombination as we neglect information on the nonradiative processes which often come from defects. To ascertain role of nonradiative processes we have carried out femtosecond transient absorption. 5.3.4. Transient absorption spectroscopy of CdSe QD: To understand further details about the dynamics of both radiative and non-radiative and charge transfer dynamics in CdSe/ZnTe core-shell QD, we have carried out transient absorption studies on both CdSe QD and CdTe/ZnTe core-shell by exiting the samples at 400nm light and monitoring the transients in the visible region. Figure 5.6 shows the transient absorption spectra of photoexcited CdSe QD materials in different time delay, which comprises a negative absorption band in 460 nm to 540 nm region and a broad positive absorption band in 550 nm – 700 nm region. The first exciton position for the CdSe core samples (Figure 3a) appear ~ 455nm, however in the transient spectrum we could show only second half of exciton bleach due to very low intensity of probe light in white light in the present experimental set-up. In steady state absorption spectrum of CdSe QD we have observed exciton peak at 455nm. Similarly, we observed bleach peak below 560nm in transient spectrum of CdSe QD. In our earlier investigations [5.20] we have described that bleach in transient spectrum of CdTe was due to state filling effect. In the present investigation also we can conclude that bleach feature in the transient spectrum is due to the ground state population depletion. The transient positive absorption beyond 550 nm regions
142 can be attributed to absorption of light by photo-generated charge carriers (both electrons and holes) in free or in trapped in the defect states of QDs. In addition to that positive absorption can also arise due to non-linear effects like two electron-hole pair interaction (bi-exciton effect) and trapped-carrier induced stark effect. To exclude these many-particle interactions we have recorded the transient data at low pump intensity so that average number of electron-hole pair (N eh >) is less than 1. 0 A(mOD) -1 -2 0.1ps 0.4ps 1ps 5ps 10ps 80ps A(mO.D) 0.5 0.0 0 5 100 200 Delay Time (ps) 450 500 550 600 650 700 Wavelength (nm) Figure 5.6: Transient absorption spectra of CdSe quantum dot (QD) at different time delay after excitation at 400 nm laser light. Inset: Kinetic decay trace monitored at 690 nm. Furthermore the stark effect induced absorption feature is highly unlikely as the feature shown is broad whereas stark effect induced features are expected to lie on the either side close to the exciton feature, also we have maintained N
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Charge Transfer Dynamics in Quantum
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DECLARATION I, hereby declare that
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ACKNOWLEDGEMENTS It is my privilege
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1.3.5. Defect Mediated Relaxation 2
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2. 8. 4. White Light Generation- 45
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6.2. Experimental 6.2.1.Synthesis o
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devices based on QDs it has been sh
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Furthermore generation of pump (~40
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shell). This clearly indicated that
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12. V. I. Klimov, J. Phys. Chem. B,
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1.13 Reactant and Product Potential
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light. Inset: Kinetic traces monito
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6.5 Transient decay kinetics of gra
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at 670 nm after exciting at 400 nm
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ABBREVIATIONS BET BQ CB CCD CdS CdT
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1 Chapter 1
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3 size dependent optical properties
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5 1.2. Physics of Semiconductors 1.
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7 As seen from the schematic, poten
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9 Substituting this in Schrödinger
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11 ( r, r ) ( r ) ( r ) (1.13) e
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13 E E E 2 2 2 EX ne, le nh,
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15 spherical symmetry of field. The
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17 gE ( ) 2Em 2 3 3 (1.25) For a
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19 1.3.2. Electron-Hole energy tran
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21 Impact Ionization Figure 1.7. Sc
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23 understanding on mechanistic asp
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25 carriers are unable to sample th
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27 CB VB QD Metal Figure. 1. 10. Sc
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29 energy barrier. Therefore it is
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31 1 f q 2 A qB (1.30) 2 In equa
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33 Vibrational contribution can be
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35 1. 7. 1. Electron Injection ET i
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37 Under assumption of invariance o
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39 distribution. To achieve good si
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41 initially achieved monodispersit
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43 and rate of charge transfer acro
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45 1.32 P. V. Kamat, J. Phys. Chem.
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47 Chapter 2
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49 chemical species. Since a partic
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51 fluorescence forms an important
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53 eliminated by use of standard wh
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55 sample. Raman spectroscopy is ba
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57 will appear bright and region wi
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59 volatile solvent is drop casted
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61 spots arise from diffraction fro
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63 The electrical signal is then ch
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65 delayed and inverted. The two si
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67 Pump-probe technique is one of t
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69 Amplifier Jade Stretcher fs Osci
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71 Figure 2.6. Optical layout of Ti
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73 Grating Convex Mirror Concave Mi
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75 changes the polarization from ho
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77 Grating Output Input Mirror Grat
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79 μJ has a very high peak power.
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81 2.6. Dynamical Theory of X-Ray D
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83 Chapter 3
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85 Therefore the study of interfaci
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87 3. 2. Experimental Section 3.2.1
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89 and intensity show absence of ot
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91 which is also neutral; therefore
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93 electron transfer times. This re
Page 138 and 139: 95 r B a * 0 3.1 me / me Now the
Page 140 and 141: 97 nonadiabatic case the electron t
Page 142 and 143: 99 drastically reduced leading to a
Page 144 and 145: 101 While the study of injection dy
Page 146 and 147: 103 study. Based on the injection d
Page 148 and 149: 105 17. L. E. Brus, J. Phys. Chem.
Page 151: 107 Chapter 4
Page 154 and 155: 109 of the QDs. As a result surface
Page 156 and 157: 111 4.2.2. Synthesis: The CdTe QDs
Page 158 and 159: 113 lower hole state. In CdSe the l
Page 160 and 161: 115 4.2 inset. The kinetic traces a
Page 162 and 163: 117 growth of the bleach kinetics (
Page 164 and 165: 119 previous section we have discus
Page 166 and 167: 121 lived charge transfer complex w
Page 168 and 169: 123 100 times concentration of the
Page 170 and 171: 125 4.5. References 4.1. Efros, Al.
Page 173: 127 Chapter 5
Page 176 and 177: 129 been made in the synthesis of t
Page 178 and 179: 131 metallic synthesis by arrested
Page 180 and 181: 133 5.3. Result and discussion: 5.3
Page 182 and 183: 135 indicating a confinement induce
Page 184 and 185: 137 absorption studies that on form
Page 186 and 187: 139 1000 c b PL Intensity 100 10 a
Page 190 and 191: 143 dynamical spectrum is negligibl
Page 192 and 193: 145 Earlier authors [5.4] reported
Page 194 and 195: 147 Sample t r(ps) t 1(ps) t 2(ps)
Page 196 and 197: 149 In addition to the cooling dyna
Page 198 and 199: 151 pulse-width time scale followed
Page 200 and 201: 153 5.20. Sreejith Kaniyankandy, Sa
Page 203 and 204: 155 CHAPTER 6 Charge Separation in
Page 205 and 206: 157 Studies by Wang et. al. [6.15]
Page 207 and 208: 159 graphene in a 1M NaOH solution.
Page 209 and 210: 161 Intensity (a.u.) 5 4 3 2 1 CdTe
Page 211 and 212: 163 dynamics of graphene oxide and
Page 213 and 214: 165 GO as shown in the Figure 3 rev
Page 215 and 216: 167 electron acceptor for Graphene.
Page 217 and 218: 169 governs the recombination dynam
Page 219 and 220: 171 Sample τ 1 (ps) τ 2 (ps) τ 3
Page 221 and 222: 173 A (mO.D) 10.0 0.0 -10.0 -20.0 0
Page 223 and 224: 175 involved in the relaxation may
Page 225 and 226: 177 Electron quencher (benzoquinone
Page 227 and 228: 179 Scheme 6.1. Schematic of Electr
Page 229 and 230: 181 6.6. Reina, A.; Jia, X.; Ho, J.
Page 231: 183 6.26. Kaiser, A. B.; Navarro, C
Page 234 and 235: 185 assigned to injection into diff
Page 236 and 237: 187 transfer from CdSe core to ZnTe
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189 However the position of bands i
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