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Surface-Area Dependent Electron Transfer Between Isoenergetic 2D Quantum Wells and a Molecular Acceptor Benjamin T. Diroll, Igor Fedin, Pierre Darancet, Dmitri V. Talapin, and Richard D. Schaller J. Am. Chem. Soc., Just Accepted Manuscript • DOI: 10.1021/jacs.6b06572 • Publication Date (Web): 12 Aug 2016 Downloaded from http://pubs.acs.org on August 15, 2016
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Figure 1. (a) Absorption spectra and (b) transmission electron microscopy-derived histograms relating total particle surface area of the four examined zinc blende CdSe nanoparticle samples. (c) Jablonski diagram indicating that driving force for this experiment between the nanomaterials and methylviologen electron acceptor is constant, yet CT rates shown below systematically differ.
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by normalizing time-resolved PL traces such as in panel (a) at long times and subtracting the nanoparticle-only signal without MV. Curves are maintained in the same color in (a) and (b).
Figure 2. (a) Raw photoluminescence dynamics of large CdSe NPLs in solution upon the addition of increasing amounts of MV. Here, the MV concentration increases from 3.1 to 310 μM with corresponding faster decay dynamics. (b) Differenced data obtained
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𝜙𝑛 (𝑧) = √2⁄𝐿 cos(𝜋𝑛𝑧⁄𝐿) 𝜒𝑘 (𝜌) = 𝑒
𝑖𝜌.𝑘
⁄ √𝐿
𝜓 𝑆 ∝ 1/𝑆
𝛤 𝑆→𝐶𝑇 ∝ 2𝜋 ħ
|〈ψ𝐶𝑇 |𝑉|ψ𝑆 〉|2 ,
Figure 3. (a) Extracted bimolecular decay traces for the four samples. Thin lines represent exponential fits of the experimental data. (b) Bimolecular quenching lifetime (1/kCT) versus per particle surface area. The dotted line relates a quadratic dependence. Inset shows the charge transfer rate plotted versus surface area. Horizontal error bars represent the standard deviation of nanoplatelet areas; vertical error bars represent fitting error. μ
𝜏𝑛=1 ⁄𝑛2
𝜏𝑛 =
𝜓𝑆 = 𝜙𝑐 (𝑧𝑒 )𝜙𝑣 (𝑧ℎ )𝜒𝑘 (𝜌𝑒 )𝜒𝑘 (𝜌ℎ )ξ(|𝜌𝑒 − 𝜌ℎ |, 𝑧𝑒 , 𝑧ℎ )
𝜙𝑐/𝑣
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Figure 4. (a) Temperature-dependent absorption spectra collected on a NPL film. Inset shows the integrated absorption of the first excitonic absorption versus temperature determined by Gaussian fitting. (b) Peak energy of the first excitonic absorption versus temperature (open circles) with a Varshni fit (solid line).
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