Journal
NANO LETTERS
Volume 13, Issue 11, Pages 5311-5315Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nl402820v
Keywords
Electron transfer; Marcus theory; molecular electronics; donor-bridge-acceptor; quantum dot sensitized solar cell; terahertz spectroscopy
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Funding
- Toyota Motor Europe NV/SA
- Max Planck Society
- Graduate School Materials Science in Mainz (MAINZ)
- German Research Foundation in the Excellence Initiative [GSC 266]
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Photoinduced electron transfer processes from semiconductor quantum dots (QDs) molecularly bridged to a mesoporous oxide phase are quantitatively surveyed using optical pump-terahertz probe spectroscopy. We control electron transfer rates in donor-bridge-acceptor systems by tuning the electronic coupling strength through the use of n-methylene (SH-[CH2](n)- COOH) and n-phenylene (SH-[C6H4](n)-COOH) molecular bridges. Our results show that electron transfer occurs as a nonresonant quantum tunneling process with characteristic decay rates of beta(n) = 0.94 +/- 0.08 and beta(n) = 1.25 per methylene and phenylene group, respectively, in quantitative agreement with reported conductance measurements through single molecules and self-assembled monolayers. For a given QD donor-oxide acceptor separation distance, the aromatic n-phenylene based bridges allow faster electron transfer processes when compared with n-methylene based ones. Implications of these results for QD sensitized solar cell design are discussed.
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