Journal
NANO LETTERS
Volume 15, Issue 10, Pages 6875-6882Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.5b02786
Keywords
Electronic coherence; quantum dots; femtosecond optical spectroscopy; electron-phonon coupling; charge migration; non-Born-Oppenheimer dynamics
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Funding
- NTU start-up grant
- A*Star Science and Engineering Research Council Public Sector Funding [122-PSF-0011]
- Nanyang Assistant Professorship
- U.S. National Science Foundation [CHE-1300118]
- National Research Foundation (NRF) Competitive Research Programme [NRF-CRP8-2011-07]
- NRF Singapore-Berkeley Research Initiative for Sustainable Energy (SinBer-RISE) CREATE Programme
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1530854] Funding Source: National Science Foundation
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Recent observations of excitonic coherences within photosynthetic complexes suggest that quantum coherences could enhance biological light harvesting efficiencies. Here, we employ optical pump-probe spectroscopy with few-femtosecond pulses to observe an excitonic quantum coherence in CdSe nanocrystals, a prototypical artificial light harvesting system. This coherence, which encodes the high-speed migration of charge over nanometer length scales, is also found to markedly alter the displacement amplitudes of phonons, signaling dynamics in the non-Born-Oppenheimer regime.
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