Observation of an Excitonic Quantum Coherence in CdSe Nanocrystals

Shuo Dong; Dhara Trivedi; Sabyasachi Chakrabortty; Takayoshi Kobayashi; Yinthai Chan; Oleg V. Prezhdo; Zhi Heng Loh

doi:10.1021/acs.nanolett.5b02786

Observation of an Excitonic Quantum Coherence in CdSe Nanocrystals

Shuo Dong, Dhara Trivedi, Sabyasachi Chakrabortty, Takayoshi Kobayashi, Yinthai Chan^*, Oleg V. Prezhdo, Zhi Heng Loh

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

29 Citations (Scopus)

Abstract

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.

Original language	English
Pages (from-to)	6875-6882
Number of pages	8
Journal	Nano Letters
Volume	15
Issue number	10
DOIs	https://doi.org/10.1021/acs.nanolett.5b02786
Publication status	Published - Oct 14 2015
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2015 American Chemical Society.

ASJC Scopus Subject Areas

Bioengineering
General Chemistry
General Materials Science
Condensed Matter Physics
Mechanical Engineering

Keywords

charge migration
electron-phonon coupling
Electronic coherence
femtosecond optical spectroscopy
non-Born-Oppenheimer dynamics
quantum dots

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10.1021/acs.nanolett.5b02786

Cite this

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title = "Observation of an Excitonic Quantum Coherence in CdSe Nanocrystals",

abstract = "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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author = "Shuo Dong and Dhara Trivedi and Sabyasachi Chakrabortty and Takayoshi Kobayashi and Yinthai Chan and Prezhdo, {Oleg V.} and Loh, {Zhi Heng}",

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T1 - Observation of an Excitonic Quantum Coherence in CdSe Nanocrystals

AU - Dong, Shuo

AU - Trivedi, Dhara

AU - Chakrabortty, Sabyasachi

AU - Kobayashi, Takayoshi

AU - Chan, Yinthai

AU - Prezhdo, Oleg V.

AU - Loh, Zhi Heng

PY - 2015/10/14

Y1 - 2015/10/14

N2 - 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.

AB - 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.

KW - charge migration

KW - electron-phonon coupling

KW - Electronic coherence

KW - femtosecond optical spectroscopy

KW - non-Born-Oppenheimer dynamics

KW - quantum dots

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Observation of an Excitonic Quantum Coherence in CdSe Nanocrystals

Abstract

Bibliographical note

ASJC Scopus Subject Areas

Keywords

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