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Persistent Inter-Excitonic Quantum Coherence in CdSe Quantum Dots.


ABSTRACT: The creation and manipulation of quantum superpositions is a fundamental goal for the development of materials with novel optoelectronic properties. In this letter, we report persistent (~80 fs lifetime) quantum coherence between the 1S and 1P excitonic states in zinc-blende colloidal CdSe quantum dots at room temperature, measured using Two-Dimensional Electronic Spectroscopy. We demonstrate that this quantum coherence manifests as an intradot phenomenon, the frequency of which depends on the size of the dot excited within the ensemble of QDs. We model the lifetime of the coherence and demonstrate that correlated interexcitonic fluctuations preserve relative phase between excitonic states. These observations suggest an avenue for engineering long-lived interexcitonic quantum coherence in colloidal quantum dots.

SUBMITTER: Caram JR 

PROVIDER: S-EPMC3976995 | biostudies-literature | 2014 Jan

REPOSITORIES: biostudies-literature

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Persistent Inter-Excitonic Quantum Coherence in CdSe Quantum Dots.

Caram Justin R JR   Zheng Haibin H   Dahlberg Peter D PD   Rolczynski Brian S BS   Griffin Graham B GB   Fidler Andrew F AF   Dolzhnikov Dmitriy S DS   Talapin Dmitri V DV   Engel Gregory S GS  

The journal of physical chemistry letters 20140101 1


The creation and manipulation of quantum superpositions is a fundamental goal for the development of materials with novel optoelectronic properties. In this letter, we report persistent (~80 fs lifetime) quantum coherence between the 1S and 1P excitonic states in zinc-blende colloidal CdSe quantum dots at room temperature, measured using Two-Dimensional Electronic Spectroscopy. We demonstrate that this quantum coherence manifests as an intradot phenomenon, the frequency of which depends on the s  ...[more]

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