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Persistent interexcitonic quantum coherence in CdSe quantum dots

  • Author(s): Caram, JR
  • Zheng, H
  • Dahlberg, PD
  • Rolczynski, BS
  • Griffin, GB
  • Fidler, AF
  • Dolzhnikov, DS
  • Talapin, DV
  • Engel, GS
  • et al.

Published Web Location

https://doi.org/10.1021/jz402336t
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 the relative phase between excitonic states. These observations suggest an avenue for engineering long-lived interexcitonic quantum coherence in colloidal quantum dots. © 2013 American Chemical Society.

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