Electric-Field Fluctuations as the Cause of Spectral Instabilities in Colloidal Quantum Dots

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Nano Letters. ACS Publications. 2023, 23(21), pp. 9753-9759. ISSN 1530-6984. eISSN 1530-6992. Available under: doi: 10.1021/acs.nanolett.3c02318
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Spectral diffusion (SD) represents a substantial obstacle toward implementation of solid-state quantum emitters as a source of indistinguishable photons. By performing high-resolution emission spectroscopy for individual colloidal quantum dots at cryogenic temperatures, we prove the causal link between the quantum-confined Stark effect and SD. Statistically analyzing the wavelength of emitted photons, we show that increasing the sensitivity of the transition energy to an applied electric field results in amplified spectral fluctuations. This relation is quantitatively fit to a straightforward model, indicating the presence of a stochastic electric field on a microscopic scale, whose standard deviation is 9 kV/cm, on average. The current method will enable the study of SD in multiple types of quantum emitters such as solid-state defects or organic lead halide perovskite quantum dots, for which spectral instability is a critical barrier for applications in quantum sensing.

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ISO 690CONRADT, Frieder, Vincent BEZOLD, Volker WIECHERT, Steffen HUBER, Stefan MECKING, Alfred LEITENSTORFER, Ron TENNE, 2023. Electric-Field Fluctuations as the Cause of Spectral Instabilities in Colloidal Quantum Dots. In: Nano Letters. ACS Publications. 2023, 23(21), pp. 9753-9759. ISSN 1530-6984. eISSN 1530-6992. Available under: doi: 10.1021/acs.nanolett.3c02318
BibTex
@article{Conradt2023-10-23Elect-68925,
  year={2023},
  doi={10.1021/acs.nanolett.3c02318},
  title={Electric-Field Fluctuations as the Cause of Spectral Instabilities in Colloidal Quantum Dots},
  number={21},
  volume={23},
  issn={1530-6984},
  journal={Nano Letters},
  pages={9753--9759},
  author={Conradt, Frieder and Bezold, Vincent and Wiechert, Volker and Huber, Steffen and Mecking, Stefan and Leitenstorfer, Alfred and Tenne, Ron}
}
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