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Electric-Field Fluctuations as the Cause of Spectral Instabilities in Colloidal Quantum Dots
Frieder Conradt1, Vincent Bezold1, Volker Wiechert1
1Department of Physics and Center for Applied Photonics, University of Konstanz, D-78457 Konstanz, Germany.
Abstract:
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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To explain the observed behavior of transition metal complexes (such as colors), a model involving electrostatic interactions between the electrons from the ligands and the electrons in the unhybridized d orbitals of the central metal atom has been developed. This electrostatic model is crystal field theory (CFT). It helps to understand, interpret, and predict the colors, magnetic behavior, and some structures of coordination compounds of transition metals.
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