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Optics and Spectroscopy

The Effects of Local Environment on a Probe Signal Absorption and Resonance Fluorescence for Quantum Emitters in Transparent Media

E. A. Smirnova, Natalia A. Lozing, M. G. Gladush, А. В. Наумов

Published Sep 1, 2023• 0 citations
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Abstract

Abstract The current paper demonstrates theoretical analysis of two types of spectral curves for several configurations of system of two-level light emitters, considering the influence of local field and close environment inside a transparent medium. Probe field absorption spectra and resonant fluorescence spectra are calculated under excitation of a strong monochromatic cw laser. The sensitivity of absorption and emission optical spectroscopy method is compared for revealing the effects of the medium on individual emitters and their ensembles. Spectral curves were calculated for model emitters considering local field influence of a transparent dielectric medium and local electron-phonon interactions, which determined the response of the emitters to an external laser field and effective relaxation mechanisms. The calculation formalism is based on a semiclassical approach, while the relaxation processes associated with the phonon contribution are introduced phenomenologically with references to other studies.

DOI
10.1134/s0030400x23070159

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Abstract The current paper demonstrates theoretical analysis of two types of spectral curves for several configurations of system of two-level light emitters, considering the influence of local field and close environment inside a transparent medium. Probe field absorption spectra and resonant fluorescence spectra are calculated under excitation of a strong monochromatic cw laser. The sensitivity of absorption and emission optical spectroscopy method is compared for revealing the effects of the medium on individual emitters and their ensembles. Spectral curves were calculated for model emitters considering local field influence of a transparent dielectric medium and local electron-phonon interactions, which determined the response of the emitters to an external laser field and effective relaxation mechanisms. The calculation formalism is based on a semiclassical approach, while the relaxation processes associated with the phonon contribution are introduced phenomenologically with references to other studies.
The current paper demonstrates theoretical analysis of two types of spectral curves for several configurations of system of two-level light emitters, considering the influence of local field and close environment inside a transparent medium. Probe field absorption spectra and resonant fluorescence spectra are calculated under excitation of a strong monochromatic cw laser. The sensitivity of absorption and emission optical spectroscopy method is compared for revealing the effects of the medium on individual emitters and their ensembles. Spectral curves were calculated for model emitters considering local field influence of a transparent dielectric medium and local electron-phonon interactions, which determined the response of the emitters to an external laser field and effective relaxation mechanisms. The calculation formalism is based on a semiclassical approach, while the relaxation processes associated with the phonon contribution are introduced phenomenologically with references to other studies.
The current paper demonstrates theoretical analysis of two types of spectral curves for several configurations of system of two-level light emitters, considering the influence of local field and close environment inside a transparent medium. Probe field absorption spectra and resonant fluorescence spectra are calculated under excitation of a strong monochromatic cw laser. The sensitivity of absorption and emission optical spectroscopy method is compared for revealing the effects of the medium on individual emitters and their ensembles. Spectral curves were calculated for model emitters considering local field influence of a transparent dielectric medium and local electron-phonon interactions, which determined the response of the emitters to an external laser field and effective relaxation mechanisms. The calculation formalism is based on a semiclassical approach, while the relaxation processes associated with the phonon contribution are introduced phenomenologically with references to other studies.
The effect of macroscopic parameters of a substance on the optical characteristics of impurity particles is investigated. A generalized control equation is derived for two-level emitters forming an ensemble of optical centers in a transparent dielectric medium. In this equation, the effective values of the acting pump field and the radiative relaxation rate of an optical center are taken into account. The formalism developed here is a completely microscopic approach based on the chain of the Bogoliubov-Born-Green-Kirkwood-Yvon equations for reduced density matrices and correlation operators for material particles and modes of a quantized radiation field. The method used here makes it possible to take into account the effects of individual and collective behavior of emitters, which are associated with the presence of an intermediate medium, consistently without using phenomenological procedures. It is shown that the resultant analytic expression for the effective lifetime of the excited state of an optical center conforms with experimental data.
The applicability of the method for measuring the probe absorption and gain spectra in a system of quantum emitters excited by a resonant driving field for studying cooperative photoluminescence is considered. The gain and attenuation of a probe signal in the system of two quantum emitters with the dipole–dipole interaction have been calculated for the conditions of observing the cooperative photoluminescence of a pair of impurity molecules described in the literature and close to them. The resulting dependences demonstrate the structure of excited collective molecular states, which can be used to reconstruct the positions of molecules in a matrix and to determine the difference in their photophysical properties. Thus, the probe absorption and gain spectra can be used to analyze the photoluminescence of quantum-entangled particles and to transform light signals.