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CAS proceedings

Fluorescence and fluorescence quenching in a two-level system

Titus Sandu

Published Oct 1, 2014• 1 citation
Publisher

Abstract

Usually, fluorescence of a two-level system increases with the coupling strength to an electromagnetic field. However, we show numerically that the fluorescence is quenched in the ultra-strong coupling limit of a two-level system interacting with an electromagnetic field. This behavior is attributed to the onset of multi-photon processes which occur for the ultra-strong coupling between the two-level system and the electromagnetic field.

DOI
10.1109/smicnd.2014.6966457

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Usually, fluorescence of a two-level system increases with the coupling strength to an electromagnetic field. However, we show numerically that the fluorescence is quenched in the ultra-strong coupling limit of a two-level system interacting with an electromagnetic field. This behavior is attributed to the onset of multi-photon processes which occur for the ultra-strong coupling between the two-level system and the electromagnetic field.
We consider the possible physical processes that may arise in a three-level atom when only two of its levels interact with a strong electromagnetic field and when the atomic transition frequency is nearly equal to once and twice the frequency of the laser field, respectively. There have been found pronounced cooperative effects in the spectrum of the two-level system, which is in resonance with the laser field, arising from the presence of the third level. The excitation spectra describing the transitions from the first excited state into the second excited state and from that to the ground state consist, apart from the two central peaks, of two pairs of sidebands which are induced by the laser field of the neighbouring system. Detailed expressions of the spectral functions for the physical processes of one- and two-photon resonance fluorescence have been derived and discussed in the limit of high photon densities. The excitation spectrum of the low frequency modes has been considered and discussed in detail. It is found that quantum beats in spontaneous emission may appear in the spectra of the one- and two-photon resonance fluorescence arising from the interference between the two atomic transition frequencies and the frequency of the laser field. The importance of the low frequency modes that occur in the processes in question has been pointed out.
We have studied the fluorescence spectra arising from the interaction of a three-level atom with two strong electromagnetic fields whose initially populated modes are equal to the two atomic transition frequencies, respectively. The Green's function formalism has been used to calculate the excitation spectrum of the system. An expression for the spectral function describing the excitation spectrum of the system has been derived in a closed form in the limit of high photon densities. Numerical computation of the expression for the spectral function indicates that at each transition frequency there may exist either one pair or two pairs or three pairs of sidebands, in addition to the central peak, depending upon the relative strength of the Rabi frequencies involved.
We study the time-resolved fluorescence spectrum in two-level systems interacting with an incident coherent field, both in the weak and intermediate coupling regimes. For a single two-level system in the intermediate-coupling case, as time flows, the spectrum develops distinct features that are not captured by a semiclassical treatment of the incident field. Specifically, for a field on resonance with the atomic transition energy, the usual Mollow spectrum is replaced by a four-peak structure, and for a frequency that is half of the atomic transition energy, the time-dependent spectrum develops a second-harmonic peak with a superimposed Mollow triplet. In the long-time limit, our description recovers results previously found in the literature. After analyzing why a different behavior is observed in the quantum and classical dynamics, the reason for the occurrence of a second-harmonic signal in a two-level system is explained via a symmetry analysis of the total (electron and photon) system and in terms of a three-level system operating in limiting regimes. We find an increased second-harmonic signal in an array of two-level systems, suggesting a superradiance-like enhancement for multiple two-level systems in cavity setups. Finally, initial explorative results are presented for two-level model atoms entering and exiting a cavity, which hint at an interesting interplay between cavity-photon screening and atomic dynamics effects.
Numerical simulations of stationary fluorescence spectra of molecular systems usually rely on the relation between the photon emission rate and the system’s dipole–dipole correlation function. However, research papers usually take this relation for granted, and standard textbook expositions of the theory of fluorescence spectra also tend to leave out this important relation. In order to help researchers with less theoretical training gain a deeper understanding of the emission process, we perform a step-by-step derivation of the expression for the fluorescence spectrum, focusing on rigorous mathematical treatment and the underlying physical content. Right from the start, we employ quantum description of the electromagnetic field, which provides a clear picture of emission that goes beyond the phenomenological treatment in terms of the Einstein A coefficient. Having obtained the final expression, we discuss the relation of the latter to the present level of theory by studying a simple two-level system. From the technical perspective, the present work also aims at familiarizing the reader with the density matrix formalism and with the application of the double-sided Feynman diagrams.