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Journal of Experimental and Theoretical Physics

Theory of Broadening of Spectral Lines and Nonradiative Transitions in Systems with Weak Coupling

Mikhail A. Krivoglaz

Published Jul 1, 1965• 2 citations
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A light-matter interaction modified by the material environment is one of the central topics in quantum electrodynamics. While a strong coupling between a single emitter and a cavity and the Markovian (exponential) relaxation regime are most straightforwardly covered by theory, real physical systems that include also various line broadening effects may possess a much more complicated behavior. Here we propose a theoretical framework to account for nonradiative interaction effects in emission in photonic and plasmonic cavities. The quantum electrodynamics model formulated via a stochastic Hamiltonian approach has been developed with nonradiative line broadening introduced via the Kubo oscillator model. The impact of competing radiative and nonradiative processes on the emitter dynamics has been studied, showing that nonradiative relaxations, having significant impact on processes in high-QQQ photonic cavities, are much less influential in the plasmonic regime. The developed theoretical framework is not restricted to the emitter in a cavity example, but represents a general tool for multiple stochastic Hamiltonian evolution, important for various types of interactions where either classical or quantum noise is present.
The simultaneous influence of homogeneous and inhomogeneous line-broadening mechanisms are investigated for a reference system embedded in a medium. An analytically solvable model is constructed which includes the interaction of the reference mode with N strongly coupled environmental states (causing an inhomogeneity) and weakly coupled bath states. The modulation of the reference mode is caused by transitions between the strongly coupled perturber states. These may be switched on with a different rate than they are switched off. Consequently, effects of energy of activation and the change in entropy for environmental transitions on the line shape can be analyzed. The spectral function as well as the relaxation function are discussed as a function of the relevant parameters such as the number of perturbers, the lifetime T1, the temperature, and transition rates.