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Spontaneous Emission from Resonance (Metastable) Electronic States

Amir Sivan, Meir Orenstein, Milan Šindelka, Nimrod Moiseyev

Published Jan 1, 2025• 0 citations
Publisher

Abstract

We expand the fundamental theory of light-matter interactions by rigorously deriving spontaneous emission from quantum resonance states. The generalized Fermi golden rule unveils nontrivial dependence between the photon lifetime and the native resonance decay.
DOI
10.1364/cleo_at.2025.jps200_42

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We demonstrate a fundamental breakdown of the photonic spontaneous emission (SE) formula derived from Fermi's golden rule, in absorptive and amplifying media, where one assumes the SE rate scales with the local photon density of states, an approach often used in more complex, semiclassical nanophotonics simulations. Using a rigorous quantization of the macroscopic Maxwell equations in the presence of arbitrary linear media, we derive a corrected Fermi's golden rule and master equation for a quantum two-level system (TLS) that yields a quantum pumping term and a modified decay rate that is net positive. We show rigorous numerical results of the temporal dynamics of the TLS for an example of two coupled microdisk resonators, forming a gain-loss medium, and demonstrate the clear failure of the commonly adopted formulas based solely on the local density of states.
Controlling transition rates is a central objective across quantum optics, condensed-matter physics, and chemical physics, encompassing processes such as spontaneous emission, energy and charge transfer, spin relaxation, and chemical reactions. Although Fermi's golden rule provides a powerful framework for calculating such rates of weakly coupled transitions, conventional calculations require the interaction to be specified in advance; the range of rate responses attainable over a broader interaction space remains unknown. We formulate spectral-overlap golden-rule rates as quadratic forms of the interaction and derive rigorous bounds on rate modulation over a specified interaction space. As an example, application to energy transfer from a donor to a molecular vibration coupled to an optical cavity reveals that enhancement and suppression depend jointly on the interaction and cavity detuning, including continuous reversal of the rate response for a fixed interaction. The same approach may elucidate rate control for other golden-rule processes, including excitation-energy transfer, nonadiabatic electron transfer, nonradiative electronic transitions, vibrational and spin relaxation, and spontaneous emission.