Environmental Nonadditivity and Franck-Condon physics in Nonequilibrium Quantum Systems

Phys Rev Lett. 2019 Aug 30;123(9):093601. doi: 10.1103/PhysRevLett.123.093601.

Abstract

We show that for a quantum system coupled to both vibrational and electromagnetic environments, enforcing additivity of their combined influences results in nonequilibrium dynamics that does not respect the Franck-Condon principle. We overcome this shortcoming by employing a collective coordinate representation of the vibrational environment, which permits the derivation of a nonadditive master equation. When applied to a two-level emitter our treatment predicts decreasing photon emission rates with increasing vibrational coupling, consistent with Franck-Condon physics. In contrast, the additive approximation predicts the emission rate to be completely insensitive to vibrations. We find that nonadditivity also plays a key role in the stationary nonequilibrium model behavior, enabling two-level population inversion under incoherent electromagnetic excitation.