Light-induced processes in nature: Coherences in the establishment of the nonequilibrium steady state in model retinal isomerization

J Chem Phys. 2019 May 14;150(18):184304. doi: 10.1063/1.5092981.

Abstract

Dynamics and coherences in retinal isomerization are investigated in a standard two-mode two-state model irradiated by natural incoherent light using the Markovian partial-secular Bloch-Redfield formalism. The two-mode two-state model is a minimal model of retinal that considers vibronic states on a ground and excited electronic manifold coupled to two continuous Ohmic harmonic baths. All light-induced coherent oscillations are shown to disappear as the turn-on time becomes realistically slow. Rather, an interplay between incoherent-light induced coherences and environmentally induced coherences is exposed as the system approaches a nonequilibrium steady state. The dynamics of the system reveal stable steady state coherences under realistic conditions, producing a small but robust transient enhancement of quantum yield.