Long-lived quantum coherences in a V -type system strongly driven by a thermal environment

Abstract

We explore the coherent dynamics of a three-level $\mathsf{V}$-type system interacting with a thermal bath in the regime where thermal excitation occurs much faster than spontaneous decay. We present analytic solutions of the Bloch-Redfield quantum master equations, which show that strong incoherent pumping can generate long-lived quantum coherences among the excited states of the $\mathsf{V}$-type system in the overdamped regime defined by the condition $\mathrm{\ensuremath{\Delta}}/(\overline{n}\ensuremath{\gamma})<f(p)$, where $\mathrm{\ensuremath{\Delta}}$ is the excited-state level splitting, $\ensuremath{\gamma}$ is the spontaneous decay rate, $\overline{n}\ensuremath{\gg}1$ is the effective photon occupation number proportional to the pumping intensity, and $f(p)$ is a universal function of the transition dipole alignment parameter $p$. In the limit of nearly parallel transition dipoles ($p\ensuremath{\rightarrow}1$) the coherence lifetime ${\ensuremath{\tau}}_{c}=1.34(\overline{n}/\ensuremath{\gamma}){(\mathrm{\ensuremath{\Delta}}/\ensuremath{\gamma})}^{\ensuremath{-}2}$ scales linearly with $\overline{n}$ and is enhanced by the factor $0.67\overline{n}$ with respect to the weak-pumping limit [Phys. Rev. Lett. 113, 113601 (2014); J. Chem. Phys. 144, 244108 (2016)]. We also establish the existence of long-lived quasistationary states, which occur in the overdamped regime and affect the process of thermalization of the $\mathsf{V}$-type system with the bath, slowing down the approach to thermal equilibrium. In the case of nonparallel transition dipole moments ($p<1$), no quasistationary states are formed and the coherence lifetime decreases sharply. The sharp transition between the different regimes of coherent dynamics is due to an interplay between coherence-generating Fano interference and various coherence-destroying processes (such as stimulated decay). Using a newly developed effective decoherence rate model, we find that in the limit $p\ensuremath{\rightarrow}1$ the rates of coherence generation and decay are almost exactly balanced and the effective decoherence rate is minimized, leading to long coherence lifetimes. Our results reveal new regimes of long-lived quantum coherent dynamics, which could be observed in thermally driven atomic and molecular systems.