Abstract
We explore the coherent dynamics of a three-level -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 -type system in the overdamped regime defined by the condition , where is the excited-state level splitting, is the spontaneous decay rate, is the effective photon occupation number proportional to the pumping intensity, and is a universal function of the transition dipole alignment parameter . In the limit of nearly parallel transition dipoles () the coherence lifetime scales linearly with and is enhanced by the factor 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 -type system with the bath, slowing down the approach to thermal equilibrium. In the case of nonparallel transition dipole moments (), 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 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.
3 More- Received 1 December 2017
- Revised 27 May 2018
DOI:https://doi.org/10.1103/PhysRevA.98.023811
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