4.7 Article

Long-lived quantum coherent dynamics of a ?-system driven by a thermal environment

Journal

JOURNAL OF CHEMICAL PHYSICS
Volume 157, Issue 12, Pages -

Publisher

AIP Publishing
DOI: 10.1063/5.0102808

Keywords

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Funding

  1. NSF
  2. [PHY-1912668]

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We present a theoretical study of quantum coherent dynamics of a three-level lambda-system driven by a thermal environment. We observe that thermal excitations can generate experimentally observable long-lived quantum coherent dynamics in the absence of coherent driving.
We present a theoretical study of quantum coherent dynamics of a three-level lambda-system driven by a thermal environment (such as black-body radiation), which serves as an essential building block of photosynthetic light-harvesting models and quantum heat engines. By solving nonsecular Bloch-Redfield master equations, we obtain analytical results for the ground-state population and coherence dynamics and classify the dynamical regimes of the incoherently driven lambda-system as underdamped and overdamped depending on whether the ratio delta/[rf(p)] is greater or less than one, where delta is the ground-state energy splitting, r is the incoherent pumping rate, and f(p) is a function of the transition dipole alignment parameter p. In the underdamped regime, we observe long-lived coherent dynamics that lasts for tau(c) ? 1/r, even though the initial state of the lambda-system contains no coherences in the energy basis. In the overdamped regime for p = 1, we observe the emergence of coherent quasi-steady states with the lifetime tau(c) = 1.34(r/delta(2)), which have a low von Neumann entropy compared to conventional thermal states. We propose an experimental scenario for observing noise-induced coherent dynamics in metastable He* atoms driven by x-polarized incoherent light. Our results suggest that thermal excitations can generate experimentally observable long-lived quantum coherent dynamics in the ground-state subspace of atomic and molecular lambda-systems in the absence of coherent driving.

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