Long-lived quantum coherent dynamics of a $\Lambda$-system driven by a thermal environment
J. Chem. Phys. 157, 124302 (2022) We present a theoretical study of quantum coherent dynamics of a three-level $\Lambda$ system driven by a thermal environment (such as blackbody radiation), which serves as an essential building block of photosynthetic light-harvesting models and quantum heat engine...
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Zusammenfassung: | J. Chem. Phys. 157, 124302 (2022) We present a theoretical study of quantum coherent dynamics of a three-level
$\Lambda$ system driven by a thermal environment (such as blackbody radiation),
which serves as an essential building block of photosynthetic light-harvesting
models and quantum heat engines. By solving the 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 $\Delta/[r f(p)]$ 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
$\tau_c\simeq 1/r$, 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 low von Neumann entropy compared
to the 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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DOI: | 10.48550/arxiv.2108.07457 |