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Download fileVariational Squeezed Davydov Ansatz for Realistic Chemical Systems with Nonlinear Vibronic Coupling
journal contribution
posted on 2022-01-31, 23:13 authored by Jiarui Zeng, Yao YaoChemical systems normally possess
strong nonlinear vibronic couplings
at both zero and finite temperature. For the lowest-order quadratic
couplings, here, we introduce a squeezing operator into a variational
coherent-state-based method, Davydov ansatz, to simulate the quantum
dynamics and the respective spectroscopy. Two molecular systems, pyrazine
and the 2-pyridone dimer, are taken as calculated model systems, both
of which involve nontrivial quadratic vibronic couplings in high-
and low-frequency regions, respectively. Upon a comparison with the
benchmarks, the method manifests its advantage for nonlinear couplings.
The squeezed bases are also proven to be applicable for the finite
temperature by adapting with the thermofield dynamics.
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two molecular systemsrealistic chemical systemscalculated model systemsorder quadratic couplingsnonlinear couplingsvariational coherentthermofield dynamicssqueezing operatorsqueezed basesrespective spectroscopyquantum dynamicspyridone dimermethod manifestsfrequency regionsfinite temperaturedavydov ansatzbased methodalso proven