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J Chem Phys ; 160(8)2024 Feb 28.
Article in English | MEDLINE | ID: mdl-38421073

ABSTRACT

By employing the numerically accurate multiple Davydov Ansatz (mDA) formalism in combination with the thermo-field dynamics (TFD) representation of quantum mechanics, we systematically explore the influence of three parameters-temperature, photonic-mode detuning, and qubit-phonon coupling-on population dynamics and absorption spectra of the Holstein-Tavis-Cummings (HTC) model. It is found that elevated qubit-phonon couplings and/or temperatures have a similar impact on all dynamic observables: they suppress the amplitudes of Rabi oscillations in photonic populations as well as broaden the peaks and decrease their intensities in the absorption spectra. Our results unequivocally demonstrate that the HTC dynamics is very sensitive to the concerted variation of the three aforementioned parameters, and this finding can be used for fine-tuning polaritonic transport. The developed mDA-TFD methodology can be efficiently applied for modeling, predicting, optimizing, and comprehensively understanding dynamic and spectroscopic responses of actual molecular systems in microcavities.

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