Entangled two-photon absorption with Brownian-oscillator fluctuations

Chen, Feng; Mukamel, Shaul

doi:10.1063/5.0082500

Title: Entangled two-photon absorption with Brownian-oscillator fluctuations

Journal Article · 14 February 2022 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0082500 · OSTI ID:1979033

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^[2]

Univ. of California, Irvine, CA (United States); Wayne State Univ., Detroit, MI (United States)
Univ. of California, Irvine, CA (United States)

Here, we theoretically investigate the two-photon absorption signals of a three-band (g, e, f) system diagonally coupled to an over-damped Brownian oscillator bath, which induces random Gaussian modulations of energy levels with an arbitrary degree of correlation. For fast modulation, extra 2ω_eg and 2ω_fe peaks may obscure the g–f transitions in the classical two-photon absorption (CTPA) spectra for nearly resonant e states. These peaks arise from one-photon resonant g–e or e–f transitions. In the slow modulation limit, these peaks vanish because of the short tails of the Gaussian line shape. CTPA strongly depends on the correlations between energy fluctuations. In entangled two-photon absorption, the extra peaks are eliminated because of the broad one-photon but narrow two-photon spectrum of the twin photons. The variation of the coherences between f states with the correlation between energy fluctuations is explored.

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Research Organization:: Wayne State Univ., Detroit, MI (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0022134

OSTI ID:: 1979033

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 7 Vol. 156; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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