Signatures of vibronic coupling in two-dimensional electronic-vibrational and vibrational-electronic spectroscopies

Gaynor, James D.; Khalil, Munira

doi:10.1063/1.4991745

Signatures of vibronic coupling in two-dimensional electronic-vibrational and vibrational-electronic spectroscopies

Journal Article · Fri Sep 01 04:00:00 EDT 2017 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4991745· OSTI ID:1474041

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Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry; Department of Chemistry, University of Washington, Seattle, Washington (United States)
Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry

Two-Dimensional Electronic-Vibrational (2D EV) spectroscopy and Two-Dimensional Vibrational-Electronic (2D VE) spectroscopy are new coherent four-wave mixing spectroscopies that utilize both electronically resonant and vibrationally resonant field-matter interactions to elucidate couplings between electronic and vibrational degrees of freedom. Here, a system Hamiltonian is developed to lay a foundation for interpreting the 2D EV and 2D VE signals that arise from a vibronically coupled molecular system in the condensed phase. A molecular system consisting of one anharmonic vibration and two electronic states is modeled. Equilibrium displacement of the vibrational coordinate and vibrational frequency shifts upon excitation to the first electronic excited state are included in our Hamiltonian through linear and quadratic vibronic coupling terms. We explicitly consider the nuclear dependence of the electronic transition dipole moment and demonstrate that these spectroscopies are sensitive to non-Condon effects. A series of simulations of 2D EV and 2D VE spectra obtained by varying parameters of the system, system-bath, and interaction Hamiltonians demonstrate that one of the following conditions must be met to observe signals: (1) non-zero linear and/or quadratic vibronic coupling in the electronic excited state, (2) vibrational-coordinate dependence of the electronic transition dipole moment, or (3) electronic-state-dependent vibrational dephasing dynamics. We explore how these vibronic interactions are manifested in the positions, amplitudes, and line shapes of the peaks in 2D EV and 2D VE spectroscopies.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Washington, Seattle, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); Camille and Henry Dreyfus Foundation

Grant/Contract Number:: SC0012450

OSTI ID:: 1474041

Alternate ID(s):: OSTI ID: 1378125

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 9 Vol. 147; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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