Multimode two-dimensional vibronic spectroscopy. I. Orientational response and polarization-selectivity

Gaynor, James D.; Weakly, Robert B.; Khalil, Munira

doi:10.1063/5.0047724

Multimode two-dimensional vibronic spectroscopy. I. Orientational response and polarization-selectivity

Journal Article · Tue May 11 04:00:00 EDT 2021 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0047724· OSTI ID:1853003

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

Two-dimensional Electronic–Vibrational (2D EV) spectroscopy and two-dimensional Vibrational–Electronic (2D VE) spectroscopy are among the newest additions to the coherent multidimensional spectroscopy toolbox, and they are directly sensitive to vibronic couplings. In this first of two papers, the complete orientational response functions are developed for a model system consisting of two coupled anharmonic oscillators and two electronic states in order to simulate polarization-selective 2D EV and 2D VE spectra with arbitrary combinations of linearly polarized electric fields. Here, we propose analytical methods to isolate desired signals within complicated spectra and to extract the relative orientation between vibrational and vibronic dipole moments of the model system using combinations of polarization-selective 2D EV and 2D VE spectral features. Time-dependent peak amplitudes of coherence peaks are also discussed as means for isolating desired signals within the time-domain. This paper serves as a field guide for using polarization-selective 2D EV and 2D VE spectroscopies to map coupled vibronic coordinates on the molecular frame.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: SC0019277

OSTI ID:: 1853003

Alternate ID(s):: OSTI ID: 1970635

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 18 Vol. 154; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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Journal Article · Tue May 11 00:00:00 EDT 2021 · Journal of Chemical Physics · OSTI ID:1853004

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Multimode two-dimensional vibronic spectroscopy. I. Orientational response and polarization-selectivity

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