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Cho, Minhaeng
분자 분광학 및 동력학 연구단
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Molecular Photothermal Effects on Time-Resolved IR Spectroscopy: Solute-Solvent Intermolecular Energy Transfer

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Title
Molecular Photothermal Effects on Time-Resolved IR Spectroscopy: Solute-Solvent Intermolecular Energy Transfer
Author(s)
Minhaeng Cho
Publication Date
2023-01
Journal
Journal of Physical Chemistry B, v.127, no.1, pp.300 - 307
Publisher
American Chemical Society
Abstract
Time-resolved IR pump-probe (IR-PP) and two-dimensional IR (2D-IR) spectroscopy are valuable tools for studying ultrafast chemical and biological processes in solutions. However, the corresponding signals at long times are obscured by the molecular photothermal effects resulting from the heat dissipation of vibrationally photoexcited molecules to the surroundings. Recently, a phenomenology model was used to describe molecular photothermal effects on IR-PP signals and the diagonal and cross-peaks of 2D-IR spectra at long pump-probe delay times. Here, we consider the thermal diffusion equation with a time-dependent heat source term to describe the solute-solvent energy transfer process. An approximate solution to the nonhomogeneous differential equation shows that the molecular photothermal effect is determined by the mean intermolecular distance between IR-Absorbing molecules. We show that the time profile of heat dissipation from a vibrationally excited molecule to the surroundings, which provides information about the mechanisms involved in the solute-solvent intermolecular energy transfer process in solutions, can be directly measured by analyzing the molecular photothermal IR-PP and 2D-IR signals. We anticipate that the present work can be used to interpret local heating-induced time-resolved IR spectroscopic signals and understand the rate of and the mechanisms involved in the conversion from high-frequency molecular vibrational energy to solvent kinetic energy in condensed phases. © 2022 Organic Letters. All rights reserved.
URI
https://pr.ibs.re.kr/handle/8788114/13742
DOI
10.1021/acs.jpcb.2c07043
ISSN
1520-6106
Appears in Collections:
Center for Molecular Spectroscopy and Dynamics(분자 분광학 및 동력학 연구단) > 1. Journal Papers (저널논문)
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