journal article·2022-10-20

Experimental and Theoretical Heterodyne-Detected Sum Frequency Generation Spectroscopy of Isotopically Pure and Diluted Water Surfaces

Shoichi Yamaguchi, Tetsuyuki Takayama, Yuki Goto, Takuhiro Otosu, Takuma Yagasaki

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Abstract

The χ (2) (second-order nonlinear optical susceptibility) spectrum of the water surface has been a matter of debate for a few decades. Here, we report that we experimentally measured the isotopic dilution dependence of the χ (2) spectrum and theoretically reproduced it by employing the quantum/classical mixed approach with a new idea to subtract an artifact. The present theoretical framework allows for clarifying the effects of the intramolecular, intermolecular, and Fermi resonance couplings on the OH-stretch vibrational spectra of water at the surface as well as in the bulk.
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Research context

OpenAlex topics: Spectroscopy and Quantum Chemical Studies · Spectroscopy and Laser Applications · Photosynthetic Processes and Mechanisms

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Affiliations

Department of Applied Chemistry, Graduate School of Science and Engineering, Saitama University, 255 Shimo-Okubo, Sakura, Saitama 338-8570, Japan

Division of Chemical Engineering, Graduate School of Engineering Science, Osaka University, Toyonaka 560-8531, Japan

Funding

Japan Society for the Promotion of Science

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