Two-dimensional infrared-Raman spectroscopy as a probe of water’s tetrahedrality

Tomislav Begušić () and Geoffrey A. Blake ()
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Tomislav Begušić: California Institute of Technology
Geoffrey A. Blake: California Institute of Technology

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Two-dimensional spectroscopic techniques combining terahertz (THz), infrared (IR), and visible pulses offer a wealth of information about coupling among vibrational modes in molecular liquids, thus providing a promising probe of their local structure. However, the capabilities of these spectroscopies are still largely unexplored due to experimental limitations and inherently weak nonlinear signals. Here, through a combination of equilibrium-nonequilibrium molecular dynamics (MD) and a tailored spectrum decomposition scheme, we identify a relationship between the tetrahedral order of liquid water and its two-dimensional IR-IR-Raman (IIR) spectrum. The structure-spectrum relationship can explain the temperature dependence of the spectral features corresponding to the anharmonic coupling between low-frequency intermolecular and high-frequency intramolecular vibrational modes of water. In light of these results, we propose new experiments and discuss the implications for the study of tetrahedrality of liquid water.

Date: 2023
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DOI: 10.1038/s41467-023-37667-7

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