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

Author

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  • Tomislav Begušić

    (California Institute of Technology)

  • Geoffrey A. Blake

    (California Institute of Technology
    California Institute of Technology)

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.

Suggested Citation

  • Tomislav Begušić & Geoffrey A. Blake, 2023. "Two-dimensional infrared-Raman spectroscopy as a probe of water’s tetrahedrality," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-37667-7
    DOI: 10.1038/s41467-023-37667-7
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    References listed on IDEAS

    as
    1. Jeffrey R. Errington & Pablo G. Debenedetti, 2001. "Relationship between structural order and the anomalies of liquid water," Nature, Nature, vol. 409(6818), pages 318-321, January.
    2. Wei Fang & Ji Chen & Philipp Pedevilla & Xin-Zheng Li & Jeremy O. Richardson & Angelos Michaelides, 2020. "Origins of fast diffusion of water dimers on surfaces," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    3. Maksim Grechko & Taisuke Hasegawa & Francesco D’Angelo & Hironobu Ito & Dmitry Turchinovich & Yuki Nagata & Mischa Bonn, 2018. "Coupling between intra- and intermolecular motions in liquid water revealed by two-dimensional terahertz-infrared-visible spectroscopy," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
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