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Dynamical Collectivity and Nuclear Quantum Effects on the Intermolecular Stretching Mode of Liquid Water
Keiichiro Shiraga1,2, Yasuhiro Fujii3, Akitoshi Koreeda3
1Graduate School of Agriculture, Kyoto University, Kyoto 606-8502, Japan.
The Journal of Physical Chemistry. B
|January 4, 2021
Summary
Broadband terahertz and Raman spectroscopy reveal differences in liquid water
Area of Science:
- Physical Chemistry
- Spectroscopy
- Liquid Water Dynamics
Background:
- Interpreting the intermolecular stretching mode in liquid water around 5 THz remains a challenge.
- Understanding water's dynamics is crucial across various scientific disciplines.
Purpose of the Study:
- To investigate the intermolecular stretching mode of liquid water using terahertz and Raman spectroscopy.
- To clarify discrepancies in spectral interpretations between the two techniques.
Main Methods:
- Broadband terahertz and low-frequency Raman spectroscopy were employed.
- Experiments were conducted on various water isotopologues (H2O, D2O, H218O).
- Measurements covered a frequency range spanning two decades.
Main Results:
- Terahertz spectroscopy showed a redshifted and broadened intermolecular stretching mode compared to Raman spectroscopy.
- Both techniques probe kinetic motion, but terahertz spectroscopy reveals enhanced dynamical collectivity.
- Temperature and isotope effects highlight the role of oscillation mass and quantum effects on the lineshape.
Conclusions:
- The observed spectral differences are attributed to the distinct dynamical collectivity probed by terahertz and Raman spectroscopy.
- Oscillation mass and quantum effects are significant factors influencing the intermolecular stretching lineshape in liquid water.
- Both spectroscopic methods provide complementary insights into water's complex dynamics.
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