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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Spectroscopy

Background:

  • Liquid's supramolecular structure dictates dynamics and macroscopic properties like viscosity.
  • Understanding structural changes with temperature is crucial for liquid-to-glass dynamics.

Purpose of the Study:

  • Quantitatively determine the intermolecular hydrogen bond length in water across a wide temperature range.
  • Investigate the relationship between hydrogen bond expansivity and average oxygen-oxygen distances.
  • Identify characteristic points in water's supramolecular arrangement related to thermal anomalies.

Main Methods:

  • Infrared (IR) spectroscopy to measure hydrogen bond stretching vibrations.
  • Molecular dynamics simulations.
  • Quantitative analysis of experimental and simulation data.

Main Results:

  • Extracted hydrogen bond expansivity differs significantly from oxygen-oxygen distance expansivity.
  • A random loose packing model connects these properties via coordination number.
  • The most compact molecular arrangement occurs around 316-331K, near pressure anomaly temperatures.

Conclusions:

  • Intermolecular H-bond expansivity is a key factor in water's thermal evolution.
  • The study confirms a quantitative method for deducing intermolecular H-bond lengths using IR spectroscopy.
  • This approach offers new insights into molecular fluctuations and supramolecular arrangements.