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An Analog Macroscopic Technique for Studying Molecular Hydrodynamic Processes in Dense Gases and Liquids

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Spatial correlations of density and structural fluctuations in liquid water: a comparative simulation study.

Felix Sedlmeier¹, Dominik Horinek, Roland R Netz

¹Physik Department, Technische Universität München, 85748 Garching, Germany.

Journal of the American Chemical Society

|January 18, 2011

Summary

Simulations reveal that liquid water

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Area of Science:

Computational physics
Physical chemistry
Materials science

Background:

Liquid water exhibits complex structural properties.
Understanding spatial correlations is key to characterizing water's behavior.

Purpose of the Study:

To investigate spatial correlations between local density and structural order in liquid water.
To compare simulation results with experimental small-angle X-ray scattering (SAXS) data.

Main Methods:

Large-scale classical simulations using various force fields.
Calculation of spatial two-point correlation functions for density and structural order parameters (tetrahedrality, hydrogen bonds).

Main Results:

Simulations accurately reproduce experimental SAXS structure factor S(q).
TIP4P/2005 force field shows near-quantitative agreement with S(q).
Structural order parameters show weak spatial correlations compared to density fluctuations.

Conclusions:

Liquid water's tendency for density clustering is significantly stronger than for structural clustering.
Spatial correlations in density do not directly translate to spatial correlations in structure for liquid water.