Connection between water's dynamical and structural properties: Insights from ab initio simulations

Area of Science:

• Computational Physics
• Physical Chemistry
• Materials Science

Background:

• Understanding the behavior of supercooled water is crucial for various scientific disciplines.
• First-principles calculations offer insights into molecular structure and dynamics.
• Density functional theory (DFT) is a key method for electronic structure calculations.

Purpose of the Study:

• To identify the optimal DFT functional for describing the temperature-dependent transport coefficients of bulk water.
• To evaluate the applicability of the Stokes-Einstein relation across different functionals and temperatures.
• To investigate the relationship between the structural properties and dynamic behavior of supercooled water.

Main Methods:

• Employed density functional theory (DFT) to perform first-principles calculations.
• Evaluated multiple DFT functionals for their accuracy in predicting water transport coefficients.
• Assessed the Stokes-Einstein relation and explored structure-dynamics correlations.

Main Results:

• Determined the DFT functional that best captures the temperature evolution of water's transport properties.
• Validated the Stokes-Einstein relation within the studied temperature range for various functionals.
• Established a connection between computable structural descriptors and transport coefficients.

Conclusions:

• DFT calculations provide a robust framework for studying supercooled water dynamics.
• Transport coefficients can be efficiently computed from structural descriptors, reducing simulation time.
• Findings guide the development of improved DFT functionals for condensed matter systems.