Working Paper
Authors
- Thomas E. Gartner III Princeton University ,
- Kelly M. Hunter University of California, San Diego ,
- Eleftherios Lambros University of California, San Diego ,
- Alessandro Caruso University of California, San Diego ,
- Marc Riera University of California, San Diego ,
- Gregory R. Medders University of California, San Diego ,
- Athanassios Z. Panagiotopoulos Princeton University ,
- Pablo G. Debenedetti Princeton University ,
- Francesco Paesani
University of California, San Diego
Abstract
For the last 50 years, researchers have sought molecular models that can accurately reproduce water’s microscopic structure and thermophysical properties across broad ranges of its complex phase diagram. Herein, molecular dynamics simulations with the many-body MB-pol model are performed to monitor the thermodynamic response functions and local structure of liquid water from the boiling point down to deeply supercooled temperatures at ambient pressure. The isothermal compressibility and isobaric heat capacity show maxima at ~223 K, in excellent agreement with recent experiments, and the liquid density exhibits a minimum at ~208 K. Furthermore, a local tetrahedral arrangement, where each water molecule accepts and donates two hydrogen bonds, is the most probable hydrogen-bonding topology at all temperatures. This work suggests that MB-pol may provide predictive capability for studies of liquid water’s physical properties across broad ranges of thermodynamic states.
Content

Supplementary material

Supporting Information
Materials and methods, and supplementary figures and tables.