TY - JOUR
T1 - Anomalies and Local Structure of Liquid Water from Boiling to the Supercooled Regime as Predicted by the Many-Body MB-pol Model
AU - Gartner, Thomas E.
AU - Hunter, Kelly M.
AU - Lambros, Eleftherios
AU - Caruso, Alessandro
AU - Riera, Marc
AU - Medders, Gregory R.
AU - Panagiotopoulos, Athanassios Z.
AU - Debenedetti, Pablo G.
AU - Paesani, Francesco
N1 - Funding Information:
We thank the late Prof. Austen Angell for countless, stimulating conversations about the properties of supercooled water and his continued support to the development of the MB-pol water model. This research was supported by the Air Force Office of Scientific Research under Award FA9550-20-1-0351 (F.P.), the “Chemistry in Solution and at Interfaces” (CSI) Center that is funded by the U.S. Department of Energy under Award DE-SC001934 (A.Z.P. and P.G.D.). Computational resources were provided by the Department of Defense High Performance Computing Modernization Program (HPCMP), the Triton Shared Computing Cluster (TSCC) at the San Diego Supercomputer Center (SDSC) Supercomputer Center (SDSC), and Princeton Research Computing, a consortium of groups including the Princeton Institute for Computational Science and Engineering (PICSciE) and the Office of Information Technology’s High Performance Computing Center and Visualization Laboratory at Princeton University.
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/4/28
Y1 - 2022/4/28
N2 - For the past 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 near 223 K, in excellent agreement with recent experiments, and the liquid density exhibits a minimum at ∼208 K. A local tetrahedral arrangement, where each water molecule accepts and donates two hydrogen bonds, is found to be 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, including the so-called water's "no man's land" which is difficult to probe experimentally.
AB - For the past 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 near 223 K, in excellent agreement with recent experiments, and the liquid density exhibits a minimum at ∼208 K. A local tetrahedral arrangement, where each water molecule accepts and donates two hydrogen bonds, is found to be 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, including the so-called water's "no man's land" which is difficult to probe experimentally.
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U2 - 10.1021/acs.jpclett.2c00567
DO - 10.1021/acs.jpclett.2c00567
M3 - Article
C2 - 35436129
AN - SCOPUS:85128827216
SN - 1948-7185
VL - 13
SP - 3652
EP - 3658
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 16
ER -