Topology induced crossover between Langevin, subdiffusion, and Brownian diffusion regimes in supercooled water
Abstract
Despite extensive studies of supercooled water, it remains challenging to understand its peculiar dynamic anomalous properties. In this work, we integrated full atomistic simulations of supercooled water over the temperature range of room temperature to 200 K using a quantum-mechanics-based polarizable force field with the dressed dynamics method that couples fast collision events and slow reorganization dynamics of hydrogen-bond networks. Our analysis unveils the salient multiscale features in the transient relaxation dynamics of supercooled water. A classical Langevin behavior dominates at fast timescales, while long-time relaxations unveil two different activation barriers in two temperature regions: below and above 230 K. The modulation of the entropy spectrum by temperature is elucidated in terms of a three-state model underlined by the complexity of the water dynamics associated with a topological transition of a strong hydrogen-bond network. This state-dependent network topology is quantitatively characterized by power-law exponents of inverse network connectivity from 200 to 298 K. This work provides valuable guidance for further studies on the transient relaxation dynamics of supercooled water.
Additional Information
© the Owner Societies 2023. KCZ and HBS would like to thank Prof. Xiaoyuan Li and Prof. Jingdi Zhang for interesting discussions on various aspects of supercooled water systems. Support for WAG and SN was provided by the Liquid Sunlight Alliance, which is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under Award Number DE-SC0021266. KCZ and HBS are supported in part by the Research Grants Council of Hong Kong (16306021), HKUST grant (R9418), and the Society of Interdisciplinary Research (SOIRÉE) in Hong Kong. This research made use of the computing resources of the X-GPU cluster supported by the Hong Kong Research Grants Council Collaborative Research Fund (C6021-19EF). There are no conflicts to declare.Files
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Additional details
- Eprint ID
- 121157
- Resolver ID
- CaltechAUTHORS:20230425-441449400.4
- DOI
- 10.1039/D2CP04645H
- DE-SC0021266
- Department of Energy (DOE)
- 16306021
- Research Grants Council of Hong Kong
- R9418
- Hong Kong University of Science and Technology
- Society of Interdisciplinary Research (SOIRÉE)
- C6021-19EF
- Research Grants Council of Hong Kong
- Created
-
2023-04-29Created from EPrint's datestamp field
- Updated
-
2023-04-29Created from EPrint's last_modified field
- Caltech groups
- Liquid Sunlight Alliance