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Breakdown of the Stokes-Einstein relation in supercooled water: the jump-diffusion perspective
Vikas Dubey1, Shivam Dueby1, Snehasis Daschakraborty1
1Department of Chemistry, Indian Institute of Technology Patna, Bihar 801106, India. snehasis@iitp.ac.in.
Supercooled water exhibits dynamical anomalies, including a breakdown of the Stokes-Einstein relation (SER). A new translational jump-diffusion (TJD) approach explains this breakdown, offering insights into water
Area of Science:
- Physical Chemistry
- Thermodynamics
- Fluid Dynamics
Background:
- Water displays thermodynamic and dynamic anomalies, particularly in the supercooled state.
- Dynamical anomalies in supercooled water, such as the breakdown of the Stokes-Einstein relation (SER), are less understood due to experimental challenges.
- Accurate viscosity measurements of supercooled water have enabled direct verification of SER violations.
Purpose of the Study:
- To provide a comprehensive analysis of past and present research on the breakdown of the Stokes-Einstein relation in supercooled water.
- To highlight the recently developed translational jump-diffusion (TJD) approach for explaining SER breakdown.
- To elucidate the molecular mechanisms underlying dynamical anomalies in supercooled water.
Main Methods:
- Review of experimental and theoretical studies on supercooled water dynamics.
- Analysis of recent viscosity measurements at various temperatures and pressures.
- Evaluation of the translational jump-diffusion (TJD) model's explanatory power for SER breakdown.
Main Results:
- The Stokes-Einstein relation (SER) shows increasing breakdown with decreasing temperature in supercooled water.
- Elevated pressure mitigates the extent of SER breakdown.
- The translational jump-diffusion (TJD) approach quantitatively explains the observed SER breakdown in pure supercooled water and methanol-water solutions.
Conclusions:
- The breakdown of the Stokes-Einstein relation is a significant dynamical anomaly in supercooled water.
- The translational jump-diffusion (TJD) model offers a promising molecular-level explanation for this phenomenon.
- Further research into TJD is crucial for understanding water's complex behavior in the supercooled regime.
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