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Title: Solvation in Space-time: Pretransition Effects in Trajectory Space

Abstract

We demonstrate pretransition effects in space-time in trajectories of systems in which the dynamics displays a first-order phase transition between distinct dynamical phases. These effects are analogous to those observed for thermodynamic first-order phase transitions, most notably the hydrophobic effect in water. Considering the (infinite temperature) East model as an elementary example, we study the properties of "space-time solvation" by examining trajectories where finite space-time regions are conditioned to be inactive in an otherwise active phase. We find that solvating an inactive region of space-time within an active trajectory shows two regimes in the dynamical equivalent of solvation free energy: An "entropic" small solute regime in which uncorrelated fluctuations are sufficient to evacuate activity from the solute, and an "energetic" large solute regime which involves the formation of a solute-induced inactive domain with an associated active-inactive interface bearing a dynamical interfacial tension. We also show that as a result of this dynamical interfacial tension there is a dynamical analog of the hydrophobic collapse that drives the assembly of large hydrophobes in water. We discuss the general relevance of these results to the properties of dynamical fluctuations in systems with slow collective relaxation such as glass formers.

Authors:
 [1];  [2];  [3]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
  2. Univ. of Nottingham (United Kingdom). School of Physics and Astronomy; Univ. of Nottingham (United Kingdom). Centre for the Mathematics and Theoretical Physics of Quantum Non-Equilibrium Systems
  3. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); Engineering and Physical Sciences Research Council (EPSRC); National Science Foundation (NSF)
OSTI Identifier:
1506321
Alternate Identifier(s):
OSTI ID: 1457822
Grant/Contract Number:  
AC02-05CH11231; EP/M014266/1
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 120; Journal Issue: 26; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Katira, Shachi, Garrahan, Juan P., and Mandadapu, Kranthi K. Solvation in Space-time: Pretransition Effects in Trajectory Space. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.120.260602.
Katira, Shachi, Garrahan, Juan P., & Mandadapu, Kranthi K. Solvation in Space-time: Pretransition Effects in Trajectory Space. United States. doi:https://doi.org/10.1103/PhysRevLett.120.260602
Katira, Shachi, Garrahan, Juan P., and Mandadapu, Kranthi K. Fri . "Solvation in Space-time: Pretransition Effects in Trajectory Space". United States. doi:https://doi.org/10.1103/PhysRevLett.120.260602. https://www.osti.gov/servlets/purl/1506321.
@article{osti_1506321,
title = {Solvation in Space-time: Pretransition Effects in Trajectory Space},
author = {Katira, Shachi and Garrahan, Juan P. and Mandadapu, Kranthi K.},
abstractNote = {We demonstrate pretransition effects in space-time in trajectories of systems in which the dynamics displays a first-order phase transition between distinct dynamical phases. These effects are analogous to those observed for thermodynamic first-order phase transitions, most notably the hydrophobic effect in water. Considering the (infinite temperature) East model as an elementary example, we study the properties of "space-time solvation" by examining trajectories where finite space-time regions are conditioned to be inactive in an otherwise active phase. We find that solvating an inactive region of space-time within an active trajectory shows two regimes in the dynamical equivalent of solvation free energy: An "entropic" small solute regime in which uncorrelated fluctuations are sufficient to evacuate activity from the solute, and an "energetic" large solute regime which involves the formation of a solute-induced inactive domain with an associated active-inactive interface bearing a dynamical interfacial tension. We also show that as a result of this dynamical interfacial tension there is a dynamical analog of the hydrophobic collapse that drives the assembly of large hydrophobes in water. We discuss the general relevance of these results to the properties of dynamical fluctuations in systems with slow collective relaxation such as glass formers.},
doi = {10.1103/PhysRevLett.120.260602},
journal = {Physical Review Letters},
number = 26,
volume = 120,
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

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Cited by: 4 works
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Figures / Tables:

Figure 1 Figure 1: (A) Thermodynamic first-order phase transition between liquid and vapor phases. (B) Solvation free energy F per unit area of a hard sphere in a liquid shows two regimes: a small solute entropic regime, and a large solute energetic regime which involves formation of a vapor domain around themore » sphere with an associated liquid–vapor interface; adapted from [4]. (C) Trajectory space phase diagram showing a dynamical first-order phase transition between active and inactive phases, cf. [10]). (D) Expected dynamical hydrophobiclike effect for “space–time solutes”.« less

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