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Title: Phase Diagram of Active Brownian Spheres: Crystallization and the Metastability of Motility-Induced Phase Separation

Abstract

Motility-induced phase separation (MIPS), the phenomenon in which purely repulsive active particles undergo a liquid-gas phase separation, is among the simplest and most widely studied examples of a nonequilibrium phase transition. Here, we show that states of MIPS coexistence are in fact only metastable for three-dimensional active Brownian particles over a very broad range of conditions, decaying at long times through an ordering transition we call active crystallization. At an activity just above the MIPS critical point, the liquid-gas binodal is superseded by the crystal-fluid coexistence curve, with solid, liquid, and gas all coexisting at the triple point where the two curves intersect. Nucleating an active crystal from a disordered fluid, however, requires a rare fluctuation that exhibits the nearly close-packed density of the solid phase. The corresponding barrier to crystallization is surmountable on a feasible timescale only at high activity, and only at fluid densities near maximal packing. The glassiness expected for such dense liquids at equilibrium is strongly mitigated by active forces, so that the lifetime of liquid-gas coexistence declines steadily with increasing activity, manifesting in simulations as a facile spontaneous crystallization at incredibly high activity.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1];  [3]
  1. Univ. of California, Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1822134
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 126; Journal Issue: 18; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Crystallization; Nucleation; Phase diagrams; Active matter; Nonequilibrium systems

Citation Formats

Omar, Ahmad K., Klymko, Katherine, GrandPre, Trevor, and Geissler, Phillip L. Phase Diagram of Active Brownian Spheres: Crystallization and the Metastability of Motility-Induced Phase Separation. United States: N. p., 2021. Web. doi:10.1103/physrevlett.126.188002.
Omar, Ahmad K., Klymko, Katherine, GrandPre, Trevor, & Geissler, Phillip L. Phase Diagram of Active Brownian Spheres: Crystallization and the Metastability of Motility-Induced Phase Separation. United States. https://doi.org/10.1103/physrevlett.126.188002
Omar, Ahmad K., Klymko, Katherine, GrandPre, Trevor, and Geissler, Phillip L. Fri . "Phase Diagram of Active Brownian Spheres: Crystallization and the Metastability of Motility-Induced Phase Separation". United States. https://doi.org/10.1103/physrevlett.126.188002. https://www.osti.gov/servlets/purl/1822134.
@article{osti_1822134,
title = {Phase Diagram of Active Brownian Spheres: Crystallization and the Metastability of Motility-Induced Phase Separation},
author = {Omar, Ahmad K. and Klymko, Katherine and GrandPre, Trevor and Geissler, Phillip L.},
abstractNote = {Motility-induced phase separation (MIPS), the phenomenon in which purely repulsive active particles undergo a liquid-gas phase separation, is among the simplest and most widely studied examples of a nonequilibrium phase transition. Here, we show that states of MIPS coexistence are in fact only metastable for three-dimensional active Brownian particles over a very broad range of conditions, decaying at long times through an ordering transition we call active crystallization. At an activity just above the MIPS critical point, the liquid-gas binodal is superseded by the crystal-fluid coexistence curve, with solid, liquid, and gas all coexisting at the triple point where the two curves intersect. Nucleating an active crystal from a disordered fluid, however, requires a rare fluctuation that exhibits the nearly close-packed density of the solid phase. The corresponding barrier to crystallization is surmountable on a feasible timescale only at high activity, and only at fluid densities near maximal packing. The glassiness expected for such dense liquids at equilibrium is strongly mitigated by active forces, so that the lifetime of liquid-gas coexistence declines steadily with increasing activity, manifesting in simulations as a facile spontaneous crystallization at incredibly high activity.},
doi = {10.1103/physrevlett.126.188002},
journal = {Physical Review Letters},
number = 18,
volume = 126,
place = {United States},
year = {Fri May 07 00:00:00 EDT 2021},
month = {Fri May 07 00:00:00 EDT 2021}
}

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