Mechanical theory of nonequilibrium coexistence and motility-induced phase separation
Abstract
Nonequilibrium phase transitions are routinely observed in both natural and synthetic systems. The ubiquity of these transitions highlights the conspicuous absence of a general theory of phase coexistence that is broadly applicable to both nonequilibrium and equilibrium systems. Here, we present a general mechanical theory for phase separation rooted in ideas explored nearly a half-century ago in the study of inhomogeneous fluids. The core idea is that the mechanical forces within the interface separating two coexisting phases uniquely determine coexistence criteria, regardless of whether a system is in equilibrium or not. We demonstrate the power and utility of this theory by applying it to active Brownian particles, predicting a quantitative phase diagram for motility-induced phase separation in both two and three dimensions. This formulation additionally allows for the prediction of novel interfacial phenomena, such as an increasing interface width while moving deeper into the two-phase region, a uniquely nonequilibrium effect confirmed by computer simulations. The self-consistent determination of bulk phase behavior and interfacial phenomena offered by this mechanical perspective provide a concrete path forward toward a general theory for nonequilibrium phase transitions.
Additional Information
© 2023 the Author(s). Published by PNAS. This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND). A.K.O. is deeply indebted to Phill Geissler for his numerous insights regarding this work. We thank Katie Klymko, Karol Makuch, Yizhi Shen, Zhiwei Peng, Andy Ylitalo, Dan Evans, and Luke Langford for helpful discussions. We gratefully acknowledge support from the Schmidt Science Fellowship in partnership with the Rhodes Trust (A.K.O.), Kwanjeong Educational Foundation (H.R.), Arnold and Mabel Beckman Foundation (S.A.M.), and NSF under grant no. CBET-1803662 (J.F.B.). Author contributions: A.K.O., H.R., S.A.M., and J.F.B. designed research; performed research; contributed new reagents/analytic tools; analyzed data; and wrote the paper. The authors declare no competing interest.Attached Files
Published - pnas.2219900120.pdf
Supplemental Material - pnas.2219900120.sapp.pdf
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Additional details
- PMCID
- PMC10160997
- Eprint ID
- 122432
- Resolver ID
- CaltechAUTHORS:20230725-49170000.16
- Schmidt Futures Program
- Rhodes Trust
- Kwanjeong Educational Foundation
- Arnold and Mabel Beckman Foundation
- NSF
- CBET-1803662
- Created
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2023-08-11Created from EPrint's datestamp field
- Updated
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2023-08-14Created from EPrint's last_modified field