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经典成核理论在活跃相分离中的应用。

Classical Nucleation Theory for Active Fluid Phase Separation.

机构信息

DAMTP, Centre for Mathematical Sciences, University of Cambridge, Wilberforce Road, Cambridge CB3 0WA, United Kingdom.

Service de Physique de l'Etat Condensé, CEA, CNRS Université Paris-Saclay, CEA-Saclay, 91191 Gif-sur-Yvette, France.

出版信息

Phys Rev Lett. 2023 Mar 3;130(9):098203. doi: 10.1103/PhysRevLett.130.098203.

Abstract

Classical Nucleation Theory (CNT), linking rare nucleation events to the free-energy landscape of a growing nucleus, is central to understanding phase-change kinetics in passive fluids. Nucleation in nonequilibrium systems is much harder to describe because there is no free energy, but instead a dynamics-dependent quasipotential that typically must be found numerically. Here we extend CNT to a class of active phase-separating systems governed by a minimal field-theoretic model (Active Model B+). In the small noise and supersaturation limits that CNT assumes, we compute analytically the quasipotential, and hence, nucleation barrier, for liquid-vapor phase separation. Crucial to our results, detailed balance, although broken microscopically by activity, is restored along the instanton trajectory, which in CNT involves the nuclear radius as the sole reaction coordinate.

摘要

经典成核理论(CNT)将稀有成核事件与生长核的自由能景观联系起来,是理解被动流体中相变化动力学的核心。由于没有自由能,而是存在依赖于动力学的准势能,因此,描述非平衡系统中的成核要困难得多,而准势能通常必须通过数值方法找到。在这里,我们将 CNT 扩展到一类由最小的场论模型(主动模型 B+)控制的主动相分离系统。在 CNT 假设的小噪声和过饱和度限制下,我们对液体-蒸汽相分离的准势能,从而也是成核势垒进行了分析计算。对我们的结果至关重要的是,尽管活性从微观上破坏了详细平衡,但沿着瞬子轨迹得到了恢复,在 CNT 中,瞬子轨迹涉及核半径作为唯一的反应坐标。

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