Nucleation is a key rate-limiting process in phase transition and phase separation. Recent studies highlight a significant discrepancy between experimentally measured nucleation rates and theoretical predictions, particularly when dynamic structural reordering occurs along multi-step pathways. To bridge this gap, we develop a multi-shell model with a space-time-dependent order-parameter field to describe the reordering-nucleation process, where structural reorganization couples with the early growth of condensed clusters. Through stochastic simulations, we track the time-resolved evolution of heterogeneous structural order inside growing clusters. Path analysis of the first-passage problem in early-stage nucleation demonstrates that shifting the reordering rate alters the nucleation rate by several orders of magnitude. Furthermore, as the coupling strength increases, the relationship between the mean first-passage time and reordering susceptibility shifts from monotonic to non-monotonic, exhibiting a turnover effect. We quantitatively rationalize these behaviors with an effective nucleation barrier that accounts for non-equilibrium properties. Our findings elucidate the mechanisms behind multi-step nucleation and offer a predictive framework for future studies.
Nucleation is a fundamental step in the formation of new materials, with nucleation rates governing phase-transition pathways and outcomes that influence material properties across chemistry, physics, and biology. Nevertheless, extracting nucleation rates remains challenging: experiments are limited by the microscopi...
Lun-Na Li, Fabienne Bachtiger, A. Finney et al.· Journal of the American Chem...· 1 citation
We extend classical nucleation theory (CNT) by explicitly incorporating the multidimensional nature of nucleation and the coupled roles of kinetics and thermodynamics. Specifically, we treat the cluster density as an independent variable, within both sharp-interface and diffuse-interface descriptions. The kinetics are...
Deciphering the microscopic details of crystal nucleation remains a key open problem in chemical physics. For aqueous sodium chloride (NaCl), the extent to which nucleation involves amorphous ion aggregation, and the supersaturation regime in which two-step-like behavior emerges, remains actively debated. In this work,...
We study dynamical effects during nucleation in thermal first-order phase transitions in field theory. Focusing on the classical regime of the decay of a metastable state, we present the general formula for the thermal decay rate including the dynamical prefactor and give a recipe for its systematic evaluation. We desc...
Oliver Gould, Joonas Hirvonen, A. Shkerin et al.· 0 citations
Two-temperature induced phase separation (2-TIPS) has emerged as a generic non-equilibrium mechanism in scalar active systems with heterogeneous activity, where particles coupled to different thermal reservoirs spontaneously demix into dense cold and dilute hot phases. Unlike equilibrium phase separation or motility-in...
Nayana Venkatareddy, Jaydeep Mandal, Jayeeta Chattopadhyay et al.· 0 citations
Smallenburg reports near-melting point simulations and observes a well-predicted spontaneous nucleation with mixed, finite-time morphology, in a Comment on our recent Perspective. The Comment's incorrect broader takeaway --- that equilibrium coexistence is"readily achievable"--- rests on an untested generalization from...
Roseanna N. Zia· AIChE Journal· 0 citations
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