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We introduce a computational method to discover polymorphs in molecular crystals at finite temperature. The method is based on reproducing the crystallization process starting from the liquid and letting the system discover the relevant…

Chemical Physics · Physics 2020-04-10 Pablo M. Piaggi , Michele Parrinello

Recently, it was shown that a theoretical description of nucleation based on fluctuating hydrodynamics and classical density functional theory can be used to determine non-classical nucleation pathways for crystallization (Lutsko, Sci. Adv.…

Chemical Physics · Physics 2024-06-26 James F. Lutsko , Cédric Schoonen

Crystallization is a process of great practical relevance in which rare but crucial fluctuations lead to the formation of a solid phase starting from the liquid. Like in all first order first transitions there is an interplay between…

Statistical Mechanics · Physics 2017-07-12 Pablo M. Piaggi , Omar Valsson , Michele Parrinello

Using state-of-the-art rare-event sampling simulations, we precisely characterize the nucleation of liquid droplets from a supersaturated Lennard-Jones gas and uncover a key physical feature: critical clusters nucleate with a density that…

Chemical Physics · Physics 2026-01-07 Yijian Wu , Thomas Philippe , Aymane Graini , Julien Lam

Non-classical two-step nucleation including preordering and crystal nucleation has been widely proposed to challenge the one-step nucleation framework in diverse materials, while what drives preordering has not been explicitly resolved yet.…

Soft Condensed Matter · Physics 2024-10-18 Renkuan Cao , Fan Peng , Yunhan Zhang , Hao Sun , Ziwei Liu , Tingyu Xu , Liangbin Li

Nucleation is an activated process in which the system has to overcome a free energy barrier in order for a first-order phase transition between the metastable and the stable phases to take place. In the liquid-to-solid transition the…

Soft Condensed Matter · Physics 2016-11-28 John Russo , Hajime Tanaka

The phenomenon of solidification of a substance from its liquid phase is of the greatest practical and theoretical importance, and atomistic simulations can provide precious information towards its understanding and control. Unfortunately,…

Soft Condensed Matter · Physics 2021-03-25 Tarak Karmakar , Michele Invernizzi , Valerio Rizzi , Michele Parrinello

Enhanced sampling methods typically require predefined collective variables (CVs) that presuppose knowledge of reaction coordinates, restricting the discovery of unanticipated transition mechanisms or intermediates. Here, we show that a…

Chemical Physics · Physics 2026-04-08 Xiangrui Li , Daniel Schwalbe-Koda

Nucleation processes, through which a new structure progressively forms within a pre-existing homogeneous phase, are fundamental in materials science, but are also typically non-trivial to elucidate. Cases in which to nucleate are defects…

Materials Science · Physics 2025-05-05 Mattia Perrone , David D. Girardier , Giovanni M. Pavan , Fabio Pietrucci

Molecule- and particle-based simulations provide the tools to test, in microscopic detail, the validity of classical nucleation theory. In this endeavour, determining nucleation mechanisms and rates for phase separation requires an…

Materials Science · Physics 2023-02-27 Aaron R. Finney , Matteo Salvalaglio

In the absence of impurities and boundary effects, first order phase transitions are initiated by the nucleation of critical bubbles. In thermally driven transitions many systems can remain metastable for an extended time, possibly tens of…

High Energy Physics - Lattice · Physics 2025-02-21 Jaakko Hällfors , Kari Rummukainen

Crystallization, a fundamental phase transition process governing material formation in natural and industrial contexts, involves the spontaneous emergence of long-range structural order from disordered phases. This long-range periodicity…

Statistical Mechanics · Physics 2025-10-13 YaoKun Lei , MaoDong Li , Yi Isaac Yang

A molecular understanding of how protein function is related to protein structure will require an ability to understand large conformational changes between multiple states. Unfortunately these states are often separated by high free energy…

Biological Physics · Physics 2011-08-08 Juan R. Perilla , Thomas B. Woolf

To locate the position and characterize the dynamics of a vacancy in a crystal, we propose to represent it by the ground state density of a quantum probe quasi-particle for the Hamiltonian associated to the potential energy field generated…

Materials Science · Physics 2013-06-04 Pierre-Antoine Geslin , Giovanni Ciccotti , Eric Vanden-Eijnden , Simone Meloni

The nucleation process under different external conditions is considered. It is shown that the duration of this process can be connected with the microscopic corrections to the free energy of the critical embryo. Connection between…

Statistical Mechanics · Physics 2008-08-25 Victor Kurasov

Recent advances in classical density functional theory are combined with stochastic process theory and rare event techniques to formulate a theoretical description of nucleation, including crystallization, that can predict nonclassical…

Chemical Physics · Physics 2019-04-09 James F. Lutsko

Kinetic barriers cause polymers to crystallize incompletely, into nanoscale lamellae interleaved with amorphous regions. As a result, crystalline polymers are full of crystal-melt interfaces, which dominate their physical properties. The…

Soft Condensed Matter · Physics 2010-09-23 Scott T. Milner

To systematically describe evaporation spectra for light and heavy compound nuclei over a large range of excitation energies, it was necessary to consider three ingredients in the statistical model. Firstly, transmission coefficients or…

Nuclear Theory · Physics 2014-11-21 R. J. Charity

A new approach in the investigation of the order parameter behaviour near ferroelectric phase transition point is suggested. The short range and dipole interactions between particles are taken into account. The logarithmic corrections and…

Statistical Mechanics · Physics 2013-07-16 M. A. Korynevskii , V. B. Solovyan

Controlling polymorphism in molecular crystals is crucial in the pharmaceutical, dye, and pesticide industries. However, its theoretical description is extremely challenging, due to the associated long timescales ($ > 1 \, \mu s$). We…

Chemical Physics · Physics 2023-02-09 Oren Elishav , Roy Podgaetsky , Olga Meikler , Barak Hirshberg
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