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NaCl crystal nucleation from metastable solutions has long been considered to occur according to a single-step mechanism. Recent experimental observations suggest that NaCl crystals emerge from disordered intermediates which is seemingly at…

Materials Science · Physics 2022-10-12 Aaron R. Finney , Matteo Salvalaglio

Molecular simulations can provide microscopic insight into the physical and chemical driving forces of complex molecular processes. Despite continued advancement of simulation methodology, model errors may lead to inconsistencies between…

Chemical Physics · Physics 2016-02-12 Joseph F. Rudzinski , Kurt Kremer , Tristan Bereau

Markov state models (MSMs) are a powerful tool to analyze and coarse-grain complex dynamical data into interpretable kinetic processes. This capability is particularly important in heterogeneous catalysis, where a medley of reactants and…

Statistical Mechanics · Physics 2026-05-11 Caitlin A. McCandler , Chatipat Lorpaiboon , Timothy C. Berkelbach , Jutta Rogal

By monitoring the sampling of states with different magnetizations in transition matrix procedures a family of accurate and easily implemented techniques are constructed that automatically control the variation of the temperature or energy…

Statistical Mechanics · Physics 2017-05-24 David Yevick , Yong Hwan Lee

Biochemical reaction networks frequently consist of species evolving on multiple timescales. Stochastic simulations of such networks are often computationally challenging and therefore various methods have been developed to obtain sensible…

Molecular Networks · Quantitative Biology 2017-04-20 Jae Kyoung Kim , Grzegorz A. Rempala , Hye-Won Kang

We study approximations of evolving probability measures by an interacting particle system. The particle system dynamics is a combination of independent Markov chain moves and importance sampling/resampling steps. Under global regularity…

Probability · Mathematics 2011-12-12 Andreas Eberle , Carlo Marinelli

Slow kinetic processes of molecular systems can be analyzed by computing dominant eigenpairs of the Koopman operator or its generator. In this context, the Variational Approach to Markov Processes (VAMP) provides a rigorous way of…

Computational Physics · Physics 2024-02-15 Feliks Nüske , Stefan Klus

MCMC methods (Monte Carlo Markov Chain) are a class of methods used to perform simulations per a probability distribution $P$. These methods are often used when we have difficulties to directly sample per a given probability distribution…

Methodology · Statistics 2014-01-21 Papa Ngom , Badiassiatta Don Bosco Diatta

In this paper we present a modeling approach to bridge the atomistic with macroscopic scales in crystalline materials. The methodology combines identification and modeling of the controlling unit processes at microscopic level with the…

Materials Science · Physics 2009-11-07 A. M. Cuitino , L. Stainier , G. Wang , A. Strachan , T. Cagin , W. A. Goddard , M. Ortiz

We propose a general procedure for estimating the variance-covariance matrix of two-step estimates of structural parameters in latent variable models. The method is partially simulation-based, in that it includes drawing simulated values of…

Methodology · Statistics 2025-07-23 Roberto Di Mari , Jouni Kuha

The non-Markovian nature of polymer motions is accounted for in folding kinetics, using frequency-dependent friction. Folding, like many other problems in the physics of disordered systems, involves barrier crossing on a correlated energy…

Statistical Mechanics · Physics 2009-10-30 Steven S. Plotkin , Peter G. Wolynes

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

Nucleation in supersaturated vapor is investigated with two series of molecular dynamics simulations in the canonical ensemble. The applied methods are: (a) analysis of critical nuclei at moderate supersaturations by simulating equilibria…

Chemical Physics · Physics 2009-11-13 Martin Horsch , Jadran Vrabec , Hans Hasse

Sensitivity analysis is a process of computing sensitivity indices, which are certain measures of importance of parameters in influencing the outputs of mathematical models. Sensitivity indices computed in variance-based sensitivity…

Computation · Statistics 2013-10-04 Tomasz Badowski

We analyze the accuracy and sample complexity of variational Monte Carlo approaches to simulate the dynamics of many-body quantum systems classically. By systematically studying the relevant stochastic estimators, we are able to: (i) prove…

Quantum Physics · Physics 2023-10-11 Alessandro Sinibaldi , Clemens Giuliani , Giuseppe Carleo , Filippo Vicentini

Two-step crystallization via a metastable intermediate phase is often regarded as a non-classical process that lies beyond the framework of classical nucleation theory (CNT). In this work, we investigate two-step crystallization in…

Soft Condensed Matter · Physics 2025-04-10 Willem Gispen , Peter G. Bolhuis , Marjolein Dijkstra

Markov state models (MSMs) have been successful in computing metastable states, slow relaxation timescales and associated structural changes, and stationary or kinetic experimental observables of complex molecules from large amounts of…

Chemical Physics · Physics 2015-06-17 Frank Noe , Hao Wu , Jan-Hendrik Prinz , Nuria Plattner

Estimation and prediction in high dimensional multivariate factor stochastic volatility models is an important and active research area because such models allow a parsimonious representation of multivariate stochastic volatility. Bayesian…

Computation · Statistics 2021-04-27 David Gunawan , Robert Kohn , David Nott

The output of molecular dynamics simulations is high-dimensional, and the degrees of freedom among the atoms are related in intricate ways. Therefore, a variety of analysis frameworks have been introduced in order to distill complex motions…

Biomolecules · Quantitative Biology 2019-08-06 Brooke E. Husic , Frank Noé

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