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Parameterized artificial neural networks (ANNs) can be very expressive ansatzes for variational algorithms, reaching state-of-the-art energies on many quantum many-body Hamiltonians. Nevertheless, the training of the ANN can be slow and…

Quantum Physics · Physics 2025-06-04 Conor Smith , Quinn T. Campbell , Tameem Albash

The transition interface sampling (TIS) technique allows to overcome large free energy barriers within reasonable simulation time, which is impossible for straightforward molecular dynamics. Still, the method does not impose an artificial…

Statistical Mechanics · Physics 2017-09-13 Titus S. van Erp , Tom P. Caremans , Christine E. A. Kirschhock , Johan A. Martens

Recent advances in random-walk particle-tracking have enabled direct simulation of mixing and reactions on particles by allowing the particles to interact with each other using a multi-point mass transfer scheme. The mass transfer scheme…

Computational Physics · Physics 2019-04-22 Nicholas B. Engdahl , Michael J. Schmidt , David A. Benson

We investigate the theoretical foundations of the simulated tempering method and use our findings to design efficient algorithms. Employing a large deviation argument first used for replica exchange molecular dynamics [Plattner et al., J.…

Chemical Physics · Physics 2019-02-08 Anton Martinsson , Jianfeng Lu , Benedict Leimkuhler , Eric Vanden-Eijnden

Diffusion models are powerful generative models but suffer from slow sampling, often taking 1000 sequential denoising steps for one sample. As a result, considerable efforts have been directed toward reducing the number of denoising steps,…

Machine Learning · Computer Science 2023-10-17 Andy Shih , Suneel Belkhale , Stefano Ermon , Dorsa Sadigh , Nima Anari

Understanding transition pathways between two meta-stable states of a molecular system is crucial to advance drug discovery and material design. However, unbiased molecular dynamics (MD) simulations are computationally infeasible because of…

Machine Learning · Computer Science 2025-01-28 Kiyoung Seong , Seonghyun Park , Seonghwan Kim , Woo Youn Kim , Sungsoo Ahn

Path sampling approaches have become invaluable tools to explore the mechanisms and dynamics of so-called rare events that are characterized by transitions between metastable states separated by sizeable free energy barriers. Their…

Statistical Mechanics · Physics 2022-06-08 Steven W. Hall , Grisell Díaz Leines , Sapna Sarupria , Jutta Rogal

Transition path sampling (TPS) is a powerful technique for investigating rare transitions, especially when the mechanism is unknown and one does not have access to the reaction coordinate. Straightforward application of TPS does not…

Chemical Physics · Physics 2019-07-11 Z. Faidon Brotzakis , Peter G. Bolhuis

Massively parallel computer architectures create new opportunities for the performance of long-timescale molecular dynamics (MD) simulations. Here, we introduce the path-accelerated molecular dynamics (PAMD) method that takes advantage of…

Computational Physics · Physics 2021-01-11 Jorge L. Rosa-Raíces , Bin Zhang , Thomas F. Miller

Simulations with an adaptive time-dependent bias, such as metadynamics, enable an efficient exploration of the conformational space of a system. However, the dynamic information of the system is altered by the bias. With infrequent…

We study by computer simulation the nucleation of a supersaturated Lennard-Jones vapor into the liquid phase. The large free energy barriers to transition make the time scale of this process impossible to study by ordinary molecular…

Statistical Mechanics · Physics 2018-08-15 Pablo M. Piaggi , Omar Valsson , Michele Parrinello

A new approach to simulating warm and hot dense matter that combines density functional theory based calculations of the electronic structure to classical molecular dynamics simulations with pair interaction potentials is presented. The new…

Plasma Physics · Physics 2015-06-22 C. E. Starrett , J. Daligault , D. Saumon

Recent advances in powerful pre-trained diffusion models encourage the development of methods to improve the sampling performance under well-trained diffusion models. This paper introduces Diffusion Rejection Sampling (DiffRS), which uses a…

Machine Learning · Computer Science 2024-05-29 Byeonghu Na , Yeongmin Kim , Minsang Park , Donghyeok Shin , Wanmo Kang , Il-Chul Moon

In this article, we propose an efficient method for sampling the relevant state space in condensed phase reactions. In the present method, the reaction is described by solving the electronic Schr\"{o}dinger equation for the solute atoms in…

Chemical Physics · Physics 2009-11-10 Radu Iftimie , Dennis Salahub , Jeremy Schofield

Accurately modeling chemical reactions in molecular dynamics simulations requires detailed pre- and post-reaction templates, often created through labor-intensive manual workflows. This work introduces a Python-based algorithm that…

Computational Engineering, Finance, and Science · Computer Science 2025-07-24 Julian Konrad , Robert Meißner

We present a time dependent variational method to learn the mechanisms of equilibrium reactive processes and efficiently evaluate their rates within a transition path ensemble. This approach builds off variational path sampling methodology…

Chemical Physics · Physics 2023-07-10 Aditya N. Singh , David T. Limmer

We introduce a rigorous method to microscopically compute the observables which characterize the thermodynamics and kinetics of rare macromolecular transitions for which it is possible to identify a priori a slow reaction coordinate. In…

Biomolecules · Quantitative Biology 2015-06-05 P. Faccioli , F. Pederiva

The computational study of conformational transitions in RNA and proteins with atomistic molecular dynamics often requires suitable enhanced sampling techniques. We here introduce a novel method where concurrent metadynamics are integrated…

Computational Physics · Physics 2015-09-01 Alejandro Gil-Ley , Giovanni Bussi

Simulation of surface processes is a key part of computational chemistry that offers atomic-scale insights into mechanisms of heterogeneous catalysis, diffusion dynamics, as well as quantum tunneling phenomena. The most common theoretical…

Chemical Physics · Physics 2023-05-01 Wei Fang , Yu-Cheng Zhu , Yi-Han Cheng , Yi-Ping Hao , Jeremy O. Richardson

Stochastic reaction networks that exhibit bistability are common in many fields such as systems biology and materials science. Sampling of the stationary distribution is crucial for understanding and characterizing the long term dynamics of…

Numerical Analysis · Mathematics 2018-01-17 Ting Wang , Petr Plecháč