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Nuclear quantum effects (NQEs) remain a major challenge for molecular simulations, as rigorous treatment requires imaginary-time path-integral methods with heavy computational overhead. Neglecting NQEs leads to systematic errors in…

Chemical Physics · Physics 2026-04-14 Jing Shen , Ziyan Ye , Ming-Zheng Du , Shi-Yu He , Dong H. Zhang , Jia-Xi Zeng , Venkat Kapil , Wei Fang

In 2000, Gillespie rehabilitated the chemical Langevin equation (CLE) by describing two conditions that must be satisfied for it yield a valid approximation of the chemical master equation (CME). In this work, we construct an original path…

Quantitative Methods · Quantitative Biology 2020-04-08 John J. Vastola , William R. Holmes

Vibrational spectra of condensed and gas-phase systems containing light nuclei are influenced by their quantum-mechanical behaviour. The quantum dynamics of light nuclei can be approximated by the imaginary time path integral (PI)…

Chemical Physics · Physics 2022-11-23 Félix Musil , Iryna Zaporozhets , Frank Noé , Cecilia Clementi , Venkat Kapil

The chemical Langevin equation (CLE) is a popular simulation method to probe the stochastic dynamics of chemical systems. The CLE's main disadvantage is its break down in finite time due to the problem of evaluating square roots of negative…

Quantitative Methods · Quantitative Biology 2014-07-22 David Schnoerr , Guido Sanguinetti , Ramon Grima

We introduce a machine learning-based approach called ab initio generalized Langevin equation (AIGLE) to model the dynamics of slow collective variables in materials and molecules. In this scheme, the parameters are learned from atomistic…

Computational Physics · Physics 2024-04-02 Pinchen Xie , Roberto Car , Weinan E

We introduce a hybrid projection scheme that combines linear Mori projection and conditional Zwanzig projection techniques and use it to derive a Generalized Langevin Equation (GLE) for a general interacting many-body system. The resulting…

Chemical Physics · Physics 2022-08-31 Cihan Ayaz , Benjamin A. Dalton , Roland R. Netz

The dynamical properties of nuclei, carried by the concept of phonon quasiparticles (QP), are central to the field of condensed matter. While the harmonic approximation can reproduce a number of properties observed in real crystals, the…

Materials Science · Physics 2023-12-19 Aloïs Castellano , J. P. Alvarinhas Batista , Matthieu J. Verstraete

Generalized Langevin dynamics (GLD) arise in the modeling of a number of systems, ranging from structured fluids that exhibit a viscoelastic mechanical response, to biological systems, and other media that exhibit anomalous diffusive…

Computational Physics · Physics 2013-07-25 Andrew D. Baczewski , Stephen D. Bond

Path integral Monte Carlo approach is used to study the coupled quantum dynamics of the electron and nuclei in hydrogen molecule ion. The coupling effects are demonstrated by comparing differences in adiabatic Born--Oppenheimer and…

Chemical Physics · Physics 2008-12-29 I. Kylänpää , M. Leino , T. T. Rantala

Path integral-based simulation methodologies play a crucial role for the investigation of nuclear quantum effects by means of computer simulations. However, these techniques are significantly more demanding than corresponding classical…

Statistical Mechanics · Physics 2018-01-17 Karsten Kreis , Kurt Kremer , Raffaello Potestio , Mark E. Tuckerman

Bistable systems present two degenerate metastable configurations separated by an energy barrier. Thermal or quantum fluctuations can promote the transition between the configurations at a rate which depends on the dynamical properties of…

Statistical Mechanics · Physics 2018-07-23 L. Stella , H. Ness , C. D. Lorenz , L. Kantorovich

We report an improved method for the calculation of tunneling splittings between degenerate configurations in molecules and clusters using path-integral molecular dynamics (PIMD). Starting from an expression involving a ratio of…

Chemical Physics · Physics 2018-03-14 C L Vaillant , D J Wales , S C Althorpe

Recent experiments have confirmed the importance of nuclear quantum effects even in large biomolecules at physiological temperature. Here we describe how the path integral formalism can be used to describe rigorously the nuclear quantum…

Chemical Physics · Physics 2012-07-03 Tomas Zimmermann , Jiri Vanicek

This study employed an artificial intelligence-enhanced molecular simulation framework to enable efficient Path Integral Molecular Dynamics (PIMD) simulations. Owing to its modular architecture and high-throughput capabilities, the…

Chemical Physics · Physics 2025-04-01 Cheng Fan , Maodong Li , Sihao Yuan , Zhaoxin Xie , Dechin Chen , Yi Isaac Yang , Yi Qin Gao

Langevin equations or generalized Langevin equations (GLEs) are popular models for describing the motion of a particle in a fluid medium in an effective manner. Here we examine particles immersed in an inherently nonequilibrium fluid, i.e.,…

Soft Condensed Matter · Physics 2024-05-03 Jeanine Shea , Gerhard Jung , Friederike Schmid

We provide a new paradigm for quantum simulation that is based on path integration that allows quantum speedups to be observed for problems that are more naturally expressed using the path integral formalism rather than the conventional…

Quantum Physics · Physics 2024-10-15 Serene Shum , Nathan Wiebe

Finding the dynamical law of observable quantities lies at the core of physics. Within the particular field of statistical mechanics, the generalized Langevin equation (GLE) comprises a general model for the evolution of observables…

Statistical Mechanics · Physics 2022-11-22 Antonio Russo , Miguel A. Duran-Olivencia , Ioannis G. Kevrekidis , Serafim Kalliadasis

We consider the generalized Langevin equation (GLE) in a harmonic potential with power law decay memory. We study the anomalous diffusion of the particle's displacement and velocity. By comparison with the free particle situation in which…

Probability · Mathematics 2023-08-02 Gustavo Didier , Hung D. Nguyen

Path integral molecular dynamics simulations, combined with an ab initio evaluation of interactions using electronic structure theory, incorporate the quantum mechanical nature of both the electrons and nuclei, which are essential to…

Chemical Physics · Physics 2016-02-15 Ondrej Marsalek , Thomas E. Markland

We introduce a new method to accurately and efficiently estimate the effective dynamics of collective variables in molecular simulations. Such reduced dynamics play an essential role in the study of a broad class of processes, ranging from…

Statistical Mechanics · Physics 2022-03-28 Hadrien Vroylandt , Ludovic Goudenège , Pierre Monmarché , Fabio Pietrucci , Benjamin Rotenberg