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Centroid molecular dynamics (CMD) incorporates nuclear quantum statistics into the calculation of vibrational spectra. However, when performed in Cartesian coordinates, CMD shows unphysical artifacts in certain vibrational bands, known as…

Chemical Physics · Physics 2025-11-04 Jorge Castro , George Trenins , Venkat Kapil , Mariana Rossi

Recently, fictitious identical particles have provided a promising way to overcome the fermion sign problem and have been used in path integral Monte Carlo (PIMC) to accurately simulate warm dense matter with up to 1000 electrons (T.…

Quantum Gases · Physics 2025-08-14 Yunuo Xiong , Shujuan Liu , Hongwei Xiong

Path Integral Molecular Dynamics (PIMD) is a well established simulation technique to compute exact equilibrium properties for a quantum system using classical trajectories in an extended phase space. Standard PIMD simulations are…

Chemical Physics · Physics 2024-11-20 Britta A. Johnson , Siyu Bu , Christopher J. Mundy , Nandini Ananth

Quasicentroid molecular dynamics (QCMD) is a path-integral method for approximating nuclear quantum effects in dynamics simulations, which has given promising results for gas- and condensed-phase water. Here, by simulating the infrared…

Chemical Physics · Physics 2021-11-29 Christopher Haggard , Vijay Ganesh Sadhasivam , George Trenins , Stuart C. Althorpe

We introduce a novel approach for a fully quantum description of coupled electron-ion systems from first principles. It combines the variational quantum Monte Carlo (QMC) solution of the electronic part with the path integral (PI) formalism…

Chemical Physics · Physics 2018-03-06 Félix Mouhat , Sandro Sorella , Rodolphe Vuilleumier , Antonino M. Saitta , Michele Casula

Path-integral molecular dynamics (PIMD) simulations have been carried out to study the influence of quantum dynamics of carbon atoms on the properties of a single graphene layer. Finite-temperature properties were analyzed in the range from…

Materials Science · Physics 2016-12-23 Carlos P. Herrero , Rafael Ramirez

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

We recently obtained a quantum-Boltzmann-conserving classical dynamics by making a single change to the derivation of the `Classical Wigner' approximation. Here, we show that the further approximation of this `Matsubara dynamics' gives rise…

Chemical Physics · Physics 2015-05-20 Timothy J. H. Hele , Michael J. Willatt , Andrea Muolo , Stuart C. Althorpe

In this paper, we propose a cost-reduced method for finite-temperature molecular dynamics on a near-term quantum computer, Quantum Car-Parrinello molecular dynamics (QCPMD). One of the most promising applications of near-term quantum…

Quantum Physics · Physics 2022-12-23 Kohdai Kuroiwa , Takahiro Ohkuma , Hirokazu Sato , Ryosuke Imai

We devise an efficient scheme to determine vibrational properties from Path Integral Molecular Dynamics (PIMD) simulations. The method is based on zero-time Kubo-transformed correlation functions and captures the anharmonicity of the…

Materials Science · Physics 2021-06-30 Tommaso Morresi , Lorenzo Paulatto , Rodolphe Vuilleumier , Michele Casula

We describe a fast implementation of the quasi-centroid molecular dynamics (QCMD) method in which the quasi-centroid potential of mean force is approximated as a separable correction to the classical interaction potential. This correction…

Chemical Physics · Physics 2021-11-24 Theo Fletcher , Andrew Zhu , Joseph E. Lawrence , David E. Manolopoulos

Ab-initio molecular dynamics (AIMD) is a powerful tool to simulate physical movements of molecules for investigating properties of materials. While AIMD is successful in some applications, circumventing its high computational costs is…

Quantum Physics · Physics 2024-06-28 Honomi Kashihara , Yudai Suzuki , Kenji Yasuoka

We describe how the fast quasi-centroid molecular dynamics (f-QCMD) method can be applied to condensed phase systems by approximating the quasi-centroid potential of mean force as a sum of inter- and intra-molecular corrections to the…

Chemical Physics · Physics 2023-10-20 Joseph E. Lawrence , Annina Z. Lieberherr , Theo Fletcher , David E. Manolopoulos

Convergence with respect to imaginary-time discretization is an essential part of any path-integral-based calculation. However, an unfortunate property of existing non-preconditioned numerical integration schemes for path-integral molecular…

Chemical Physics · Physics 2020-03-17 Roman Korol , Jorge L. Rosa-Raíces , Nawaf Bou-Rabee , Thomas F. Miller

Including quantum mechanical effects on the dynamics of nuclei in the condensed phase is challenging, because the complexity of exact methods grows exponentially with the number of quantum degrees of freedom. Efforts to circumvent these…

Chemical Physics · Physics 2015-06-23 Mariana Rossi , Hanchao Liu , Francesco Paesani , Joel Bowman , Michele Ceriotti

The quantum harmonic oscillator is the fundamental building block to compute thermal properties of virtually any dielectric crystal at low temperatures in terms of phonons, extended further to cases with anharmonic couplings, or even…

Statistical Mechanics · Physics 2021-10-05 Vladislav Efremkin , Jean-Louis Barrat , Stefano Mossa , Markus Holzmann

The quantum thermal average plays a central role in describing the thermodynamic properties of a quantum system. Path integral molecular dynamics (PIMD) is a prevailing approach for computing quantum thermal averages by approximating the…

Numerical Analysis · Mathematics 2024-06-25 Xuda Ye , Zhennan Zhou

We apply the restricted-path-integral (RPI) theory of non-minimally disturbing continuous measurements for correct description of frictional Brownian motion. The resulting master equation is automatically of the Lindblad form, so that the…

Quantum Physics · Physics 2009-11-07 Michael B. Mensky , Stig Stenholm

For nearly the past 30 years, Centroid Molecular Dynamics (CMD) has proven to be a viable classical-like phase space formulation for the calculation of quantum dynamical properties. However, calculation of the centroid effective force…

Chemical Physics · Physics 2022-09-15 Timothy D. Loose , Patrick G. Sahrmann , Gregory A. Voth

Markov-modulated Brownian motion is a popular tool to model continuous-time phenomena in a stochastic context. The main quantity of interest is the invariant density, which satisfies a differential equation associated with the quadratic…

Probability · Mathematics 2016-05-06 Giang T. Nguyen , Federico Poloni