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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

Vibrational spectroscopy is key for probing the interplay between the structure and dynamics of aqueous systems. In order to map different regions of experimental spectra to the microscopic structure of a system, it is important to combine…

Chemical Physics · Physics 2021-08-09 Sam Shepherd , Jinggang Lan , David M. Wilkins , Venkat Kapil

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 properties of molecules and materials containing light nuclei are affected by their quantum mechanical nature. Modelling these quantum nuclear effects accurately requires computationally demanding path integral techniques. Considerable…

Chemical Physics · Physics 2020-04-22 Venkat Kapil , David M. Wilkins , Jinggang Lan , Michele Ceriotti

We present a simple and accurate computational method, which facilitates ab-initio path-integral molecular dynamics simulations, where the quantum mechanical nature of the nuclei is explicitly taken into account, at essentially no…

Chemical Physics · Physics 2016-04-21 Chris John , Thomas Spura , Scott Habershon , Thomas D. Kühne

Recent developments in path integral methodology have significantly reduced the computational expense of including quantum mechanical effects in the nuclear motion in ab initio molecular dynamics simulations. However, the implementation of…

Computational Physics · Physics 2014-02-06 Michele Ceriotti , Joshua More , David E. Manolopoulos

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

In computer simulations, quantum delocalization of atomic nuclei can be modeled making use of the Path Integral (PI) formulation of quantum statistical mechanics. This approach, however, comes with a large computational cost. By restricting…

Statistical Mechanics · Physics 2015-04-13 Karsten Kreis , Mark E. Tuckerman , Davide Donadio , Kurt Kremer , Raffaello Potestio

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

An approximate approach to quantum vibrational dynamics, "Brownian Chain Molecular Dynamics (BCMD)", is proposed to alleviate the chain resonance and curvature problems in the imaginary time-based path integral (PI) simulation. Here the…

Chemical Physics · Physics 2024-01-26 Motoyuki Shiga

Quantum computing has the potential to reduce the computational cost required for quantum dynamics simulations. However, existing quantum algorithms for coupled electron-nuclear dynamics simulation either require fault-tolerant devices, or…

Quantum Physics · Physics 2026-03-03 Jong-Kwon Ha , Ryan J. MacDonell

The development and implementation of increasingly accurate methods for electronic structure calculations mean that, for many atomistic simulation problems, treating light nuclei as classical particles is now one of the most serious…

Materials Science · Physics 2016-02-12 Venkat Kapil , Joost VandeVondele , Michele Ceriotti

The precise description of quantum nuclear fluctuations in atomistic modelling is possible by employing path integral techniques, which involve a considerable computational overhead due to the need of simulating multiple replicas of the…

Chemical Physics · Physics 2017-03-23 Venkat Kapil , Jörg Behler , Michele Ceriotti

Imaginary-time path integral (PI) is a rigorous tool to treat nuclear quantum effects in static properties. However, with its high computational demand, it is crucial to devise precise estimators. We introduce generalized PI estimators for…

Statistical Mechanics · Physics 2024-08-22 Sabry G. Moustafa , Andrew J. Schultz

Spectroscopy is one of the most accurate probes of the molecular world. However, predicting molecular spectra accurately is computationally difficult because of the presence of entanglement between electronic and nuclear degrees of freedom.…

Classical simulation of real-space quantum dynamics is challenging due to the exponential scaling of computational cost with system dimensions. Quantum computer offers the potential to simulate quantum dynamics with polynomial complexity;…

Quantum Physics · Physics 2021-10-13 Chee-Kong Lee , Chang-Yu Hsieh , Shengyu Zhang , Liang Shi

We propose an implementation of quantum logic gates via virtual vibrational excitations in an ion trap quantum computer. Transition paths involving unpopulated, vibrational states interfere destructively to eliminate the dependence of rates…

Quantum Physics · Physics 2009-10-31 Anders Sorensen , Klaus Molmer

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

Bosonic exchange symmetry leads to fascinating quantum phenomena, from exciton condensation in quantum materials to the superfluidity of liquid Helium-4. Unfortunately, path integral molecular dynamics (PIMD) simulations of bosons are…

Computational Physics · Physics 2025-02-18 Yotam M. Y. Feldman , Barak Hirshberg

Accounting for nuclear quantum effects (NQEs) can significantly alter material properties at finite temperatures. Atomic modeling using the path-integral molecular dynamics (PIMD) method can fully account for such effects, but requires…

Materials Science · Physics 2025-05-21 A. A. Solovykh , N. E. Rybin , I. S. Novikov , A. V. Shapeev
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