Chemical Reaction Rates from Ring Polymer Molecular Dynamics: Theory and Practical Applications

Abstract

This Feature Article presents an overview of the current status of Ring Polymer Molecular Dynamics (RPMD) rate theory. We first analyze the RPMD approach and its connection to quantum transition-state theory. We then focus on its practical applications to prototypical chemical reactions in the gas phase, which demonstrate how accurate and reliable RPMD is for calculating thermal chemical reaction rate coefficients in multifarious cases. This review serves as an important checkpoint in RPMD rate theory development, which shows that RPMD is shifting from being just one of recent novel ideas to a well-established and validated alternative to conventional techniques for calculating thermal chemical rate coefficients. We also hope it will motivate further applications of RPMD to various chemical reactions.

References in corpus (13)

• How to remove the spurious resonances from ring polymer molecular dynamics
• Direct simulation of electron transfer using ring polymer molecular dynamics: Comparison with semiclassical instanton theory and exact quantum methods
• Boltzmann-conserving classical dynamics in quantum time-correlation functions: Matsubara dynamics
• Derivation of a true (t->0+) quantum transition-state theory. Part I: Uniqueness and equivalence to ring-polymer molecular dynamics transition-state-theory
• Kinetically Constrained Ring-Polymer Molecular Dynamics for Non-adiabatic Chemical Reactions
• Relation of centroid molecular dynamics and ring-polymer molecular dynamics to exact quantum dynamics
• Ab initio molecular dynamics with nuclear quantum effects at classical cost: ring polymer contraction for density functional theory
• Accurate molecular dynamics and nuclear quantum effects at low cost by multiple steps in real and imaginary time: using density functional theory to accelerate wavefunction methods
• Derivation of a true (t->0+) quantum transition-state theory. II. Recovery of the exact quantum rate in the absence of recrossing
• Quantum Ring-Polymer Contraction Method: Including nuclear quantum effects at no additional computational cost in comparison to ab-initio molecular dynamics
• On the uniqueness of t->0+ quantum transition-state theory
• Should Thermostatted Ring Polymer Molecular Dynamics be used to calculate thermal reaction rates?
• An alternative derivation of ring-polymer molecular dynamics transition-state theory

Cited by in corpus (22)

• Simulating Quantum Materials with Digital Quantum Computers
• An analysis of nonadiabatic ring-polymer molecular dynamics and its application to vibronic spectra
• Automated Calculation of Thermal Rate Coefficients using Ring Polymer Molecular Dynamics and Machine-Learning Interatomic Potentials with Active Learning
• An experimental and theoretical investigation of the C(1D) + D2 reaction
• Gas-phase Elemental abundances in Molecular cloudS (GEMS) III. Unlocking the CS chemistry: the CS+O reaction
• Microcanonical rates from ring-polymer molecular dynamics: Direct-shooting, stationary-phase, and maximum-entropy approaches
• Mean-field Matsubara dynamics: Analysis of path-integral curvature effects in rovibrational spectra
• Thermal quantum time-correlation functions from classical-like dynamics
• Thermal Rate Coefficients for the Astrochemical Process C + CH${}^{+}$ $\to$ C${}_2^{+}$ + H by Ring Polymer Molecular Dynamics
• Testing the quasicentroid molecular dynamics method on gas-phase ammonia
• Nonadiabatic quantum transition-state theory in the golden-rule limit. I. Theory and application to model systems
• Ring Polymer Molecular Dynamics and Active Learning of Moment Tensor Potential for Gas-Phase Barrierless Reactions: Application to S + H2
• Isotopic Separation of Helium through Nanoporous Graphene Membranes: A Ring Polymer Molecular Dynamics Study
• The low temperature D${}^{+}$ + H${}_2$ $\to$ HD + H${}^{+}$ reaction rate coefficient: a ring polymer molecular dynamics and quasi-classical trajectory study
• New Stable and Fast Ring-Polymer Molecular Dynamics for Calculating Bimolecular Rate Coefficients with Example of OH + CH_4
• Quantum rates in dissipative systems with spatially varying friction
• Experimental and theoretical studies of the gas-phase reactions of O(${}^1$D) with H${}_2$O and D${}_2$O at low temperature
• Non-Markovian Effects in Quantum Rate Calculations of Hydrogen Diffusion with Electronic Friction
• Semiclassical Dynamics in Wigner Phase Space I : Adiabatic Hybrid Wigner Dynamics
• Neural Network Potential Energy Surface for the low temperature Ring Polymer Molecular Dynamics of the H2CO + OH reaction
• Ring Polymer Molecular Dynamics in Gas-Surface Reactions: Inclusion of Quantum Effects Made Simple
• Equilibrium-nonequilibrium ring-polymer molecular dynamics for nonlinear spectroscopy