相关论文: Automated Calculation of Thermal Rate Coefficients…
Mean-field Ring Polymer Molecular Dynamics (MF-RPMD) offers a computationally efficient method for the simulation of reaction rates in multi-level systems. Previous work has established that, to model a nonadiabatic state-to-state reaction…
A new potential energy surface (PES) and dynamical study are presented of the reactive process between H2CO + OH towards the formation of HCO + H2O and HCOOH + H. In this work a source of spurious long range interactions in symmetry adapted…
Mean-Field Ring Polymer Molecular Dynamics (MF-RPMD) is a powerful, efficient, and accurate method for approximate quantum dynamic simulations of multi-level system dynamics. Initial efforts to compute nonadiabatic reaction rates using…
Ab initio molecular dynamics (AIMD) simulations employing density functional theory (DFT) and plane waves are routinely carried out using density functionals at the level of Generalized Gradient Approximation (GGA). AIMD simulations…
The reaction between D$^+$ and H$_2$ plays an important role in astrochemistry at low temperatures and also serves as a prototype for simple ion-molecule reaction. Its ground $\tilde{X}~^1A^{\prime}$ state has a very small thermodynamic…
We train an equivariant machine learning model to predict energies and forces for a real-world study of hydrogen combustion under conditions of finite temperature and pressure. This challenging case for reactive chemistry illustrates that…
Here, we demonstrate how machine learning enables the prediction of comonomers reactivity ratios based on the molecular structure of monomers. We combined multi-task learning, multi-inputs, and Graph Attention Network to build a model…
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…
Computing accurate rate constants for catalytic events occurring at the surface of a given material represents a challenging task with multiple potential applications in chemistry. To address this question, we propose an approach based on a…
We introduce mapping-variable ring polymer molecular dynamics (MV-RPMD), a model dynamics for the direct simulation of multi-electron processes. An extension of the RPMD idea, this method is based on an exact, imaginary time path-integral…
Real-time acquisition of accurate machine parameters is of significance to achieving high performance in electric drives, particularly targeted for mission-critical applications. Unlike the saturation effects, the temperature variations are…
The temperature dependence of the thermal rate constant for the reaction Cl($^2$P) + CH$_4$ $\rightarrow$ CH$_3$ + HCl is calculated using a Gaussian Process machine learning (ML) approach to train on and predict thermal rate constants over…
Predicting monomer reactivity ratios is crucial for controlling monomer sequence distribution in copolymers and their properties. Traditional experimental methods of determining reactivity ratios are time-consuming and resource-intensive,…
Simulations of chemical reaction probabilities in gas surface dynamics require the calculation of ensemble averages over many tens of thousands of reaction events to predict dynamical observables that can be compared to experiments. At the…
Accurately modeling gas-surface collision dynamics presents a great challenge for theory, especially in the low energy (or temperature) regime where quantum effects are important. Here, a path integral based non-equilibrium ring polymer…
Temperature is a fundamental regulator of chemical and biochemical kinetics, yet capturing nonlinear thermal effects directly from experimental data remains a major challenge due to limited throughput and model flexibility. Recent advances…
Machine-learning-based interatomic potential energy surface (PES) models are revolutionizing the field of molecular modeling. However, although much faster than electronic structure schemes, these models suffer from costly computations via…
We investigate whether making the friction spatially dependent on the reaction coordinate introduces quantum effects into the thermal reaction rates for dissipative reactions. Quantum rates are calculated using the numerically exact…
We present an analytical model for calculating the thermodynamic properties of monoatomic liquids using a rough potential energy surface (PES). The PES is transformed into an equivalent simple harmonic oscillator. Without employing any…
An exact approach to compute physical properties for general multi-electronic-state (MES) systems in thermal equilibrium is presented. The approach is extended from our recent progress on path integral molecular dynamics (PIMD) [J. Chem.…