相关论文: Initial Sampling in Symmetrical Quasiclassical Dyn…

The symmetrical quasi-classical dynamics method based on the Meyer-Miller mapping Hamiltonian (MM-SQC) shows the great potential in the treatment of the nonadiabatic dynamics of complex systems. We performed the comprehensive benchmark…

The supervised machine learning (ML) approach is applied to realize the trajectory-based nonadiabatic dynamics within the framework of the symmetrical quasi-classical dynamics method based on the Meyer-Miller mapping Hamiltonian (MM-SQC).…

We perform on-the-fly non-adiabatic molecular dynamics simulations using the symmetrical quasi-classical (SQC) approach with the recently suggested molecular Tully models: ethylene and fulvene. We attempt to provide benchmarks of the SQC…

Mixed-quantum classical (MQC) methods for simulating the dynamics of molecules at metal surfaces have the potential to accurately and efficiently provide mechanistic insight into reactive processes. Here, we introduce simple two-dimensional…

Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…

Efficient sampling from high-dimensional distributions is a challenging issue which is encountered in many large data recovery problems involving Markov chain Monte Carlo schemes. In this context, sampling using Hamiltonian dynamics is one…

We extend the Mixed Quantum-Classical Initial Value Representation (MQC-IVR), a semiclassical method for computing real-time correlation functions, to electronically nonadiabatic systems using the Meyer-Miller-Stock-Thoss (MMST) Hamiltonian…

We propose a quantum Monte Carlo (QMC) algorithm for non-equilibrium dynamics in a system with a parameter varying as a function of time. The method is based on successive applications of an evolving Hamiltonian to an initial state and…

Hamiltonian Monte Carlo (HMC) is an efficient Bayesian sampling method that can make distant proposals in the parameter space by simulating a Hamiltonian dynamical system. Despite its popularity in machine learning and data science, HMC is…

Hamiltonian Monte Carlo (HMC) is a state of the art method for sampling from distributions with differentiable densities, but can converge slowly when applied to challenging multimodal problems. Running HMC with a time varying Hamiltonian,…

We apply a recently developed quasi-diabatic (QD) scheme to the symmetric quasi-classical (SQC) approach for accurate quantum dynamics propagation. By using the adiabatic states as the quasi-diabatic states during a short-time quantum…

Robust control design for quantum systems has been recognized as a key task in the development of practical quantum technology. In this paper, we present a systematic numerical methodology of sampling-based learning control (SLC) for…

Quantum molecular dynamics requires an accurate representation of the molecular potential energy surface from a minimal number of electronic structure calculations, particularly for nonadiabatic dynamics where excited states are required.…

Sampling from an unnormalized probability distribution is a fundamental problem in machine learning with applications including Bayesian modeling, latent factor inference, and energy-based model training. After decades of research,…

In the previous paper [J. R. Mannouch and J. O. Richardson, J.~Chem.~Phys.~xxx, xxxxx (xxxx)] we derived a new partially linearized mapping-based classical-trajectory technique, called spin-PLDM. This method describes the dynamics…

Nonadiabatic dynamics methods are an essential tool for investigating photochemical processes. In the context of employing first principles electronic structure techniques, such simulations can be carried out in a practical manner using…

Excited-state molecular dynamics (ESMD) simulations near conical intersections (CIs) pose significant challenges when using machine learning potentials (MLPs). Although MLPs have gained recognition for their integration into mixed…

Diabatization of the molecular Hamiltonian is a standard approach to removing the singularities of nonadiabatic couplings at conical intersections of adiabatic potential energy surfaces. In general, it is impossible to eliminate the…

Simulating the nonadiabatic dynamics of condensed-phase systems continues to pose a significant challenge for quantum dynamics methods. Approaches based on sampling classical trajectories within the mapping formalism, such as the linearized…

We simulate the nonadiabatic dynamics of photo-induced isomerization and dissociation in ethylene using ab initio classical trajectories in an extended phase space of nuclear and electronic variables. This is achieved by employing the…