Related papers: High-order geometric integrators for representatio…

Nonadiabatic effects in chemical reaction at metal surfaces, due to excitation of electron-hole pairs, stand at the frontier of the studies of gas-surface reaction dynamics. However, the first principles description of electronic excitation…

We propose Ehrenfest Dynamics with Spontaneous Localization (SLED), a decoherence-corrected extension of Ehrenfest dynamics based on the Gisin-Percival quantum-state diffusion (QSD) equation. In SLED, the electronic wavefunction evolves…

In the last two decades, significant effort has been put in understanding and designing so-called structure-preserving numerical methods for the simulation of mechanical systems. Geometric integrators attempt to preserve the geometry…

A first-principles coupled electron-nuclear dynamics simulation based on real-time, time-dependent density functional theory and Ehrenfest dynamics quantitatively repro-duces bimodal translational energy loss and angular distributions…

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…

Far out-of-equilibrium many-body quantum dynamics in isolated systems necessarily generate interferences beyond an Ehrenfest time scale, where quantum and classical expectation values diverge. Of great recent interest is the role these…

Among the single-trajectory Gaussian-based methods for solving the time-dependent Schr\"{o}dinger equation, the variational Gaussian approximation is the most accurate one. In contrast to Heller's original thawed Gaussian approximation, it…

This work proposes a suite of numerical techniques to facilitate the design of structure-preserving integrators for nonlinear dynamics. The celebrated LaBudde-Greenspan integrator and various energy-momentum schemes adopt a difference…

We investigated the high-order harmonic generation (HHG) process of diatomic molecular ion $\mathrm{H}_2^+$ in non-Born-Oppenheimer approximations. The corresponding three-dimensional time-dependent Schr\"odinger equation is solved with…

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…

Chemical relaxation phenomena, including photochemistry and electron transfer processes, form a vigorous area of research in which nonadiabatic dynamics plays a fundamental role. Here, we show that for nonadiabatic dynamics with two…

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…

Nonequilibrium electronic forces play a central role in voltage-driven phase transitions but are notoriously expensive to evaluate in dynamical simulations. Here we develop a machine learning framework for adiabatic lattice dynamics coupled…

The force exerted by the electrons on the nuclei of a current-carrying molecular junction can be manipulated to engineer nanoscale mechanical systems. In the adiabatic regime a peculiarity of these forces is negative friction, responsible…

The so-called Born-Huang ansatz is a fundamental tool in the context of ab-initio molecular dynamics, viz., it allows to effectively separate fast and slow degrees of freedom and thus treating electrons and nuclei at different mathematical…

Recently introduced methods which result in shortcuts to adiabaticity, particularly in the context of frictionless cooling, are rederived and discussed in the framework of an approach based on Ehrenfest dynamics. This construction provides…

We propose explicit symplectic integrators of molecular dynamics (MD) algorithms for rigid-body molecules in the canonical and isothermal-isobaric ensembles. We also present a symplectic algorithm in the constant normal pressure and lateral…

Using a generalized energy-conserving transition probability, it is shown how nonadiabatic calculations, within the Wigner-Heisenberg representation of quantum mechanics, can be reliably extended to far longer times than those allowed by a…

Symplectic integrators that preserve the geometric structure of Hamiltonian flows and do not exhibit secular growth in energy errors are suitable for the long-term integration of N-body Hamiltonian systems in the solar system. However, the…

Single-Hessian Gaussian wavepacket dynamics (GWD) significantly reduces the computational burden of Heller's local harmonic GWD, while maintaining comparable accuracy in approximating vibronic spectra. Here, we provide a new, symplectic…