Related papers: An Improved Ehrenfest Approach to Model Correlated…
A non-adiabatic nuclear wavepacket dynamics simulation of the H$_2$O$^+$ de-excitation process is performed based on electronic structure calculations using the variational quantum eigensolver. The adiabatic potential energy surfaces and…
We present a new approach to calculate real-time quantum dynamics in complex systems. The formalism is based on the partitioning of a system's environment into "core" and "reservoir" modes, with the former to be treated quantum mechanically…
This report presents a new approach for treating the coupling of electrons and nuclei in quantum mechanical calculations for molecules and condensed matter. It includes the standard "Born-Oppenheimer approximation" as a special case but…
A novel quantum dynamical method to simulate vibronic reaction dynamics in molecules at metal surfaces is proposed. The method is based on the hierarchical quantum master equation approach and uses a discrete variable representation of the…
Kinetic equations governing time evolution of positions and momenta of atoms in extended systems are derived using quantum-classical ensembles within the Non-Equilibrium Statistical Operator Method (NESOM). Ions are treated classically,…
We study the semiclassical Ehrenfest trajectories in open quantum systems. We first derive in explicit form the Fokker-Planck equation that governs the time evolution of the mixing measure for a Gaussian mixture. Then, we embed the…
The violation of detailed balance poses a serious problem for the majority of current quasiclassical methods for simulating nonadiabatic dynamics. In order to analyze the severity of the problem, we predict the long-time limits of the…
We study the dynamics of non-adiabatic transitions in non-Hermitian multi-level parabolic models where the separations of the diabatic energies are quadratic function of time. The model Hamiltonian has been used to describe the…
Several methods in nonadiabatic molecular dynamics are based on Madelung's hydrodynamic description of nuclear motion, while the electronic component is treated as a finite-dimensional quantum system. In this context, the quantum potential…
In closed quantum systems, wavepackets can spread exponentially in time due to chaos, forming long-range superpositions in just seconds for ordinary macroscopic systems. A weakly coupled environment is conjectured to decohere the system and…
The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between…
We introduce a novel computational framework for excited-states molecular quantum dynamics simulations driven by quantum computing-based electronic-structure calculations. This framework leverages the fewest-switches surface-hopping method…
A long-standing challenge in mixed quantum-classical trajectory simulations is the treatment of entanglement between the classical and quantal degrees of freedom. We present a novel approach which describes the emergence of entangled states…
We address the nonadiabatic quantum dynamics of macrosystems with several coupled electronic states, taking into account the possibility of multi-state conical intersections. The general situation of an arbitrary number of states and…
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…
We introduce a hybrid classical-quantum algorithm to compute dynamical correlation functions and excitation spectra in many-body quantum systems, with a focus on molecular systems. The method combines classical preparation of a perturbed…
Stochastic Langevin molecular dynamics for nuclei is derived from the Ehrenfest Hamiltonian system (also called quantum classical molecular dynamics) in a Kac-Zwanzig setting, with the initial data for the electrons stochastically perturbed…
Classical simulation of quantum systems plays an important role in the study of many-body phenomena and in the benchmarking and verification of quantum technologies. Exact simulation is often limited to small systems because the dimension…
Simulating electron-ion dynamics using time-dependent density functional theory within an Ehrenfest dynamics scheme can be done in two ways that are in principle exact and identical: propagating time-dependent electronic Kohn-Sham equations…
We introduce a novel methodology for simulating the excited-state dynamics of extensive molecular aggregates in the framework of the long-range corrected time-dependent density-functional tight-binding fragment molecular orbital method…