Related papers: An Improved Ehrenfest Approach to Model Correlated…
A novel treatment of non-adiabatic couplings is proposed. The derivation starts from the long-known, but not well-known, fact that the wave function of the complete system of elctrons and nuclei can be written, without approximation, as a…
Modern X-ray spectroscopy has proven itself as a robust tool for probing the electronic structure of atoms in complex environments. Despite working on energy scales that are much larger than those corresponding to nuclear motions, taking…
Quantum and classical systems evolving under the same formal Hamiltonian $H$ may dramatically differ after the Ehrenfest timescale $t_E \sim \log(\hbar^{-1})$, even as $\hbar \to 0$. Coupling the system to a Markovian environment results in…
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…
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…
It was recently shown [Phys. Rev. Lett. 105, 123002 (2010)] that the complete wavefunction for a system of electrons and nuclei evolving in a time-dependent external potential can be exactly factorized into an electronic wavefunction and a…
Accurately treating electron correlation in the wavefunction is a key challenge for both classical and quantum computational chemistry. Classical methods have been developed which explicitly account for this correlation by incorporating…
Nuclear physics is ideal to test and develop techniques to describe the microscopic dynamics of quantum many-body systems. At low energy, nuclear dynamics is described with non-relativistic approaches based on the mean-field approximation…
We derive an electron-vibration model Hamiltonian in a quantum chemical framework, and explore the extent to which such a Hamiltonian can capture key effects of nonadiabatic dynamics. The model Hamiltonian is a simple two-body operator, and…
A gauge-invariant wave equation for the dynamics of hybrid quantum-classical systems is formulated by combining the variational setting of Lagrangian paths in continuum theories with Koopman wavefunctions in classical mechanics. We identify…
A semiclassical approximation is derived by using a family of wavepackets to map arbitrary wavefunctions into phase space. If the Hamiltonian can be approximated as linear over each individual wavepacket, as often done when presenting…
The static and dynamical properties of a one-dimensional quantum system described by a non-Hermitian Hamiltonian of the so-called Hatano-Nelson type; a tight-binding model with asymmetric (or non-reciprocal) hopping, are studied. The static…
In this work we make a high precision numerical study of the Ehrenfest theorem using the Bohmian approach, where we obtain classical solutions from the quantum trajectories performing the Bohmian averages. We analyse the one-dimensional…
Simulations of interacting electrons and bosons out of equilibrium, starting from first principles and aiming at realistic multiscale scenarios, is a grand theoretical challenge. Here, using the formalism of nonequilibrium Green's functions…
Conservation of energy and momentum in the classical theory of radiating electrons has been a challenging problem since its inception. We propose a formulation of classical electrodynamics in Hamiltonian form that satisfies the Maxwell…
The work is devoted to studying some new classical electrodynamics models of interacting charged point particles and the aspects of the quantization via the Dirac procedure related to them. Based on the vacuum field theory no-geometry…
Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an…
Accurate description of nonadiabatic dynamics of molecules at metal surfaces involving electron transfer has been a longstanding challenge for theory. Here, we tackle this problem by first constructing high-dimensional neural network…
In order to alleviate the computational costs of fully quantum nonadiabatic dynamics, we present a mixed quantum-classical (MQC) particle method based on the theory of Koopman wavefunctions. Although conventional MQC models often suffer…
We show how to evaluate mobility profiles, characterizing the transport of confined fluids under a perturbation, from equilibrium molecular simulations. The correlation functions derived with the Green-Kubo formalism are difficult to sample…