相关论文: Born-Oppenheimer Dynamics, Electronic Friction, an…

A theory of electronic friction is developed using the exact factorization of the electron-nuclear wavefunction. No assumption is made regarding the electronic bath, which can be made of independent or interacting electrons, and the nuclei…

When the coupled electron-nuclear dynamics are subjected to strong Floquet driving, there is a strong breakdown of the Born-Oppenheimer approximation. In this article, we derive a Fokker-Planck equation to describe non-adiabatic molecular…

We derive an explicit form for the electronic friction as felt by a molecule near a metal surface for the general case that molecule-metal couplings depend on nuclear coordinates. Our work generalizes a previous study by von Oppen et al…

The break-down of the Born-Oppenheimer approximation is an important topic in chemical dynamics on metal surfaces. In this context, the most frequently used "work-horse" is electronic friction theory, commonly relying on friction…

Molecular adsorbates on metal surfaces exchange energy with substrate phonons and low-lying electron-hole pair excitations. In the limit of weak coupling, electron-hole pair excitations can be seen as exerting frictional forces on…

We analyze the entanglement between electronic and nuclear motions in molecular wave functions, by using different widely used ansatzes in molecular Hamiltonian models (H$^+_2$ in 1D and the Shin-Metiu model); namely, i) Born-Oppenheimer…

A model detector undergoing constant, infinite-duration acceleration converges to an equilibrium state described by the Hawking-Unruh temperature $T_a=(a/2\pi)(\hbar/c)$. To relate this prediction to experimental observables, a point-like…

The assumptions underpinning the adiabatic Born-Oppenheimer (BO) approximation are broken for molecules interacting with attosecond laser pulses, which generate complicated coupled electronic-nuclear wavepackets that generally will have…

We introduce a theory that exposes the fundamental and previously overlooked connection between the correlation among electrons and the degree of quantum coherence of electronic states in matter. For arbitrary states, the effects only…

Photoionization using attosecond pulses can lead to the formation of coherent superpositions of the electronic states of the parent ion. However, ultrafast electron ejection triggers not only electronic but also nuclear dynamics---leading…

The electronic friction-Langevin dynamics (EF-LD) offers a simplified framework for describing nonadiabatic effects at metal surfaces, particularly in electrochemical and molecular electronic applications. We investigate the electronic…

This article presents a systematic theoretical enquiry concerning the conceptual foundations and the nature of phonon-mediated electron-electron interactions. Starting from the fundamental many-body Hamiltonian, we propose a simple scheme…

An accurate description of nonadiabatic energy relaxation is crucial for modeling atomistic dynamics at metal surfaces. Interfacial energy transfer due to electron-hole pair excitations coupled to motion of molecular adsorbates is often…

The non-equilibrium dynamics of electrons is of a great experimental and theoretical value providing important microscopic parameters of the Coulomb and electron-phonon interactions in metals and other cold plasmas. Because of the…

We present a novel theory and implementation for computing coupled electronic and quantal nuclear subsystems on a single potential energy surface, moving beyond the standard Born-Oppenheimer (BO) separation of nuclei and electrons. We…

We develop a density matrix formalism to describe coupled electron-nuclear dynamics. To this end we introduce an effective Hamiltonian formalism that describes electronic transitions and small (quantum) nuclear fluctuations along a…

In this work we develop a theory of correlated many-electron dynamics dressed by the presence of a finite-temperature harmonic bath. The theory is based on the ab-initio Hamiltonian, and thus well-defined apart from any phenomenological…

This paper presents the calculation of the electric transition dipole moment in a pre-Born-Oppenheimer framework. Electrons and nuclei are treated equally in terms of the parametrization of the non-relativistic total wave function, which is…

Electronic friction-Langevin dynamics (EF-LD) provides an efficient framework for capturing nonadiabatic effects at solid surfaces, with particular relevance to electrochemistry and molecular electronics. In this work, we investigate…

The thermal friction force acting on an atom moving relative to a thermal photon bath has recently been calculated on the basis of the fluctuation-dissipation theorem. The thermal fluctuations of the electromagnetic field give rise to a…