Related papers: On Corrections to the Born-Oppenheimer Approximati…
The harmonic approximation of ionic fluctuations and the linear coupling between phonons and electrons provide the standard framework to compute, from first principles, the contribution of nuclear dynamics and its interaction with electrons…
We prove that for a combined system of classical and quantum particles, it is possible to write a dynamics for the classical particles that incorporates in a natural way the Boltzmann equilibrium population for the quantum subsystem. In…
Incorporating nuclear quantum effects into nonadiabatic dynamics remains a significant challenge. Herein we introduce new nonadiabatic dynamics approaches based on the recently developed constrained nuclear-electronic orbital (CNEO) theory.…
Continuum states of the Dirac equation are calculated numerically for the electrostatic field generated by the charge distribution of an atomic nucleus. The behavior of the wave functions of an incoming electron with a given asymptotic…
We incorporate explicit, non-perturbative treatment of spin-orbit coupling into ab initio auxiliary-field quantum Monte Carlo (AFQMC) calculations. The approach allows a general computational framework for molecular and bulk systems in…
Experimental observations of multi-quantum relaxation of highly vibrationally excited NO scattering from Au(111) are a benchmark for the breakdown of Born-Oppenheimer approximation in molecule-surface systems. This remarkable vibrational…
By employing an analytically solvable model including the Duschinsky rotation effect, we investigated the applicability of the commonly used Born-Oppenheimer (BO) approximation for separating the proton and proton donor-acceptor motions in…
Nonadiabatic coupling between electrons and molecular motion at metal surfaces leads to energy dissipation and dynamical steering effects during chemical surface dynamics. We present a theoretical approach to the scattering of molecules…
In this paper we calculate and visualize the dynamics of an ensemble of electrons trapping in an electrostatic wave of slowly increasing amplitude, illustrating that, despite disordering of particles in angle during the trapping transition…
The nonlinear development of the strong Buneman instability and the associated fast electron heating in thin current layers with $\Omega_e/\omega_{pe} <1$ are explored. Phase mixing of the electrons in wave potential troughs and a rapid…
We derive formulas and perform calculations of nonadiabatic corrections to rates of electric quadrupole transitions in the hydrogen molecule. These corrections can be represented in terms of the quadrupole moment curve $D^{(1)}(R)$,…
We present a universal expression for the electronic friction as felt by a set of classical nuclear degrees of freedom (DoF's) coupled to a manifold of quantum electronic DoF's; no assumptions are made regarding the nature of the electronic…
We theoretically study nonadiabatic corrections for charge pumping in a noninteracting electron model of a single-level quantum dot. We derive a formula for the velocity limit of parameter driving to realize adiabatic pumping and illustrate…
Many areas of physics rely upon adiabatic state transfer protocols, allowing a quantum state to be moved between different physical systems for storage and retrieval or state manipulation. However, these state-transfer protocols suffer from…
Alchemical transformations showed that perturbation theory can be applied also to changes in the atomic nuclear charges of a molecule. The alchemical path that connects two different chemical species involves the conceptualization of a…
The main concern of the present paper is the study of the multi-scale dynamics of thermonuclear fusion plasmas via a multi-species Fokker-Planck kinetic model. One of the goals is the generalization of the standard Fokker-Planck collision…
We consider nonadiabatic systems in which the classical Born-Oppenheimer approximation breaks down. We present a general theory that accurately captures the full transmitted wavepacket after multiple transitions through either a single or…
There is currently much interest in the development of improved trajectory-based methods for the simulation of nonadiabatic processes in complex systems. An important goal for such methods is the accurate calculation of the rate constant…
Adiabatic quantum pumping in noninteracting, phase coherent quantum dots is elegantly described by Brouwer's formula. Interactions within the dot, while suppressing phase coherence, make Brouwer's formalism inapplicable. In this paper, we…
We show how the dynamically nonlocal formulation of classical nuclear motion in the presence of quantal electronic transitions presented many years ago by Pechukas can be localized in time using time dependent perturbation theory to give an…