Quantum Dynamics with Electronic Friction

Abstract

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 are treated quantally. The ensuing equation of motion for the nuclear wavefunction is a non-linear Schrödinger equation including a friction term. The resulting friction kernel agrees with a previously derived mixed quantum-classical result by Dou, Miao \& Subotnik (\emph{Phys. Rev. Lett.} \textbf{119}, 046001 (2017)), except for a \emph{pseudo}-magnetic contribution in the latter that is here removed. More specifically, it is shown that the electron dynamics generally washes out the\emph{ gauge} fields appearing in the adiabatic dynamics. However, at T=0 K, the \emph{pseudo}-magnetic force is fully re-established in the typical situation where the electrons respond rapidy on the slow time-scale of the nuclear dynamics (Markov limit). Hence, we predict Berry's phase effects to be observable also in the presence of electronic friction, and non-trivial geometric phases should be attainable for molecules on metallic magnetic surfaces.

20 pages (with Supplemental Material)

References in corpus (5)

• Scattering theory of current-induced forces in mesoscopic systems
• Current-induced atomic dynamics, instabilities, and Raman signals: Quasi-classical Langevin equation approach
• Ab-initio tensorial electronic friction for molecules on metal surfaces: nonadiabatic vibrational relaxation
• Symmetry-Adapted High Dimensional Neural Network Representation of Electronic Friction Tensor of Adsorbates on Metals
• Electron corrected Lorentz forces in solids and molecules in magnetic field

Cited by in corpus (10)

• i-PI 3.0: a flexible and efficient framework for advanced atomistic simulations
• Classical quantum friction at water-carbon interfaces
• Total Angular Momentum Conservation in Ab Initio Born-Oppenheimer Molecular Dynamics
• Assessing mixed quantum-classical molecular dynamics methods for nonadiabatic dynamics of molecules on metal surfaces
• Floquet driven frictional effects
• Local diabatic representation of conical intersection quantum dynamics
• Current-induced forces in nanosystems: A hierarchical equations of motion approach
• Quantum rates in dissipative systems with spatially varying friction
• Dynamics with Simultaneous Dissipations to Fermionic and Bosonic Reservoirs
• NQCDynamics.jl: A Julia Package for Nonadiabatic Quantum Classical Molecular Dynamics in the Condensed Phase