Born-Oppenheimer Dynamics, Electronic Friction, and the Inclusion of Electron-Electron Interactions

Abstract

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 Hamiltonian and electron-electron repulsions are allowed. Our derivation is based on a quantum-classical Liouville equation (QCLE) for the coupled electronic-nuclear motion, followed by an adiabatic approximation whereby electronic transitions are assumed to equilibrate faster than nuclear movement. The resulting form of friction is completely general, but does reduce to previously published expressions for the quadratic Hamiltonian (i.e. Hamiltonians without electronic correlation). At equilibrium, the second fluctuation-dissipation theorem is satisfied and the frictional matrix is symmetric. To demonstrate the importance of electron-electron correlation, we study electronic friction within the Anderson-Holstein model, where a proper treatment of electron-electron interactions shows signatures of a Kondo resonance and a mean-field treatment is completely inadequate.

References in corpus (9)

• The numerical renormalization group method for quantum impurity systems
• Molecular Transport Junctions: Vibrational Effects
• 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
• Spectral Functions of the Uniform Electron Gas via Coupled-Cluster Theory and Comparison to the $GW$ and Related Approximations
• Phonon runaway in nanotube quantum dots
• Out-of-equilibrium catalysis of chemical reactions by electronic tunnel currents
• Electronic friction near metal surfaces: a case where molecule-metal couplings depend on nuclear coordinates
• Mixed quantum-classical dynamics using collective electronic variables: A better alternative to electronic friction theories

Cited by in corpus (48)

• i-PI 3.0: a flexible and efficient framework for advanced atomistic simulations
• A universal approach to quantum thermodynamics in the strong coupling regime
• Spin Polarization through A Molecular Junction Based on Nuclear Berry Curvature Effects
• Current-induced forces for nonadiabatic molecular dynamics
• Electron-mediated phonon-phonon coupling drives the vibrational relaxation of CO on Cu(100)
• The universality of electronic friction II: Equivalence of the quantum-classical Liouville equation approach with von Oppen's nonequilibrium Green's function methods out of equilibrium
• Spintronics meets nonadiabatic molecular dynamics: Geometric spin torque and damping on noncollinear classical magnetism due to electronic open quantum system
• Molecular junctions and molecular motors: Including Coulomb repulsion in electronic friction using nonequilibrium Green's functions
• Lead Geometry and Transport Statistics in Molecular Junctions
• Current-induced atomic motion, structural instabilities, and negative temperatures on molecule-electrode interfaces in electronic junctions
• Assessing mixed quantum-classical molecular dynamics methods for nonadiabatic dynamics of molecules on metal surfaces
• Universal approach to quantum thermodynamics of strongly coupled systems under nonequilibrium conditions and external driving
• Vibrational Relaxation at a Metal Surface: Electronic Friction Versus Classical Master Equations
• A Demonstration of Consistency between the Quantum Classical Liouville Equation and Berry's Phase and Curvature
• Quantum Dynamics with Electronic Friction
• Timescale separation solution of Kadanoff-Baym equations for quantum transport in time-dependent fields
• First-passage time theory of activated rate chemical processes in electronic molecular junctions
• Electronic friction in interacting systems
• Non-Adiabatic Effects of Nuclear Motion in Quantum Transport of Electrons: A Self-Consistent Keldysh-Langevin Study
• Non-equilibrium Green's function theory for non-adiabatic effects in quantum transport: inclusion of electron-electron interactions
• Cooling molecular electronic junctions by AC current
• Dissipative Tunneling Rates through the Incorporation of First-Principles Electronic Friction in Instanton Rate Theory I: Theory
• Dissipative Tunneling Rates through the Incorporation of First-Principles Electronic Friction in Instanton Rate Theory II: Benchmarks and Applications
• Floquet driven frictional effects
• One-body Langevin dynamics in heavy-ion collisions at intermediate energies
• Nonadiabatic corrections to electric current in molecular junction due to nuclear motion at the molecule-electrode interfaces
• Current-induced forces in nanosystems: A hierarchical equations of motion approach
• Emergence of negative viscosities and colored noise under current-driven Ehrenfest molecular dynamics
• On the Breakdown of the Ehrenfest Method for Molecular Dynamics on Surfaces
• Non-Adiabatic Quantum Molecular Dynamics with Detailed Balance
• Should it really be that hard to model the chirality induced spin selectivity effect?
• Electronic Friction Near Metal Surface: Incorporating Nuclear Quantum Effect with Ring Polymer Molecular Dynamics
• Transport and thermodynamics in quantum junctions: A scattering approach
• A complete quasiclassical map for the dynamics of interacting fermions
• Numerical study of non-adiabatic quantum thermodynamics of the driven resonant level model: Non-equilibrium entropy production and higher order corrections
• Analytic Gradients and Derivative Couplings for Configuration Interaction with All Single Excitations and One Double Excitation -- En Route to Nonadiabatic Dynamics
• Configuration interaction approaches for solving quantum impurity models
• Viscous current-induced forces
• Electron transfer at electrode interfaces via a straightforward quasiclassical fermionic mapping approach
• Boosting current-induced molecular dynamics with machine-learning potential
• Dynamics with Simultaneous Dissipations to Fermionic and Bosonic Reservoirs
• A semiclassical nonequilibrium Green's Function approach to electron transport in systems exhibiting electron-phonon couplings
• Orbital Surface Hopping with an Electron Thermostat Yields Accurate Dynamics and Detailed Balance
• Nonadiabatic dynamics at metal surfaces: fewest switches surface hopping with electronic relaxation
• An Antisymmetric Berry Frictional Force At Equilibrium in the Presence of Spin-Orbit Coupling
• Stochastic Schrödinger equation approach to real-time dynamics of Anderson-Holstein impurities: an open quantum system perspective
• Motion-driven quantum dissipation in an open electronic system with nonlocal interaction
• NQCDynamics.jl: A Julia Package for Nonadiabatic Quantum Classical Molecular Dynamics in the Condensed Phase