Nuclear dynamics at molecule-metal interfaces: A pseudoparticle perspective

Abstract

We discuss nuclear dynamics at molecule-metal interfaces including non-equilibrium molecular junctions. Starting from the many-body states (pseudoparticle) formulation of the molecule-metal system in the molecular vibronic basis, we introduce gradient expansion in order to reduce the adiabatic nuclear dynamics (that is, nuclear dynamics on a single molecular potential surface) into its semi-classical form while maintaining the effect of the non-adiabatic electronic transitions between different molecular charge states. This yields a set of equations for the nuclear dynamics in the presence of these non-adiabatic transitions, which reproduce surface hopping formulation in the limit of small metal-molecule coupling (where broadening of the molecular energy levels can be disregarded) and Ehrenfest dynamics (motion on the potential of mean force) when information on the different charging states is traced out, which is relevant when this coupling is strong.

9 pages

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Cited by in corpus (18)

• Green's function methods for single molecule junctions
• Current-induced forces for nonadiabatic molecular dynamics
• Chemical Reaction Rates for Systems with Spin-Orbit Coupling and an Odd Number of Electrons: Does Berry's Phase Lead to Meaningful Spin-Dependent Nuclear Dynamics for a Two State Crossing?
• 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
• Hierarchical quantum master equation approach to vibronic reaction dynamics at metal surfaces
• Current-induced atomic motion, structural instabilities, and negative temperatures on molecule-electrode interfaces in electronic junctions
• Nonequilibrium reaction rate theory: Formulation and implementation within the hierarchical equations of motion approach
• Vibrational Relaxation at a Metal Surface: Electronic Friction Versus Classical Master Equations
• Coupled Wavepackets for Non-Adiabatic Molecular Dynamics: A Generalization of Gaussian Wavepacket Dynamics to Multiple Potential Energy Surfaces
• Non-Adiabatic Effects of Nuclear Motion in Quantum Transport of Electrons: A Self-Consistent Keldysh-Langevin Study
• Nonequilibrium Green's function theory for nonadiabatic effects in quantum electron transport
• Non-equilibrium Green's function theory for non-adiabatic effects in quantum transport: inclusion of electron-electron interactions
• Energy Transfer and Thermoelectricity in Molecular Junctions in Non-Equilibrated Solvents
• Floquet driven frictional effects
• Nonadiabatic corrections to electric current in molecular junction due to nuclear motion at the molecule-electrode interfaces
• Orbital Surface Hopping with an Electron Thermostat Yields Accurate Dynamics and Detailed Balance
• An Antisymmetric Berry Frictional Force At Equilibrium in the Presence of Spin-Orbit Coupling
• Nonadiabatic dynamics at metal surfaces: fewest switches surface hopping with electronic relaxation