Nuclear Dynamics at Molecule–Metal Interfaces: A Pseudoparticle Perspective

2015/09/21 by Michael Galperin, Abraham Nitzan · 35 citations
Engineering · Physics and Astronomy · #Artificial intelligence #Computer science #Dynamics (music) #Instanton #Molecular Junctions and Nanostructures #Perspective (graphical) #Physics #Quantum and electron transport phenomena #Quantum mechanics #Spectroscopy and Quantum Chemical Studies #cond-mat.mes-hall

paper · pdf · doi:10.1021/acs.jpclett.5b02331

published in The Journal of Physical Chemistry Letters 6(24), 4898-4903 (American Chemical Society) · 9 pages

arxiv created 2015/09/21 · openalex publication_date 2015/11/21 · arxiv updated 2015/11/30 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/05

Abstract

We discuss nuclear dynamics at molecule-metal interfaces including nonequilibrium molecular junctions. Starting from the many-body states (pseudoparticle) formulation of the molecule-metal system in the molecular vibronic basis, we introduce gradient expansion to reduce the adiabatic nuclear dynamics (that is, nuclear dynamics on a single molecular potential surface) into its semiclassical form while maintaining the effect of the nonadiabatic electronic transitions between different molecular charge states. This yields a set of equations for the nuclear dynamics in the presence of these nonadiabatic transitions, which reproduce the 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.

Citations

• Born Oppenheimer Dynamics Near Metal Surfaces
• Inelastic transport in the Coulomb blockade regime within a nonequilibrium atomic limit
• Colloquium: Phononics: Manipulating heat flow with electronic analogs and beyond
• Tunneling through nanosystems: Combining broadening with many-particle states
• Memory effects in nonequilibrium quantum impurity models
• Kinetic equations for transport through single-molecule transistors
• Theory of strongly correlated electron systems: Hubbard–Anderson models from an exact Hamiltonian, and perturbation theory near the atomic limit within a nonorthogonal basis set
• Current-induced nonequilibrium vibrations in single-molecule devices
• Transport in molecular states language: Generalized quantum master equation approach

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