2024/02/20 by Samuel L. Rudge, Rudge, Samuel L., Christoph Kaspar +9 · 2 citations
Engineering · Physics and Astronomy · #FOS: Physical sciences #Mesoscale and Nanoscale Physics (cond-mat.mes-hall) #Molecular Junctions and Nanostructures #Spectroscopy and Quantum Chemical Studies
paper · pdf · doi:10.48550/arxiv.2402.13161
openalex publication_date 2024/02/20 · openalex created_date 2024/02/23 · openalex updated_date 2026/07/28
A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees of freedom with Langevin dynamics for the classical degrees of freedom, namely, low-frequency vibrational modes within the molecule. The approach extends previous mixed quantum-classical methods based on Langevin equations to models containing strong electron-electron or quantum electronic-vibrational interactions, while maintaining a nonperturbative and non-Markovian treatment of the molecule-metal coupling. To demonstrate the approach, nonequilibrium transport observables are calculated for a molecular nanojunction containing strong interactions.