A broadened classical master equation approach for nonadiabatic dynamics at metal surfaces: Beyond the weak molecule-metal coupling limit
Abstract
A broadened classical master equation (BCME) is proposed for modeling nonadiabatic dynamics for molecules near metal surfaces over a wide range of parameter values and with arbitrary initial conditions. Compared with a standard classical master equation–which is valid in the limit of weak molecule-metal couplings–this BCME should be valid for both weak and strong molecule-metal couplings. (The BCME can be mapped to a Fokker-Planck equation that captures level broadening correctly.) Finally, our BCME can be solved with a simple surface hopping algorithm; numerical tests of equilibrium and dynamical observables look very promising.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Jan 13, 2016
- Source ID
- 10.1063/1.4939734
Entities
People
- Joseph E Subotnik
- Wenjie Dou
Organizations
- Air Force Office of Scientific Research
- University of Pennsylvania