Nonequilibrium solvent effects in Born-Oppenheimer molecular dynamics for ground and excited electronic states
- Theoretical Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545 (United States)
The effects of solvent on molecular processes such as excited state relaxation and photochemical reaction often occurs in a nonequilibrium regime. Dynamic processes such as these can be simulated using excited state molecular dynamics. In this work, we describe methods of simulating nonequilibrium solvent effects in excited state molecular dynamics using linear-response time-dependent density functional theory and apparent surface charge methods. These developments include a propagation method for solvent degrees of freedom and analytical energy gradients for the calculation of forces. Molecular dynamics of acetaldehyde in water or acetonitrile are demonstrated where the solute-solvent system is out of equilibrium due to photoexcitation and emission.
- OSTI ID:
- 22660834
- Journal Information:
- Journal of Chemical Physics, Vol. 144, Issue 15; Other Information: (c) 2016 Author(s); Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
Similar Records
Real-Time Time-Dependent Nuclear–Electronic Orbital Approach: Dynamics beyond the Born–Oppenheimer Approximation
Non-adiabatic Excited State Molecule Dynamics Modeling of Photochemistry and Photophysics of Materials