Naslov
Mixed-quantum-classical or fully-quantized dynamics? A unified code to compare methods

Autori
Coonjobeeharry, J. ; Spinlove, K. E. ; Sanz Sanz, C. ; Sapunar, Marin ; Došlić, Nađa ; Worth, G. A.

Izvornik
Philosophical transactions - Royal Society. Mathematical, Physical and engineering sciences (1364-503X) 380 (2022), 2223; 20200386, 17

Vrsta, podvrsta i kategorija rada
Radovi u časopisima, članak, znanstveni

Ključne riječi
MCTDH ; direct dynamics ; non-adiabatic dynamics ; vMCG ; surface hopping

Sažetak
Three methods for non-adiabatic dynamics are compared to highlight their capabilities. Multi-configurational time-dependent Hartree is a full grid-based solution to the time-dependent Schrödinger equation, variational multi-configurational Gaussian (vMCG) uses a less flexible but unrestricted Gaussian wavepacket basis, and trajectory surface hopping (TSH) replaces the nuclear wavepacket with a swarm of classical trajectories. Calculations with all methods using a model Hamiltonian were performed. The vMCG and TSH were also then run in a direct dynamics mode, with the potential energy surfaces calculated on-the-fly using quantum chemistry calculations. All dynamics calculations used the Q uantics package, with the TSH calculations using a new interface to a surface hopping code. A novel approach to calculate adiabatic populations from grid-based quantum dynamics using a time-dependent discrete variable representation is presented, allowing a proper comparison of methods.

Izvorni jezik
Engleski

Znanstvena područja
Kemija

POVEZANOST RADA