Related papers: Modeling Spin-Dependent Nonadiabatic Dynamics with…
Within the context of very simple avoided crossing, we investigate the investigate the effect of a complex diabatic coupling in determining spin-dependent rate constants and scattering states. We find that, if the molecular geometry is not…
We perform extensive benchmark comparisons of surface hopping dynamics with numerically exact calculations for the spin-boson model over a wide range of energetic and coupling parameters as well as temperature. We find that deviations from…
Nonadiabatic molecular dynamics is a key technique for investigating a broad range of photochemical and photophysical processes. Among the established approaches, surface hopping schemes are widely used and can be easily integrated with…
This research examines the nonadiabatic dynamics of cyclobutanone after excitation into the n-3s Rydberg S2 state. It stems from our contribution to the Special Topic of the Journal of Chemical Physics to test the predictive capability of…
We investigate two well-known approaches for extending the fewest switches surface hopping (FSSH) algorithm to periodic time-dependent couplings. The first formalism acts as if the instantaneous adiabatic electronic states were standard…
Accurate simulation the many-electronic nonadiabatic dynamics process at metal surfaces remains as a significant task. In this work, we present an orbital surface hopping (OSH) algorithm rigorously derived from the orbital quantum classical…
We demonstrate that, for systems with spin-orbit coupling and an odd number of electrons, the standard fewest switches surface hopping (FSSH) algorithm does not conserve the total linear or angular momentum. This lack of conservation arises…
Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…
We study the spin-dependent stereodynamics of the S + H2 -> SH + H reaction using full-dimensional quantum dynamics calculations with zero total nuclear angular momentum along the triplet 3A" states and singlet 1A' states. We find that the…
In the spirit of the fewest switches surface hopping, the frozen Gaussian approximation with surface hopping (FGA-SH) method samples a path integral representation of the non-adiabatic dynamics in the semiclassical regime. An improved…
We explore the effects of spin-orbit coupling on nuclear wave packet motion near an out-of-equilibrium molecular junction, where nonzero Berry curvature emerges as the antisymmetric part of the electronic friction tensor. The existence of…
The importance of triplet states in the photorelaxation dynamics of SO2 is studied by mixed quantum-classical dynamics simulations. Using the Surface Hopping including ARbitrary Couplings (Sharc) method, intersystem crossing processes…
Fewest-switches surface hopping is studied in the context of quantum-classical Liouville dynamics. Both approaches are mixed quantum-classical theories that provide a way to describe and simulate the nonadiabatic quantum dynamics of…
Incorporating nuclear quantum effects into nonadiabatic dynamics remains a significant challenge. Herein we introduce new nonadiabatic dynamics approaches based on the recently developed constrained nuclear-electronic orbital (CNEO) theory.…
It is well known that fewest-switches surface hopping (FSSH) fails to correctly capture the quadratic scaling of rate constants with diabatic coupling in the weak-coupling limit, as expected from Fermi's golden rule and Marcus theory. To…
We present a preliminary extension of the fewest switches surface hopping (FSSH) algorithm to the case of complex Hamiltonians as appropriate for modeling the dynamics of photoexcited molecules in magnetic fields. We make ansatze for the…
Independent electron surface hopping (IESH) is a computational algorithm for simulating the mixed quantum-classical molecular dynamics of adsorbate atoms and molecules interacting with metal surfaces. It is capable of modelling the…
The powerful molecular dynamics (MD) simulation is basically based on a picture that the atoms experience classical-like trajectories under the exertion of classical force field determined by the quantum mechanically solved electronic…
Dissociative chemisorption is a key process in hydrogen-metal surface chemistry, where nonadiabatic effects due to low-lying electron-hole-pair excitations may affect reaction outcomes. Molecular dynamics with electronic friction…
In the paper we derive a semiclassical model for surface hopping allowing quantum dynamical non-adiabatic transition between different potential energy surfaces in which cases the classical Born-Oppenheimer approximation breaks down. The…