GPU-accelerated on-the-fly nonadiabatic semiclassical dynamics.

GPU-accelerated on-the-fly nonadiabatic dynamics is enabled by interfacing the linearized semiclassical dynamics approach with the TeraChem electronic structure program. We describe the computational workflow of the "PySCES" code interface, a Python code for semiclassical dynamics with on-the-fly electronic structure, including parallelization over multiple GPU nodes. We showcase the abilities of this code and present timings for two benchmark systems: fulvene solvated in acetonitrile and a charge transfer system in which a photoexcited zinc-phthalocyanine donor transfers charge to a fullerene acceptor through multiple electronic states on an ultrafast timescale.

Superadiabatic Forces via the Acceleration Gradient in Quantum Many-Body Dynamics.

We apply the formally exact quantum power functional framework ( , , 174108) to a one-dimensional Hooke's helium model atom. The physical dynamics are described on the one-body level beyond the density-based adiabatic approximation. We show that gradients of both the microscopic velocity and acceleration field are required to correctly describe the effects due to interparticle interactions.