Related papers: Improved sampling and validation of frozen Gaussia…
While surface-hopping has emerged as a powerful method to simulate non-adiabatic dynamics in large molecules, the ad hoc nature of the necessary velocity adjustments and decoherence corrections in the algorithm somewhat reduces its…
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…
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…
Rare nonadiabatic reactions are a key component of many important molecular processes but are challenging to capture with direct dynamical simulations. In this paper, we combine our recently developed mapping approach to surface hopping…
Non-adiabatic chemical reactions involving continuous circularly polarized light (cw CPL) have not attracted as much attention as dynamics in unpolarized/linearly polarized light. However, including circularly (in contrast to linearly)…
In this paper, we develop a Monte Carlo algorithm named the Frozen Gaussian Sampling (FGS) to solve the semiclassical Schr\"odinger equation based on the frozen Gaussian approximation. Due to the highly oscillatory structure of the wave…
A class of surface hopping algorithms is studied comparing two recent Landau-Zener (LZ) formulas for the probability of nonadiabatic transitions. One of the formulas requires a diabatic representation of the potential matrix while the other…
A new methodology of simulating nonadiabatic dynamics using frozen-width Gaussian wavepackets within the moving crude adiabatic representation with the on-the-fly evaluation of electronic structure is presented. The main feature of the new…
The quantum-classical Liouville equation offers a rigorous approach to nonadiabatic quantum dynamics based on surface hopping type trajectories. However, in practice the applicability of this approach has been limited to short times owing…
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…
Nuclear Berry curvature effects emerge from electronic spin degeneracy and canlead to non-trivial spin-dependent (nonadiabatic) nuclear dynamics. However, such effects are completely neglected in all current mixed quantum-classical methods…
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…
We develop a gauge-invariant frozen Gaussian approximation (GIFGA) method for the linear Schr\"odinger equation (LSE) with periodic potentials in the semiclassical regime. The method generalizes the Herman-Kluk propagator for LSE to the…
Simulating Markovian open quantum systems in the semiclassical regime poses a grand challenge for computational physics, as the highly oscillatory nature of the dynamics imposes prohibitive resolution requirements on traditional grid-based…
Two-frequency (two-color) laser fields provide a powerful and flexible means for steering molecular dynamics. However, quantitatively reliable and scalable theoretical tools for simulating laser-driven nonadiabatic processes under such…
We propose a surface hopping Gaussian beam method to numerically solve a class of high frequency linear transport systems in high spatial dimensions, based on asymptotic analysis. The stochastic surface hopping is combined with Gaussian…
We develop a refined Frozen Gaussian approximation (FGA) for the fractional Schr\"odinger equation in the semi-classical regime, where the solution exhibits rapid oscillations as the scaled Planck constant $\varepsilon$ becomes small. Our…
We investigate a simple and robust scheme for choosing the phases of adiabatic electronic states smoothly (as a function of geometry) so as to maximize the performance of ab initio non-adiabatic dynamics methods. Our approach is based upon…
Quantum molecular dynamics requires an accurate representation of the molecular potential energy surface from a minimal number of electronic structure calculations, particularly for nonadiabatic dynamics where excited states are required.…
We present a detailed study of the decoherence correction to surface-hopping that was recently derived from the exact factorization approach. Ab initio multiple spawning calculations that use the same initial conditions and same electronic…