Related papers: Fully quantum non-adiabatic dynamics in electronic…
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…
Simulation and analysis of multidimensional dynamics of a quantum non-Hmeritian system is a challenging problem. Gaussian wavepacket dynamics has proven to be an intuitive semiclassical approach to approximately solving the dynamics of…
Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as…
We review techniques for simulating fully quantum nonadiabatic dynamics using the frozen-width moving Gaussian basis functions to represent the nuclear wavefunction. A choice of these basis functions is primarily motivated by the idea of…
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 an approach for carrying out non-adiabatic molecular dynamics simulations of systems in which non-adiabatic transitions arise from the coupling between the classical atomic motions and a quasi-continuum of electronic quantum…
Gaussian wave packets (GWPs) are well suited as basis functions to describe the time evolution of arbitrary wave functions in systems with nonsingular smooth potentials. They are less so in atomic systems on account of the singular behavior…
We introduce a class of interatomic potential models that can be automatically generated from data consisting of the energies and forces experienced by atoms, derived from quantum mechanical calculations. The resulting model does not have a…
A non-adiabatic nuclear wavepacket dynamics simulation of the H$_2$O$^+$ de-excitation process is performed based on electronic structure calculations using the variational quantum eigensolver. The adiabatic potential energy surfaces and…
Trajectory-based mixed quantum-classical approaches to coupled electron-nuclear dynamics suffer from well-studied problems such as the lack of (or incorrect account for) decoherence in the trajectory surface hopping method and the inability…
On-the-fly quantum nonadiabatic dynamics for large systems greatly benefits from the adiabatic representation readily available from the electronic structure programs. However, frequently occurring in this representation conical…
We present a method to calculate exact dynamics of a wave-packet in a quantum two-state problem with Dirac delta coupling. The advantage of our method is that the calculations are done in the time domain. Hence inverting the solutions from…
A quantum-mechanical Gaussian wave-packet approach to the theoretical description of nuclear motions in a condensed-phase environment is developed. General expressions for the time-dependent reduced density matrix are given for a harmonic…
We develop a unified quantum geometric framework to understand reactive quantum dynamics. The critical roles of the quantum geometry of adiabatic electronic states in both adiabatic and non-adiabatic quantum dynamics are unveiled. A…
The combined quantum electron-nuclear dynamics is often associated with the Born-Huang expansion of the molecular wave function and the appearance of nonadiabatic effects as a perturbation. On the other hand, native multicomponent…
The theoretical investigation of non-adiabatic processes is hampered by the complexity of the coupled electron-nuclear dynamics beyond the Born-Oppenheimer approximation. Classically, the simulation of such reactions is limited by the…
We analyse a nonadiabatic self-consistent field method by means of an exactly-solvable model. The method is based on nuclear and electronic orbitals that are functions of the cartesian coordinates in the laboratory-fixed frame. The kinetic…
We describe a path-integral approach for including nuclear quantum effects in non-adiabatic chemical dynamics simulations. For a general physical system with multiple electronic energy levels, a corresponding isomorphic Hamiltonian is…
An approach to non-adiabatic dynamics of atoms in molecular and condensed matter systems under general non-equilibrium conditions is proposed. In this method interaction between nuclei and electrons is considered explicitly up to the second…
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…