Related papers: A mapping approach to surface hopping
We present a highly efficient method to directly simulate the photodissociation followed by Coulomb explosion of methyl iodide. In order to achieve statistical reliability, more than 40,000 trajectories are calculated on accurate potential…
Gradient descent is a fundamental algorithm in both theory and practice for continuous optimization. Identifying its quantum counterpart would be appealing to both theoretical and practical quantum applications. A conventional approach to…
Trajectory-based methods that propagate classical nuclei on multiple quantum electronic states are often used to simulate nonadiabatic processes in the condensed phase. A long-standing problem of these methods is their lack of detailed…
Adequate simulation of non-adiabatic dynamics through conical intersection requires account for a non-trivial geometric phase (GP) emerging in electronic and nuclear wave-functions in the adiabatic representation. Popular mixed…
Excited-state nonadiabatic simulations with quantum mechanics/molecular mechanics (QM/MM) are essential to understand photoinduced processes in explicit environments. However, the high computational cost of the underlying quantum chemical…
We present a novel shape-approximating anisotropic re-meshing algorithm as a geometric generalization of the adaptive moving mesh method. Conventional moving mesh methods reduce the interpolation error of a mesh that discretizes a given…
We investigate the well-known Shin-Metiu model for an electronic crossing, using both a standard Born-Huang (BH) framework and a novel phase space (PS) electronic Hamiltonian framework. We show that as long as we are not in the strongly…
We propose to measure nonadiabaticity of molecular quantum dynamics rigorously with the quantum fidelity between the Born-Oppenheimer and fully nonadiabatic dynamics. It is shown that this measure of nonadiabaticity applies in situations…
Adiabatic Quantum Computing relies on the quantum adiabatic theorem, which states that a quantum system evolves along its ground state with time if the governing Hamiltonian varies infinitely slowly. However, practical limitations force…
Quantum computing offers promising new avenues for tackling the long-standing challenge of simulating the quantum dynamics of complex chemical systems, particularly open quantum systems coupled to external baths. However, simulating such…
The hierarchical equations of motion technique has found widespread success as a tool to generate the numerically exact dynamics of non-Markovian open quantum systems. However, its application to low temperature environments remains a…
Nonadiabatic molecular dynamics simulations aim to describe the coupled electron-nuclear dynamics of molecules in excited electronic states. These simulations have been applied to understand a plethora of photochemical and photophysical…
The athermal quasistatic deformation method provides an elegant solution to overcome the limitation of short time spans in molecular simulations. It provides overdamped conditions, allowing for the extraction of purely structural responses…
Quantum pumping, in its different forms, is attracting attention from different fields, from fundamental quantum mechanics, to nanotechnology, to superconductivity. We investigate the crossover of quantum pumping from the adiabatic to the…
We develop a non-empirical scheme to search for the minimum-energy escape paths from the minima of the potential surface to unknown saddle points nearby. A stochastic algorithm is constructed to move the walkers up the surface through the…
Due to particle conservation, Canonical Molecular Dynamics (MD) simulations fail in the description of surface phase transitions involving coverage or lateral density changes. However, a step on the surface can act effectively as a source…
Nonadiabatic molecular dynamics is an effective method for modeling nonradiative decay in electronically excited molecules. Its accuracy depends strongly on the quality of the potential energy surfaces, and its affordability for long…
In this article we show how Ehrenfest mean field theory can be made both a more accurate and efficient method to treat nonadiabatic quantum dynamics by combining it with the generalized quantum master equation framework. The resulting mean…
Direct dynamics methods using Gaussian wavepackets have to rely only on local properties, such as gradients and hessians at the center of the wavepacket, so as to be compatible with the usual quantum chemistry methods. Matrix elements of…
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…