Related papers: Robust non-adiabatic molecular dynamics for metals…
Coupled trajectory mixed quantum classical (CTMQC) dynamics is a rigorous approach to trajectory-based non-adiabatic dynamics, which has recently seen an improvement to energy conservation via the introduction of the CTMQC-E algorithm.…
We develop a novel approach to the coupled motion of electrons and ions that focuses on the dynamics of the electronic subsystem. Usually the description of electron dynamics involves an electronic Schr\"odinger equation where the nuclear…
A new "on the fly" method to perform Born-Oppenheimer ab initio molecular dynamics (AIMD) is presented. Inspired by Ehrenfest dynamics in time-dependent density functional theory, the electronic orbitals are evolved by a Schroedinger-like…
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…
Transitions out of the ground space limit the performance of quantum adiabatic algorithms, while hardware imperfections impose stringent limitations on the circuit depth. We propose an adiabatic echo verification protocol which mitigates…
A mixed quantum-classical approach to simulate the coupled dynamics of electrons and nuclei in nanoscale molecular systems is presented. The method relies on a second order expansion of the Lagrangian in time-dependent density functional…
We present an ab-initio-based effective interaction model (EIM) for the study of magnetism, thermodynamics, and their interplay in body-centered cubic Fe-Co alloys, with Co content from 0 to 70%. The model includes explicitly both spin and…
We introduce a simple ansatz for the wavefunction of a many-body system based on coupled forward and backward-propagating semiclassical trajectories. This method is primarily aimed at, but not limited to, treating nonequilibrium dynamics in…
This paper provides the first ab-initio on-the-fly example of using the Quasi-Diabatic (QD) scheme for non-adiabatic simulations with diabatic dynamics approaches. The QD scheme provides a seamless interface between diabatic quantum…
Non-adiabatic dynamics at molecule-metal interfaces govern diverse and technologically important phenomena, from heterogeneous catalysis to dye-sensitized solar energy conversion and charge transport across molecular junctions. Realistic…
An extension of the CCS-method [Chem. Phys. 2004, 304, p. 103-120] for simulating non-adiabatic dynamics with quantum effects of the nuclei is put forward. The time-dependent Schr\"{o}dinger equation for the motion of the nuclei is solved…
We present a new approach to calculate real-time quantum dynamics in complex systems. The formalism is based on the partitioning of a system's environment into "core" and "reservoir" modes, with the former to be treated quantum mechanically…
Mixed-quantum classical (MQC) methods for simulating the dynamics of molecules at metal surfaces have the potential to accurately and efficiently provide mechanistic insight into reactive processes. Here, we introduce simple two-dimensional…
We study the dynamics of a molecule's nuclear wave-function near an avoided crossing of two electronic energy levels, for one nuclear degree of freedom. We derive the general form of the Schroedinger equation in the n-th superadiabatic…
Nonadiabatic coupling between electrons and molecular motion at metal surfaces leads to energy dissipation and dynamical steering effects during chemical surface dynamics. We present a theoretical approach to the scattering of molecules…
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…
A new scheme is proposed for modeling molecular nonadiabatic dynamics near metal surfaces. The charge-transfer character of such dynamics is exploited to construct an efficient reduced representation for the electronic structure. In this…
The exact factorization approach has led to the development of new mixed quantum-classical methods for simulating coupled electron-ion dynamics. We compare their performance for dynamics when more than two electronic states are occupied at…
We perform nonadiabatic simulations of warm dense aluminum based on the electron-force field (EFF) variant of wave-packet molecular dynamics. Comparison of the static ion-ion structure factor with density functional theory (DFT) is used to…
We study the dynamics of initial nucleation processes of photoinduced structural change of molecular crystals. In order to describe the nonadiabatic transition in each molecule, we employ a model of localized electrons coupled with a fully…