Related papers: Real-time non-adiabatic dynamics in the one-dimens…
Due to the exponential growth of the state space of coupled quantum systems it is not possible, in general, to numerically store the state of a very large number of quantum systems within a classical computer. We demonstrate a method for…
The exact nuclear time-dependent potential energy surface arises from the exact decomposition of electronic and nuclear motion, recently presented in [A. Abedi, N. T. Maitra, and E. K. U. Gross, Phys. Rev. Lett. 105, 123002 (2010)]. Such…
Ehrenfest, Born-Oppenheimer, Langevin and Smoluchowski dynamics are shown to be accurate approximations of time-independent Schr\"odinger observables for a molecular system avoiding caustics, in the limit of large ratio of nuclei and…
We investigate detailed balance for a quantum system interacting with thermal radiation within mixed quantum-classical theory. For a two-level system coupled to classical radiation fields, three semiclassical methods are benchmarked: (1)…
The two-dimensional electron-nuclear Schr\"odinger equation using soft-core Coulomb potentials has been a cornerstone for modeling and predicting the behavior of one-active-electron diatomic molecules, particularly for processes where both…
The increasing need to simulate the dynamics of photoexcited molecular and nanosystems in the sub-picosecond regime demands new efficient tools able to describe the quantum nature of matter at a low computational cost. By combining the…
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…
Two-dimensional electronic spectroscopy (2DES) provides a detailed picture of electronically nonadiabatic dynamics that can be interpreted with the aid of simulations. Here, we develop and contrast trajectory-based nonadiabatic dynamics…
We investigate the nonequilibrium dynamics induced by an interaction quench in the semiclassical Holstein model within the Ehrenfest nonadiabatic framework, which describes an isolated hybrid quantum-classical system with strictly conserved…
A general theoretical framework is derived for the recently developed multi-state trajectory (MST) approach from the time dependent Schr\"odinger equation, resulting in equations of motion for coupled nuclear-electronic dynamics equivalent…
One key challenge in the study of nonadiabatic dynamics in open quantum systems is to balance computational efficiency and accuracy. Although Ehrenfest dynamics (ED) is computationally efficient and well-suited for large complex systems, ED…
We analyze ultrafast tunneling experiments in which electron transport through a localized orbital is induced by a single cycle THz pulse. We include both electron-electron and electron-phonon interactions on the localized orbital using the…
Within the nuclear-electronic orbital (NEO) framework, the real-time NEO time-dependent density functional theory (RT-NEO-TDDFT) approach enables the simulation of coupled electronic-nuclear dynamics. In this approach, the electrons and…
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…
Computational chemistry at the atomic level has largely branched into two major fields, one based on quantum mechanics and the other on molecular mechanics using classical force fields. Because of high computational costs, quantum…
We present a comprehensive computational framework for simulating nonadiabatic molecular dynamics with explicit inclusion of geometric phase (GP) effects. Our approach is based on a generalized two-level Hamiltonian model that can represent…
Electronic and/or vibronic coherence has been found by recent ultrafast spectroscopy experiments in many chemical, biological and material systems. This indicates that there are strong and complicated interactions between electronic states…
We develop a density matrix formalism to describe coupled electron-nuclear dynamics. To this end we introduce an effective Hamiltonian formalism that describes electronic transitions and small (quantum) nuclear fluctuations along a…
The nonequilibrium dynamics of a quantum dot with electron-phonon interactions described by a generalized Holstein model is presented. A combination of methodologies including the reduced density matrix formalism, the multilayer…
In this paper we propose an ab initio method to solve quantum many-body problems of molecular dynamics where both the electronic and the nuclear degrees are represented by ensembles of trajectories and guiding waves in physical space. Both…