Related papers: Ehrenfest dynamics with localized atomic-orbital b…
We have derived equations for nonadiabatic Ehrenfest molecular dynamics which conserve the total energy in the case of time-dependent discretization for electrons. A discretization is time-dependent in all cases where it or part of it…
We present in detail the recently derived ab-initio molecular dynamics (AIMD) formalism [Phys. Rev. Lett. 101 096403 (2008)], which due to its numerical properties, is ideal for simulating the dynamics of systems containing thousands of…
Ehrenfest Dynamics combined with real-time time-dependent density functional theory has proven to be a reliable tool to study non-adiabatic molecular dynamics with a reasonable computational cost. Among other possibilities, it allows for…
Mixed quantum-classical mechanics descriptions are critical to modeling coupled electron-nuclear dynamics, i.e. non-adiabatic molecular dynamics, relevant to photochemical and photophysical processes. We argue that, for polyatomic…
We present a Lagrangian-based implementation of Ehrenfest dynamics with nuclear-electronic orbital (NEO) theory and real-time time-dependent density functional theory (RT-TDDFT) for extended periodic systems. In addition to a quantum…
Mixed quantum-classical methods, such as surface hopping and Ehrenfest dynamics, have proven useful for describing molecular processes involving multiple electronic states. These methods require propagating many independent trajectories,…
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 present an implementation of localized atomic orbital basis sets in the projector augmented wave (PAW) formalism within the density functional theory (DFT). The implementation in the real-space GPAW code provides a complementary basis…
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…
Due to a continuum of electronic states present in periodic systems, the description of molecular dynamics on surfaces poses a serious computational challenge. One of the most used families of approaches in these settings are friction…
We benchmark a set of quantum-chemistry methods, including multitrajectory Ehrenfest, fewest-switches surface-hopping, and multiconfigurational-Ehrenfest dynamics, against exact quantum-many-body techniques by studying real-time dynamics in…
Electronic circular dichroism (ECD) is a powerful spectroscopical method for investigating chiral properties at the molecular level. ECD calculations with the commonly used linear-response time-dependent density functional theory (LR-TDDFT)…
The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between…
We propose Ehrenfest Dynamics with Spontaneous Localization (SLED), a decoherence-corrected extension of Ehrenfest dynamics based on the Gisin-Percival quantum-state diffusion (QSD) equation. In SLED, the electronic wavefunction evolves…
The interaction of laser fields with solid-state systems can be modeled efficiently within the velocity-gauge formalism of real-time time dependent density functional theory (RT-TDDFT). In this article, we discuss the implementation of the…
Simulating electron-ion dynamics using time-dependent density functional theory within an Ehrenfest dynamics scheme can be done in two ways that are in principle exact and identical: propagating time-dependent electronic Kohn-Sham equations…
The optical response of an electronic two-level system (TLS) coupled to an incident continuous wave (cw) electromagnetic (EM) field is simulated explicitly in one dimension by the following five approaches: (i) the coupled Maxwell-Bloch…
Ehrenfest dynamics is a useful approximation for ab initio mixed quantum-classical molecular dynamics that can treat electronically nonadiabatic effects. Although a severe approximation to the exact solution of the molecular time-dependent…
Application of the time-dependent variational principle to a linear combination of frozen-width Gaussians describing the nuclear wavefunction provides a formalism where the total energy is conserved. The computational downside of this…
In this work, we present a computationally efficient methodology that utilizes a local real-space formulation of the projector augmented wave (PAW) method discretized with a finite-element (FE) basis to enable accurate and large-scale…