Related papers: Density-matrix based Extended Lagrangian Born-Oppe…
A new electronic structure model is developed in which the ground state energy of a molecular system is given by a Hartree-Fock-like expression with parametrized one- and two-electron integrals over an extended (minimal + polarization) set…
Recently, a microscopically motivated nuclear energy density functional was derived by applying the density matrix expansion to the Hartree-Fock (HF) energy obtained from long-range chiral effective field theory two- and three-nucleon…
A real-space formalism for density-functional perturbation theory (DFPT) is derived and applied for the computation of harmonic vibrational properties in molecules and solids. The practical implementation using numeric atom-centered…
Computational studies of electrochemical interfaces based on density-functional theory (DFT) play an increasingly important role in present research on electrochemical processes for energy conversion and storage. The homogeneous background…
The assumptions underpinning the adiabatic Born-Oppenheimer (BO) approximation are broken for molecules interacting with attosecond laser pulses, which generate complicated coupled electronic-nuclear wavepackets that generally will have…
We have developed and implemented a new quantum molecular dynamics approximation that allows fast and accurate simulations of dense plasmas from cold to hot conditions. The method is based on a carefully designed orbital-free implementation…
A Gaussian operator representation for the many body density matrix of fermionic systems, developed by Corney and Drummond [Phys. Rev. Lett, v93, 260401 (2004)], is used to derive approximate decoupling schemes for their dynamics. In this…
Modeling many-body quantum systems with strong interactions is one of the core challenges of modern physics. A range of methods has been developed to approach this task, each with its own idiosyncrasies, approximations, and realm of…
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…
Laser-induced molecular alignment is well understood within the framework of the Born-Oppenheimer (BO) approximation Without the BO approximation, however, the concept of molecular structure is lost, making alignment hard to define…
In this article, we consider the extended Kohn-Sham model for atoms subjected to cylindrically-symmetric external potentials. The variational approximation of the model and the construction of appropriate discretization spaces are detailed…
In traditional finite-temperature Kohn-Sham density functional theory (KSDFT), the well-known orbitals wall restricts the use of first-principles molecular dynamics methods at extremely high temperatures. However, stochastic density…
Orbital-free density functional theory (OF-DFT) provides an alternative approach for calculating the molecular electronic energy, relying solely on the electron density. In OF-DFT, both the ground-state density is optimized variationally to…
Dynamical electronic- and vibrational-structure theories have received a growing interest in the last years due to their ability to simulate spectra recorded with ultrafast experimental techniques. The exact time evolution of a molecular…
This article describes a method for calculating higher order or nonadiabatic corrections in Born-Oppenheimer theory and its interaction with the translational degrees of freedom. The method uses the Wigner-Weyl correspondence to map nuclear…
The recent progress of linear-scaling or O(N) methods in the density functional theory (DFT) is remarkable. We expect that first-principles molecular dynamics (FPMD) simulations based on DFT can now treat more realistic and complex systems…
Extended Lagrangian molecular dynamics (XLMD) is a general method for performing molecular dynamics simulations using quantum and classical many-body potentials. Recently several new XLMD schemes have been proposed and tested on several…
Methods based on propagation of the one-body reduced density-matrix hold much promise for the simulation of correlated many-electron dynamics far from equilibrium, but difficulties with finding good approximations for the interaction term…
We present a universal expression for the electronic friction as felt by a set of classical nuclear degrees of freedom (DoF's) coupled to a manifold of quantum electronic DoF's; no assumptions are made regarding the nature of the electronic…
We present a substantial extension of our constraint-based approach for development of orbital-free (OF) kinetic-energy (KE) density functionals intended for the calculation of quantum-mechanical forces in multi-scale molecular dynamics…