Related papers: Extended Lagrangian Born-Oppenheimer Molecular Dyn…
Efficient molecular dynamics (MD) simulation is vital for understanding atomic-scale processes in materials science and biophysics. Traditional density functional theory (DFT) methods are computationally expensive, which limits the…
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 self-consistent calculation scheme for correlated electron systems is created based on the density-functional theory (DFT). Our scheme is a multi-reference DFT (MR-DFT) calculation in which the electron charge density is reproduced by an…
This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…
This article proposes a so-called Quasi Time-Reversible (QTR G-Ext) scheme based on Grassmann extrapolation of density matrices for an accurate calculation of initial guesses in Born-Oppenheimer Molecular Dynamics simulations. The method…
We implemented various DFT+U schemes, including the ACBN0 self-consistent density-functional version of the DFT+U method [Phys. Rev. X 5, 011006 (2015)] within the massively parallel real-space time-dependent density functional theory…
We describe a massively parallel implementation of the recently developed discontinuous Galerkin density functional theory (DGDFT) [J. Comput. Phys. 2012, 231, 2140] method, for efficient large-scale Kohn-Sham DFT based electronic structure…
Wavefunction extrapolation greatly reduces the number of self-consistent field (SCF) iterations and thus the overall computational cost of Born-Oppenheimer molecular dynamics (BOMD) that is based on the Kohn-Sham density functional theory.…
The Ziegler-Rauk-Baerends multiplet sum method (MSM) assumes that density-functional theory (DFT) provides a good description of states dominated by a single determinant. It then uses symmetry to add static correlation to DFT. In our…
We present an orbital-resolved extension of the Hubbard $U$ correction to density-functional theory (DFT). Compared to the conventional shell-averaged approach, the prediction of energetic, electronic and structural properties is strongly…
We present an approach to the DFT+U method (Density Functional Theory + Hubbard model) within which the computational effort for calculation of ground state energies and forces scales linearly with system size. We employ a formulation of…
Extended free energy Lagrangians are proposed for first principles molecular dynamics simulations at finite electronic temperatures for plane-wave pseudopotential and local orbital density matrix based calculations. Thanks to the extended…
We introduce a method to carry out zero-temperature calculations within density functional theory (DFT) but without relying on the Born-Oppenheimer (BO) approximation for the ionic motion. Our approach is based on the finite-temperature…
An atomic-orbital basis set framework is presented for carrying out velocity- gauge real-time time-dependent density functional theory (TDDFT) simulations in periodic systems employing range-separated hybrid functionals. Linear optical…
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…
Fromager and Lasorne [Electron. Struct. 6 025002 (2024)] have recently derived an in-principle exact Kohn-Sham density functional theory (KS-DFT) of electrons and nuclei, where the nuclear density and the (so-called conditional) electronic…
In this article we introduce a generalization of the popular DFT+U method based on the extended Hubbard model that includes on-site and inter-site electronic interactions. The novel corrective Hamiltonian is designed to study systems for…
Time-dependent density-functional theory (TDDFT) is a central tool for studying the dynamical electronic structure of molecules and solids, yet aspects of its mathematical foundations remain insufficiently understood. In this work, we…
The Born--Oppenheimer approximation is the standard tool for the study of molecular systems. It is founded on the observation that the energy scale of the electron dynamics in a molecule is larger than that of the nuclei. A very similar…
Ideal density-functional approximations (DFAs) should account for dynamic, static, and nondynamic correlation. While common DFAs struggle with the latter two, the Ziegler-Rauk-Baerends-Daul multiplet sum method (MSM) provides a pragmatic…