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We present a novel energy-based localization procedure able to localize molecular orbitals into specific spatial regions. The method is applied to several cases including both conjugated and non-conjugated systems. The obtained localized…

Chemical Physics · Physics 2022-09-13 Tommaso Giovannini , Henrik Koch

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…

Strongly Correlated Electrons · Physics 2012-02-14 David D. O'Regan , Nicholas D. M. Hine , Mike C. Payne , Arash A. Mostofi

Density-functional theory (DFT) has revolutionized computer simulations in chemistry and material science. A faithful implementation of the theory requires self-consistent calculations. However, this effort involves repeatedly diagonalizing…

Quantum Physics · Physics 2023-07-17 Taehee Ko , Xiantao Li , Chunhao Wang

Efficient hybrid DFT simulations of solid state materials would be extremely beneficial for computational chemistry and materials science, but is presently bottlenecked by difficulties in computing Hartree-Fock (HF) exchange with plane wave…

Chemical Physics · Physics 2024-10-30 Yuanheng Wang , Diptarka Hait , Pablo A. Unzueta , Juncheng Harry Zhang , Todd J. Martínez

In this study, we propose a quantum-classical hybrid scheme for performing orbital-free density functional theory (OFDFT) using probabilistic imaginary-time evolution (PITE), designed for the era of fault-tolerant quantum computers (FTQC),…

Quantum Physics · Physics 2024-07-24 Yusuke Nishiya , Hirofumi Nishi , Taichi Kosugi , Yu-ichiro Matsushita

A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…

Computational Physics · Physics 2022-11-09 Aleksei V. Ivanov , Gianluca Levi , Elvar Ö. Jónsson , Hannes Jónsson

Recently, an approximate theoretical framework was introduced, called local reduced density matrix functional theory (local-RDMFT), where functionals of the one-body reduced density matrix (1-RDM) are minimized under the additional…

Due to efficient scaling with electron number N, density functional theory (DFT) is widely used for studies of large molecules and solids. Restriction of an exact mean-field theory to local potential functions has recently been questioned.…

Other Condensed Matter · Physics 2015-06-24 Robert K. Nesbet

Given a set of Kohn-Sham orbitals from an insulating system, we present a simple, robust, efficient and highly parallelizable method to construct a set of, optionally orthogonal, localized basis functions for the associated subspace. Our…

Computational Physics · Physics 2014-11-05 Anil Damle , Lin Lin , Lexing Ying

First principles calculations based on density functional theory are having an incerasing impact on our understanding of molecule-surface interactions. For example, calculations of the multi-dimensional potential energy surface have…

Materials Science · Physics 2007-05-23 O. Gulseren , D. M. Bird , S. E. Humphreys

Linear-response time-dependent (TD) density-functional theory (DFT) has been implemented in the pseudopotential wavelet-based electronic structure program BigDFT and results are compared against those obtained with the all-electron…

We introduce a new multilevel domain decomposition method (MDD) for electronic structure calculations within semi-empirical and Density Functional Theory (DFT) frameworks. This method iterates between local fine solvers and global coarse…

Computational Physics · Physics 2007-05-23 M. Barrault , E. Cances , W. W. Hager , C. Le Bris

Nonlocal kinetic energy density functionals (KEDFs) with density-dependent kernels are currently the most accurate functionals available for orbital-free density functional theory (OF-DFT) calculations. However, despite advances in…

Materials Science · Physics 2024-12-05 Yongshuo Chen , Cheng Ma , Boning Cui , Tian Cui , Wenhui Mi , Qiang Xu , Yanchao Wang , Yanming Ma

We present a numerical method for grand canonical density functional theory (DFT) tailored to solid-state systems, employing Gaussian-type orbitals as the primary basis. Our approach directly minimizes the grand canonical free energy using…

Chemical Physics · Physics 2025-10-09 Anton Z. Ni , Adam Rettig , Joonho Lee

Quantum mechanical calculations for material modelling using Kohn-Sham density functional theory (DFT) involve the solution of a nonlinear eigenvalue problem for $N$ smallest eigenvector-eigenvalue pairs with $N$ proportional to the number…

Computational Physics · Physics 2023-09-26 Sameer Khadatkar , Phani Motamarri

The exact formulation of multi-configuration density-functional theory (DFT) is discussed in this work. As an alternative to range-separated methods, where electron correlation effects are split in the coordinate space, the combination of…

Chemical Physics · Physics 2015-02-26 Emmanuel Fromager

Simulations in the warm dense matter regime using finite temperature Kohn-Sham density functional theory (FT-KS-DFT), while frequently used, are computationally expensive due to the partial occupation of a very large number of high-energy…

Materials Science · Physics 2018-04-04 Yael Cytter , Eran Rabani , Daniel Neuhauser , Roi Baer

A new method for calculating optical absorption spectra within linear-scaling density-functional theory (LS-DFT) is presented, incorporating a scheme for optimizing a set of localized orbitals to accurately represent unoccupied Kohn-Sham…

Materials Science · Physics 2015-05-30 Laura E. Ratcliff , Nicholas D. M. Hine , Peter D. Haynes

Density Functional Theory (DFT) is a pivotal method within quantum chemistry and materials science, with its core involving the construction and solution of the Kohn-Sham Hamiltonian. Despite its importance, the application of DFT is…

The description of realistic strongly correlated systems has recently advanced through the combination of density functional theory in the local density approximation (LDA) and dynamical mean field theory (DMFT). This LDA+DMFT method is…

Strongly Correlated Electrons · Physics 2009-11-13 B. Amadon , F. Lechermann , A. Georges , F. Jollet , T. O. Wehling , A. I. Lichtenstein