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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

We investigate fully self-consistent multiscale quantum-classical algorithms on current generation superconducting quantum computers, in a unified approach to tackle the correlated electronic structure of large systems in both quantum…

A recently developed density functional method, within Hohenberg-Kohn-Sham framework, is used for faithful description of atoms, molecules in Cartesian coordinate grid, by using an LCAO-MO ansatz. Classical Coulomb potential is obtained by…

Chemical Physics · Physics 2013-07-16 Amlan K. Roy

We develop a stochastic formulation of the optimally-tuned range-separated hybrid density functional theory which enables significant reduction of the computational effort and scaling of the non-local exchange operator at the price of…

Chemical Physics · Physics 2016-09-28 Daniel Neuhauser , Eran Rabani , Yael Cytter , Roi Baer

We present an O(N) algorithm to study the vibrational properties of amorphous silicon within the framework of tight-binding approach. The dynamical matrix elements have been evaluated numerically in the harmonic approximation exploiting the…

Disordered Systems and Neural Networks · Physics 2009-11-07 Parthapratim Biswas

With the widespread use of self-consistent field methods, including Hartree-Fock and Density Functional Theory, the implications of accelerating these methods are immense. To this end, we develop a tensor hypercontraction construction with…

Chemical Physics · Physics 2025-08-27 Andreas Erbs Hillers-Bendtsen , Todd J. Martínez

We explore and compare three approximate schemes allowing simple implementation of complex density functionals by making use of selfconsistent implementation of simpler functionals: (i) post-LDA evaluation of complex functionals at the LDA…

Given the widespread use of density functional theory (DFT), there is an increasing need for the ability to model large systems (beyond 1,000 atoms). We present a brief overview of the large-scale DFT code Conquest, which is capable of…

An algorithm for first-principles electronic structure calculations having a computational cost which scales linearly with the system size is presented. Our method exploits the real-space localization of the density matrix, and in this…

mtrl-th · Physics 2016-09-07 E. Hernandez , M. J. Gillan

We report an efficient algorithm using density fitting for the relativistic complete active space self-consistent field (CASSCF) method, which is significantly more stable than the algorithm previously reported by one of the authors [J. E.…

Chemical Physics · Physics 2018-08-01 Ryan D. Reynolds , Takeshi Yanai , Toru Shiozaki

We present a novel route to constructing cost-efficient semi-empirical approximations for the non-additive kinetic energy in subsystem density functional theory. The developed methodology is based on the use of Slater determinants composed…

Chemical Physics · Physics 2025-01-13 Larissa Sophie Eitelhuber , Denis G. Artiukhin

Noncollinear (NC) magnetism and spin-orbit coupling (SOC) are indispensable for predictive ab initio materials simulations with pronounced relativistic effects and magnetic frustration, yet they significantly increase the cost of…

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

Hybrid density functional calculation is indispensable to accurate description of electronic structure, whereas the formidable computational cost restricts its broad application. Here we develop a deep equivariant neural network method…

Materials Science · Physics 2023-02-17 Zechen Tang , He Li , Peize Lin , Xiaoxun Gong , Gan Jin , Lixin He , Hong Jiang , Xinguo Ren , Wenhui Duan , Yong Xu

Kohn-Sham spin-density functional theory provides an efficient and accurate model to study electron-electron interaction effects in quantum dots, but its application to large systems is a challenge. An efficient algorithm for the…

Mesoscale and Nanoscale Physics · Physics 2007-05-23 Hong Jiang , Harold U. Baranger , Weitao Yang

A method to calculate the hole spectral function in the discrete part of the spectrum is suggested within the natural orbital representation of the one-body density matrix of $A$-nucleon system using its relationship with the overlap…

Nuclear Theory · Physics 2009-10-28 A. N. Antonov , M. V. Stoitsov , M. K. Gaidarov , S. S. Dimitrova , P. E. Hodgson

A new order-N method for calculating the electronic structure of general (non-tight-binding) potentials is presented. The method uses a combination of the ``purification''-based approaches used by Li, Nunes and Vanderbilt, and Daw, and a…

mtrl-th · Physics 2016-09-07 A. E. Carlsson

The general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…

Chemical Physics · Physics 2017-03-16 Alain C. Vaucher , Markus Reiher

We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…

Chemical Physics · Physics 2016-12-04 Ralph Gebauer , Morrel H. Cohen , Roberto Car

Classical density functional theory (DFT) of fluids is a valuable tool to analyze inhomogeneous fluids. However, few numerical solution algorithms for three-dimensional systems exist. Here we present an efficient numerical scheme for fluids…