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The density functional theory (DFT) in electronic structure calculations can be formulated as either a nonlinear eigenvalue or direct minimization problem. The most widely used approach for solving the former is the so-called…

Computational Physics · Physics 2013-08-14 Xin Zhang , Jinwei Zhu , Zaiwen Wen , Aihui Zhou

This article is concerned with the numerical solution of subspace optimization problems, consisting of minimizing a smooth functional over the set of orthogonal projectors of fixed rank. Such problems are encountered in particular in…

Numerical Analysis · Mathematics 2022-10-17 Eric Cancès , Gaspard Kemlin , Antoine Levitt

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

We describe a version of an algorithm for evolving self-gravitating collections of particles that should be nearly ideal for parallel architectures. Our method is derived from the ``self-consistent field'' (SCF) approach suggested…

Astrophysics · Physics 2016-08-30 Lars Hernquist , Steinn Sigurdsson , Greg L. Bryan

The implementation of an efficient self-consistent field (SCF) method including both scalar relativistic effects and spin-orbit interaction in density functional theory (DFT) is presented. We make use of Gaussian-type orbitals (GTOs) and…

Chemical Physics · Physics 2024-05-03 Yannick J. Franzke , Werner M. Schosser , Fabian Pauly

Kohn-Sham Density Functional Theory (KS-DFT) has been traditionally solved by the Self-Consistent Field (SCF) method. Behind the SCF loop is the physics intuition of solving a system of non-interactive single-electron wave functions under…

Solving the Kohn-Sham eigenvalue problem constitutes the most computationally expensive part in self-consistent density functional theory (DFT) calculations. In a previous paper, we have proposed a nonlinear Chebyshev-filtered subspace…

Materials Science · Physics 2009-11-13 Yunkai Zhou , Yousef Saad , Murilo L. Tiago , James R. Chelikowsky

Self-consistent field theory (SCFT) is one of the most widely-used framework in studying the equilibrium phase behaviors of inhomogenous polymers. For liquid crystalline polymeric systems, the main numerical challenges of solving SCFT…

Numerical Analysis · Mathematics 2024-09-16 Zhijuan He , Kai Jiang , Liwei Tan , Xin Wang

We propose an efficient algorithm for the recently published electron/hole-transfer Dynamical-weighted State-averaged Constrained CASSCF (eDSC/hDSC) method studying charge transfer states and D$_1$-D$_0$ crossings for systems with odd…

Computational Physics · Physics 2024-09-24 Tian Qiu , Joseph E. Subotnik

The convergence property of a stochastic algorithm for the self-consistent field (SCF) calculations of electron structures is studied. The algorithm is formulated by rewriting the electron charges as a trace/diagonal of a matrix function,…

Numerical Analysis · Mathematics 2023-04-20 Taehee Ko , Xiantao Li

We present an algorithm and its parallel implementation for solving a self consistent problem as encountered in Hartree Fock or Density Functional Theory. The algorithm takes advantage of the sparsity of matrices through the use of local…

Chemical Physics · Physics 2016-07-25 Anthony Scemama , Nicolas Renon , Mathias Rapacioli

We propose a novel adaptive damping algorithm for the self-consistent field (SCF) iterations of Kohn-Sham density-functional theory, using a backtracking line search to automatically adjust the damping in each SCF step. This line search is…

Materials Science · Physics 2022-03-14 Michael F. Herbst , Antoine Levitt

A new iterative solver is proposed to efficiently calculate the ground state electronic structure in Density Functional Theory calculations. This algorithm is particularly useful for simulating physical systems considered difficult to…

Computational Physics · Physics 2021-11-24 Jean-Luc Fattebert

The central importance of large scale eigenvalue problems in scientific computation necessitates the development of massively parallel algorithms for their solution. Recent advances in dense numerical linear algebra have enabled the routine…

Numerical Analysis · Mathematics 2020-05-08 David B. Williams-Young , Paul G. Beckman , Chao Yang

Linear scaling density functional theory approaches to electronic structure are often based on the tendency of electrons to localize even in large atomic and molecular systems. However, in many cases of actual interest, for example in…

Chemical Physics · Physics 2022-03-25 Marcel David Fabian , Ben Shpiro , Roi Baer

We present an efficient computational approach to perform real-space electronic structure calculations using an adaptive higher-order finite-element discretization of Kohn-Sham density-functional theory (DFT). To this end, we develop an…

Computational Physics · Physics 2015-06-05 Phani Motamarri , Michael R Nowak , Kenneth Leiter , Jaroslaw Knap , Vikram Gavini

Large-scale applications of energy density functional (EDF) methods depend on fast and reliable algorithms to solve the associated non-linear self-consistency problem. When dealing with large single-particle variational spaces, existing…

Nuclear Theory · Physics 2019-06-24 W. Ryssens , M. Bender , P. -H. Heenen

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…

A novel parallel hybrid quantum-classical algorithm for the solution of the quantum-chemical ground-state energy problem on gate-based quantum computers is presented. This approach is based on the reduced density-matrix functional theory…

We investigate the feasibility of early fault-tolerant quantum algorithms focusing on ground-state energy estimation problems. In particular, we examine the computation of the cumulative distribution function (CDF) of the spectral measure…

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