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DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

Chemical Physics · Physics 2022-03-15 Eunji Sim , Suhwan Song , Stefan Vuckovic , Kieron Burke

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

Kohn-Sham density functional theory (DFT) has long struggled with the accurate description of strongly correlated and open shell systems and improvements have been minor even in the newest hybrid functionals. In this Letter we treat the…

Chemical Physics · Physics 2021-04-01 Danny Gibney , Jan-Niklas Boyn , David A. Mazziotti

Two of the most widely used electronic structure theory methods, namely Hartree-Fock and Kohn-Sham density functional theory, both requires the iterative solution of a set of Schr\"odinger-like equations. The speed of convergence of such…

Chemical Physics · Physics 2024-06-06 S. Hazra , U. Patil , S. Sanvito

In many Direct and Inverse Scattering problems one has to use a parameter-fitting procedure, because analytical inversion procedures are often not available. In this paper a variety of such methods is presented with a discussion of…

Numerical Analysis · Mathematics 2007-05-23 Alexander G. Ramm , Semion Gutman

We re-adapt a spectral renormalization method, introduced in nonlinear optics, to solve the Kohn-Sham (KS) equations of density functional theory (DFT), with a focus on functionals based on the strictly-correlated electrons (SCE) regime,…

Strongly Correlated Electrons · Physics 2020-04-23 Juri Grossi , Ziad H. Musslimani , Michael Seidl , Paola Gori-Giorgi

We present two stochastic descent algorithms that apply to unconstrained optimization and are particularly efficient when the objective function is slow to evaluate and gradients are not easily obtained, as in some PDE-constrained…

Optimization and Control · Mathematics 2019-04-30 David Kozak , Stephen Becker , Alireza Doostan , Luis Tenorio

We review the role of self-consistency in density functional theory. We apply a recent analysis to both Kohn-Sham and orbital-free DFT, as well as to Partition-DFT, which generalizes all aspects of standard DFT. In each case, the analysis…

Chemical Physics · Physics 2016-11-22 Adam Wasserman , Jonathan Nafziger , Kaili Jiang , Min-Cheol Kim , Eunji Sim , Kieron Burke

The Hartree-Fock equation is a fundamental equation in many-electron problems. It is of practical importance in quantum chemistry to find solutions to the Hartree-Fock equation. The self-consistent field (SCF) method is a standard numerical…

Analysis of PDEs · Mathematics 2023-11-17 Sohei Ashida

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

We have developed a couple of optimal damping algorithms (ODAs) for unrestricted Hartree-Fock (UHF) calculations of open-shell molecular systems. A series of equations were derived for both concurrent and alternate constructions of alpha-…

Chemical Physics · Physics 2018-01-25 Jun-ichi Yamamoto , Yuji Mochizuki

Submodular function minimization is a fundamental optimization problem that arises in several applications in machine learning and computer vision. The problem is known to be solvable in polynomial time, but general purpose algorithms have…

Machine Learning · Computer Science 2015-02-10 Alina Ene , Huy L. Nguyen

In this paper, we analyze the optimization landscape of gradient descent methods for static output feedback (SOF) control of discrete-time linear time-invariant systems with quadratic cost. The SOF setting can be quite common, for example,…

Optimization and Control · Mathematics 2023-10-31 Jingliang Duan , Jie Li , Shengbo Eben Li , Lin Zhao

Standard density functional approximations often give questionable results for odd-electron radical complexes, with the error typically attributed to self-interaction. In density corrected density functional theory (DC-DFT), certain classes…

Chemical Physics · Physics 2015-06-19 Min-Cheol Kim , Eunji Sim , Kieron Burke

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

In this work, we consider convex optimization problems with smooth objective function and nonsmooth functional constraints. We propose a new stochastic gradient algorithm, called Stochastic Halfspace Approximation Method (SHAM), to solve…

Optimization and Control · Mathematics 2024-12-04 Nitesh Kumar Singh , Ion Necoara

We propose an efficient algorithm for solving orthogonal canonical correlation analysis (OCCA) in the form of trace-fractional structure and orthogonal linear projections. Even though orthogonality has been widely used and proved to be a…

Machine Learning · Computer Science 2019-09-26 Leihong Zhang , Li Wang , Zhaojun Bai , Ren-cang Li

We consider optimization problems in which the goal is find a $k$-dimensional subspace of $\mathbb{R}^n$, $k<<n$, which minimizes a convex and smooth loss. Such problems generalize the fundamental task of principal component analysis (PCA)…

Optimization and Control · Mathematics 2022-10-27 Dan Garber , Ron Fisher

This paper deals with convex nonsmooth optimization problems. We introduce a general smooth approximation framework for the original function and apply random (accelerated) coordinate descent methods for minimizing the corresponding smooth…

Optimization and Control · Mathematics 2024-01-10 Flavia Chorobura , Ion Necoara

In this paper, we present a local convergence analysis of the self-consistent field (SCF) iteration using the density matrix as the state of a fixed-point iteration. Sufficient and almost necessary conditions for local convergence are…

Numerical Analysis · Mathematics 2018-11-26 Parikshit Upadhyaya , Elias Jarlebring , Emanuel H. Rubensson