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Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…

Chemical Physics · Physics 2025-01-22 Hanh D. M. Pham , Rustam Z. Khaliullin

Gradient-based methods are well-suited for derivative-free optimization (DFO), where finite-difference (FD) estimates are commonly used as gradient surrogates. Traditional stochastic approximation methods, such as Kiefer-Wolfowitz (KW) and…

Optimization and Control · Mathematics 2025-03-03 Guo Liang , Guangwu Liu , Kun Zhang

The optimization with orthogonality has been shown useful in training deep neural networks (DNNs). To impose orthogonality on DNNs, both computational efficiency and stability are important. However, existing methods utilizing Riemannian…

Machine Learning · Computer Science 2022-07-12 Fanchen Bu , Dong Eui Chang

We present a novel approach to address the challenges of variable occupation numbers in direct optimization of density functional theory (DFT). By parameterizing both the eigenfunctions and the occupation matrix, our method minimizes the…

We propose a simple and efficient method to calculate the electronic self-energy in dynamical mean-field theory (DMFT), addressing a numerical instability often encountered when solving the Dyson equation. Our approach formulates the Dyson…

Strongly Correlated Electrons · Physics 2025-03-27 Harrison LaBollita , Jason Kaye , Alexander Hampel

This article is part-I of a review of density-functional theory (DFT) that is the most widely used method for calculating electronic structure of materials. The accuracy and ease of numerical implementation of DFT methods has resulted in…

Materials Science · Physics 2023-05-25 Prashant Singh , Manoj K Harbola

Stochastic and mixed stochastic-deterministic density functional theory (DFT) are promising new approaches for the calculation of the equation-of-state and transport properties in materials under extreme conditions. In the intermediate warm…

Computational Physics · Physics 2023-09-27 Vidushi Sharma , Lee A. Collins , Alexander J. White

Large-scale density functional theory (DFT) calculations provide a powerful tool to investigate the atomic and electronic structure of materials with complex structures. This article reviews a large-scale DFT calculation method, the…

Materials Science · Physics 2022-08-31 Ayako Nakata , David R. Bowler , Tsuyoshi Miyazaki

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

This paper presents a novel Riemannian conjugate gradient method for the Kohn-Sham energy minimization problem in density functional theory (DFT), with a focus on non-metallic crystal systems. We introduce an energy-adaptive metric that…

Numerical Analysis · Mathematics 2025-03-21 Daniel Peterseim , Jonas Püschel , Tatjana Stykel

In this paper, we consider a class of stochastic optimization problems over the expectation-formulated generalized Stiefel manifold (SOEGS), where the objective function $f$ is continuously differentiable. We propose a novel constraint…

Optimization and Control · Mathematics 2024-12-31 Linshuo Jiang , Nachuan Xiao , Xin Liu

Density Functional Theory (DFT) allows for predicting all the chemical and physical properties of molecular systems from first principles by finding an approximate solution to the many-body Schr\"odinger equation. However, the cost of these…

Machine Learning · Computer Science 2025-06-03 Majdi Hassan , Cristian Gabellini , Hatem Helal , Dominique Beaini , Kirill Neklyudov

This paper investigates a category of constrained fractional optimization problems that emerge in various practical applications. The objective function for this category is characterized by the ratio of a numerator and denominator, both…

Optimization and Control · Mathematics 2026-05-28 Yizun Lin , Jian-Feng Cai , Zhao-Rong Lai , Cheng Li

We present a systematic, quasi-automated methodology for generating electronic models in the framework of second-principles density functional theory (SPDFT). This approach enables the construction of accurate and computationally efficient…

Projection-free optimization via different variants of the Frank-Wolfe (FW), a.k.a. Conditional Gradient method has become one of the cornerstones in optimization for machine learning since in many cases the linear minimization oracle is…

Optimization and Control · Mathematics 2020-06-30 Pavel Dvurechensky , Petr Ostroukhov , Kamil Safin , Shimrit Shtern , Mathias Staudigl

Density functional theory (DFT) is an essential building block for modern theoretical physics, chemistry, and engineering, especially those concerning electronic properties. Through decades of development, various program packages for…

Materials Science · Physics 2022-11-21 Yusuke Nomura , Ryosuke Akashi

One of the most promising techniques used for studying the electronic properties of materials is based on Density Functional Theory (DFT) approach and its extensions. DFT has been widely applied in traditional solid state physics problems…

Materials Science · Physics 2013-06-03 Nicola Varini , Davide Ceresoli , Layla Martin-Samos , Ivan Girotto , Carlo Cavazzoni

We show that classical molecular density functional theory (MDFT), here in the homogeneous reference fluid approximation in which the functional is inferred from the properties of the bulk solvent, is a powerful new tool to study, at a…

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

Chemical Physics · Physics 2022-04-18 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

The simulation of fracture using continuum ductile damage models attains a pathological discretization dependence caused by strain localization, after loss of ellipticity of the problem, in regions whose size is connected to the spatial…

Computational Engineering, Finance, and Science · Computer Science 2021-04-21 M. Magri , S. Lucarini , G. Lemoine , L. Adam , J. Segurado