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We demonstrate in the present study that self-consistent calculations based on the self-energy functional theory (SFT) are possible for the electronic structure of realistic systems in the context of quantum chemistry. We describe the…

Materials Science · Physics 2018-06-14 Taichi Kosugi , Hirofumi Nishi , Yoritaka Furukawa , Yu-ichiro Matsushita

We introduce an efficient finite-element approach for large-scale real-space pseudopotential density functional theory (DFT) calculations incorporating noncollinear magnetism and spin-orbit coupling. The approach, implemented within the…

Materials Science · Physics 2025-06-11 Nikhil Kodali , Phani Motamarri

The practical utility of M{\o}ller-Plesset (MP) perturbation theory is severely constrained by the use of Hartree-Fock (HF) orbitals. It has recently been shown that use of regularized orbital-optimized MP2 orbitals and scaling of MP3…

Chemical Physics · Physics 2021-01-06 Adam Rettig , Diptarka Hait , Luke W. Bertels , Martin Head-Gordon

We present a comparative study of the spatial distribution of the spin density (SD) of the ground state of CuCl2 using Density Functional Theory (DFT), quantum Monte Carlo (QMC), and post-Hartree-Fock wavefunction theory (WFT). A number of…

Chemical Physics · Physics 2016-07-25 Michel Caffarel , Emmanuel Giner , Anthony Scemama , Alejandro Ramírez-Solís

Unrestricted DFT methods are typically expected to describe the homolytic dissociation of nonpolar single bonds in neutral species with qualitative accuracy, due to the lack of significant delocalization error. We however find that many…

Chemical Physics · Physics 2019-03-15 Diptarka Hait , Adam Rettig , Martin Head-Gordon

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…

Density functional theory (DFT) is an exact alternative formulation of quantum mechanics, in which it is possible to calculate the total energy, the spin and the charge density of many-electron systems in the ground state. In practice, it…

Atomic Physics · Physics 2014-03-25 Uri Argaman , Guy Makov , Eli Kraisler

We present a critical analysis of the popular fragment-orbital density-functional theory (FO-DFT) scheme for the calculation of electronic coupling values. We discuss the characteristics of different possible formulations or 'flavors' of…

Materials Science · Physics 2016-02-17 Christoph Schober , Karsten Reuter , Harald Oberhofer

We study the spin-crossover molecule Fe(phen)$_2$(NCS)$_2$ using density functional theory (DFT) plus dynamical mean-field theory, which allows access to observables not attainable with traditional quantum chemical or electronic structure…

Materials Science · Physics 2015-06-30 Jia Chen , Andrew Millis , Chris Marianetti

This chapter concerns with the recent development of a new DFT methodology for accurate, reliable prediction of many-electron systems. Background, need for such a scheme, major difficulties encountered, as well as their potential remedies…

Chemical Physics · Physics 2019-04-19 Amlan K. Roy

Density functional theory (DFT), one of the most widely utilized methods available to computational chemistry, fails to describe systems with statically correlated electrons. To address this shortcoming, in previous work we transformed DFT…

Chemical Physics · Physics 2023-01-02 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

We estimate the prediction sensitivity with respect to Hartree-Fock exchange in approximate density functionals for representative Fe(II) and Fe(III) octahedral complexes. Based on the observation that the range of parameters spanned by the…

Materials Science · Physics 2015-07-16 Efthymios I. Ioannidis , Heather J. Kulik

We present a systematic Density Functional Theory (DFT) study of geometries and energies of the nucleic acid DNA bases (guanine, adenine, cytosine and thymine) and 30 different DNA base-pairs. We use a recently developed linear-scaling DFT…

Chemical Physics · Physics 2007-05-23 Maider Machado , Pablo Ordejon , Emilio Artacho , Daniel Sanchez-Portal , Jose M. Soler

Self-consistency based Kohn-Sham density functional theory (KS-DFT) electronic structure calculations with Gaussian basis sets are reported for a set of 17 protein-like molecules with geometries obtained from the protein data bank. It is…

Chemical Physics · Physics 2012-01-10 Elias Rudberg

Density-corrected density functional theory (DC-DFT) is enjoying substantial success in improving semilocal DFT calculations in a wide variety of chemical problems. This paper provides the formal theoretical framework and assumptions for…

Chemical Physics · Physics 2019-08-19 Stefan Vuckovic , Suhwan Song , John Kozlowski , Eunji Sim , Kieron Burke

Standard flavors of density-functional theory (DFT) calculations are known to fail in describing anions, due to large self-interaction errors. The problem may be circumvented by using localized basis sets of reduced size, leaving no…

Chemical Physics · Physics 2019-12-23 Francesco Nattino , Céline Dupont , Nicola Marzari , Oliviero Andreussi

Evolutionary algorithms for molecular design require computationally efficient yet accurate fitness functions. We systematically benchmark Hartree-Fock and density functional theory for predicting molecular first hyperpolarizability…

Chemical Physics · Physics 2026-04-24 Dominic Mashak , S. A. Alexander

Within the nuclear density functional theory (DFT) we study the effect of reflection-asymmetric shapes on ground-state binding energies and binding energy differences. To this end, we developed the new DFT solver AxialHFB that uses an…

Nuclear Theory · Physics 2013-03-05 E. Olsen , J. Erler , W. Nazarewicz , M. Stoitsov

Density functional theory (DFT) underpins modern atomistic simulations of transition-metal surfaces. It can predict key properties linked to catalytic performance, such as adsorption energies and barrier heights, enabling new paradigms in…

Materials Science · Physics 2026-03-23 Benjamin X. Shi , Timothy C. Berkelbach

The design of better exchange-correlation functionals for Density Functional Theory (DFT) is a central challenge of modern electronic structure theory. However, current developments are limited by the mathematical form of the functional,…

Chemical Physics · Physics 2024-08-19 Kyle Bystrom , Boris Kozinsky