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In recent years, "composite" density-functional-theory-based methods comprising specially optimized combinations of functionals, basis sets, and empirical corrections have become widely used owing to their robustness and computational…

Chemical Physics · Physics 2024-11-21 Corin C. Wagen , Jonathon E. Vandezande

Approximate density functional theory (DFT) suffers from many-electron self- interaction error, otherwise known as delocalization error, that may be diagnosed and then corrected through elimination of the deviation from exact piecewise…

Materials Science · Physics 2016-11-08 Terry Z. H. Gani , Heather J. Kulik

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

Using GPU-accelerated state-vector emulation, we propose to embed a quantum computing ansatz into density-functional theory via density-based basis-set corrections (DBBSC) to obtain quantitative quantum-chemistry results on molecules that…

Delocalization errors, such as charge-transfer and some self-interaction errors, plague computationally-efficient and otherwise-accurate density functional approximations (DFAs). Evaluating a semi-local DFA non-self-consistently on the…

Chemical Physics · Physics 2023-01-02 Aaron D. Kaplan , Chandra Shahi , Pradeep Bhetwal , Raj K. Sah , John P. Perdew

Delocalization error prevents density functional theory (DFT) from reaching its full potential, causing problems like systematically underestimated band gaps and misaligned energy levels at interfaces. We introduce lrLOSC to correct…

Materials Science · Physics 2026-04-29 Jacob Z. Williams , Weitao Yang

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

Recent work has shown that a fully many-body treatment of noncovalent interactions, such as that given by the method of many-body dispersion (MBD), is vital to accurately modeling the structure and energetics of many molecular systems with…

Here we present a density matrix based KS inversion method formulated entirely within a Gaussian basis representation to optimize a KS potential matrix that reproduces a target electron density. Inverse Kohn-Sham (KS) density functional…

Chemical Physics · Physics 2026-03-24 Ziwei Chai , Sandra Luber

Double-hybrid density functional theory (DHDFT) offers a pathway to accuracies approaching composite wavefunction approaches like G4 theory. However, the GLPT2 (G{\"o}rling 2nd order perturbation theory) term causes them to partially…

Chemical Physics · Physics 2022-10-13 Nisha Mehta , Jan M. L. Martin

Nuclear density functional theory (DFT) is the only microscopic, global approach to the structure of atomic nuclei. It is used in numerous applications, from determining the limits of stability to gaining a deep understanding of the…

Nuclear Theory · Physics 2015-02-06 Nicolas Schunck , Jordan D. McDonnell , Jason Sarich , Stefan M. Wild , Dave Higdon

We present the first application to real molecular systems of the recently proposed linear-response theory for the density-based basis-set correction method [J. Chem. Phys. 158, 234107 (2023)]. We apply this approach to accelerate the…

Chemical Physics · Physics 2024-02-27 Diata Traore , Julien Toulouse , Emmanuel Giner

In approximate density functional theory (DFT), the self-interaction error is an electron delocalization anomaly associated with underestimated insulating gaps. It exhibits a predominantly quadratic energy-density curve that is amenable to…

Chemical Physics · Physics 2016-12-21 Glenn Moynihan , Gilberto Teobaldi , David D. O'Regan

In this work we explore the performance of approximations to electron correlation in reduced density-matrix functional theory (RDMFT) and of approximations to the observables calculated within this theory. Our analysis focuses on the…

Strongly Correlated Electrons · Physics 2015-02-26 Stefano Di Sabatino , Jan A. Berger , Lucia Reining , Pina Romaniello

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

Hydrogen bonding is an important non-covalent interaction that plays a major role in molecular self-organization and supramolecular structures. It can be described accurately with ab initio quantum chemical wave function methods, which…

Chemical Physics · Physics 2025-05-16 Usman Ahmed , Mikael P. Johansson , Susi Lehtola , Dage Sundholm

We present a detailed analysis of the broken-symmetry mean-field solutions using a four-electron rectangular quantum dot as a model system. Comparisons of the density-functional theory predictions with the exact ones show that the symmetry…

Condensed Matter · Physics 2009-11-10 A. Harju , E. Rasanen , H. Saarikoski , M. J. Puska , R. M. Nieminen , K. Niemela

The delocalization error of popular density functional approximations (DFAs) leads to diversified problems in present-day density functional theory calculations. For achieving a universal elimination of delocalization error, we develop a…

Chemical Physics · Physics 2017-09-07 Chen Li , Xiao Zheng , Neil Qiang Su , Weitao Yang

We develop a second order correction to commonly used density functional approximations (DFA) to eliminate the systematic delocalization error. The method, based on the previously developed global scaling correction (GSC), is an exact…

Chemical Physics · Physics 2021-07-22 Yuncai Mei , Zehua Chen , Weitao Yang

A recent paper compares density functional theory results for atomization energies and dipole moments using a multi-wavelet based method with traditional Gaussian basis set results, and concludes that Gaussian basis sets are problematic for…

Computational Physics · Physics 2017-11-01 Frank Jensen