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First principles calculations based on density functional theory are having an incerasing impact on our understanding of molecule-surface interactions. For example, calculations of the multi-dimensional potential energy surface have…

Materials Science · Physics 2007-05-23 O. Gulseren , D. M. Bird , S. E. Humphreys

We develop an efficient sampling and free energy calculation technique within the adaptive biasing potential (ABP) framework. By mollifying the density of states we obtain an approximate free energy and an adaptive bias potential that is…

Statistical Mechanics · Physics 2010-01-29 Bradley M. Dickson , Frederic Legoll , Tony Lelievre , Gabriel Stoltz , Paul Fleurat-Lessard

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

We present an approach for generating local numerical basis sets of improving accuracy for first-principles nanoplasmonics simulations within time-dependent density functional theory. The method is demonstrated for copper, silver, and gold…

Materials Science · Physics 2015-09-04 Tuomas P. Rossi , Susi Lehtola , Arto Sakko , Martti J. Puska , Risto M. Nieminen

Data-driven and non-intrusive DMDc and DMDspc models successfully expedite the reconstruction and forecasting of CO2 fluid flow with acceptable accuracy margins, aiding in the rapid optimization of geological CO2 storage forecast and…

Computational Physics · Physics 2025-04-01 Dimitrios Voulanas , Eduardo Gildin

We implement a total-energy minimization scheme to allow for relaxation of atomic positions in density functional calculations for two-dimensional (2D) systems using a mixed basis set. The basis functions consist of products of 2D plane…

Materials Science · Physics 2022-03-14 Chung-Yuan Ren , Yia-Chung Chang

This paper presents a systematic study of applying composite method approximations with locally dense basis sets (LDBS) to efficiently calculate NMR shielding constants in small and medium-sized molecules. The pcSseg-n series of basis sets…

Chemical Physics · Physics 2022-11-15 Jiashu Liang , Zhe Wang , Jie Li , Jonathan Wong , Xiao Liu , Brad Ganoe , Teresa Head-Gordon , Martin Head-Gordon

Density matrix embedding theory (DMET) is a fully quantum-mechanical embedding method which shows great promise as a method of defeating the inherent exponential cost scaling of multiconfigurational wave function-based calculations by…

Chemical Physics · Physics 2019-02-07 Matthew R. Hermes , Laura Gagliardi

A mixed basis approach based on density functional theory is extended to one-dimensional(1D) systems. The basis functions here are taken to be the localized B-splines for the two finite non-periodic dimensions and the plane waves for the…

Materials Science · Physics 2016-04-20 Chung-Yuan Ren , Yia-Chung Chang , Chen-Shiung Hsue

Methods of the explicitly correlated F12 approach are applied to the problem of calculating the uncoupled second-order dispersion energy in symmetry-adapted perturbation theory. The accuracy of the new method is tested for noncovalently…

Chemical Physics · Physics 2018-05-15 Michal Przybytek

Semi-empirical quantum mechanical methods traditionally expand the electron density in a minimal, valence-only electron basis set. The minimal-basis approximation causes molecular polarization to be underestimated, and hence intermolecular…

Chemical Physics · Physics 2015-09-30 Anders S. Christensen , Marcus Elstner , Qiang Cui

Despite the great success Kohn-Sham density functional theory (KS-DFT) has achieved, the delocalization error remains a major challenge for commonly used density functional approximations (DFAs), resulting in systematic errors in ionization…

Chemical Physics · Physics 2026-02-12 Yichen Fan , Jincheng Yu , Jiayi Du , Weitao Yang

An accurate determination of the electron correlation energy is essential for describing the structure, stability, and function in a wide variety of systems, ranging from gas-phase molecular assemblies to condensed matter and…

Chemical Physics · Physics 2014-03-05 Alberto Ambrosetti , Anthony M. Reilly , Robert A. DiStasio , Alexandre Tkatchenko

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…

The reduced basis method is used to construct a "universal" basis of Dirac orbitals that may be applicable throughout the nuclear chart to calibrate covariant energy density functionals. Relative to our earlier work using the…

Nuclear Theory · Physics 2024-06-05 Amy L. Anderson , J. Piekarewicz

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 offers accurate structure prediction at acceptable computational cost, but commonly used approximations suffer from delocalization error; this results in inaccurate predictions of quantities such as energy band…

Materials Science · Physics 2022-08-17 Aaron Mahler , Jacob Z. Williams , Neil Qiang Su , Weitao Yang

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

In many supervised learning applications, the response consists of both continuous and binary outcomes. Studies have shown that jointly modeling such mixed-type responses can substantially improve predictive performance compared to separate…

Methodology · Statistics 2026-03-13 Yu Wang , Ran Jin , Lulu Kang

Density fitting (DF), also known as the resolution of the identity (RI), is a widely used technique in quantum chemical calculations with various types of atomic basis sets - Gaussian-type orbitals, Slater-type orbitals, as well as…

Chemical Physics · Physics 2021-12-22 Susi Lehtola