Density-functional theory calculations of electronic transport based on local exchange and correlation functionals contain self-interaction errors. As a consequence, insulating molecules in weak contact with metallic electrodes erroneously form highly conducting junctions. Here we present a fully self-consistent and still computationally undemanding self-interaction correction scheme that overcomes these limitations. The method is implemented in the transport code SMEAGOL and applied to the prototypical case of benzene molecules and gold electrodes. The Kohn-Sham highest occupied molecular orbital now reproduces closely the negative of the molecular ionization potential and is moved away from the gold Fermi energy. This leads to a drastic reduction of the low-bias current in much better agreement with experiments.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1103/PhysRevLett.99.056801 | DOI Listing |
J Chem Phys
January 2025
Department of Physics, Chemistry and Pharmacy, University of Southern Denmark, Campusvej 55, DK-5230 Odense M, Denmark.
We present the theory and implementation of a fully variational wave function-density functional theory (DFT) hybrid model, which is applicable to many cases of strong correlation. We denote this model as the multiconfigurational self-consistent on-top pair-density functional theory (MC-srPDFT) model. We have previously shown how the multiconfigurational short-range DFT (MC-srDFT) hybrid model can describe many multiconfigurational cases of any spin symmetry and also state-specific calculations on excited states [Hedegård et al.
View Article and Find Full Text PDFMaterials (Basel)
December 2024
Faculty of Science and Technology, Norwegian University of Life Sciences, Drøbakveien 31, 1430 Ås, Norway.
The interaction of Ni with (6,0) and (8,0) zigzag carbon nanotube exterior surfaces containing two vacancies was studied using density functional theory (DFT). A two-vacancy defect was analysed in order to anchor Ni, and the pristine nanotube was also considered as a reference for each chirality. The adsorbed Ni stability and the nanotube's geometry and electronic structure were analysed before and after the adsorption.
View Article and Find Full Text PDFJ Phys Condens Matter
December 2024
Queensland Micro-nanotechnology Center, Griffith University, West Creek Road, Nathan, QLD 4111, Brisbane, Queensland, 4059, AUSTRALIA.
Charge transfer excitation energies are known to be challenging for standard time-dependent (TD) density functional theory (DFT) calculations. Perturbative ensemble DFT (pEDFT) was suggested as an easy-to-implelemt, low-cost alternative to TDDFT, because it is an in principle exact theory for calculating excitation energies that produces useful valence excitation energies. Here, we examine analytically and numerically (based on the benzene-tetracyanoethylene complex) how well pEDFT performs in the charge transfer limit.
View Article and Find Full Text PDFCells
December 2024
Institute of Biochemistry II, Jena University Hospital, Friedrich Schiller University Jena, Nonnenplan 2-4, 07743 Jena, Germany.
There is no doubt that the proper development of the heart is important for its correct function, in addition, maturation processes of the heart are crucial as well. The actin-binding protein nexilin seems to take over central roles in the latter processes, as nexilin-deficient mice are phenotypically inconspicuous at birth but die within short time thereafter. Recently, it has been proposed that nexilin plays a role in the formation and function of transverse tubules (T-tubules), which are essential for excitation-contraction coupling in the hearts of mature animals.
View Article and Find Full Text PDFChem Sci
December 2024
Department of Chemistry & Biochemistry, The Ohio State University 151 W. Woodruff Ave. Columbus Ohio 43210 USA
The many-body expansion is a fragment-based approach to large-scale quantum chemistry that partitions a single monolithic calculation into manageable subsystems. This technique is increasingly being used as a basis for fitting classical force fields to electronic structure data, especially for water and aqueous ions, and for machine learning. Here, we show that the many-body expansion based on semilocal density functional theory affords wild oscillations and runaway error accumulation for ion-water interactions, typified by F(HO) with ≳ 15.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!