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In the dynamics of atoms and molecules at metal surfaces, electron-hole pair excitations can play a crucial role. In the case of hyperthermal hydrogen atom scattering, they lead to nonadiabatic energy loss and highly inelastic scattering.…

Materials Science · Physics 2024-12-02 Connor L. Box , Nils Hertl , Wojciech G. Stark , Reinhard J. Maurer

We introduce an orbital free electron density functional approximation based on alchemical perturbation theory. Given convergent perturbations of a suitable reference system, the accuracy of popular self-consistent Kohn-Sham density…

Chemical Physics · Physics 2020-05-27 Guido Falk von Rudorff , O. Anatole von Lilienfeld

The hydrogen molecule has become a test ground for quantum electrodynamical calculations in molecules. Expanding beyond studies on stable hydrogenic species to the heavier radioactive tritium-bearing molecules, we report on a measurement of…

Chemical Physics · Physics 2018-04-25 T. Madhu Trivikram , M. Schlösser , W. Ubachs , E. J. Salumbides

The accuracy of applying density functional theory to noncovalent interactions is hindered by errors arising from low-density regions of interaction-induced change in the density gradient, error compensation between correlation and exchange…

Chemical Physics · Physics 2014-10-22 Marcin Modrzejewski , Grzegorz Chałasiński , Małgorzata M. Szczęśniak

By using the quantum Ising chain as a test bed and treating the spin polarization along the external transverse field as the "generalized density", we examine the performance of different levels of density functional approximations parallel…

Computational Physics · Physics 2021-10-27 Jiahao Mao , Haifeng Tang , Wenhui Duan , Zheng Liu

The construction of meta generalized gradient approximations based on the density matrix expansion (DME) is considered as one of the most accurate technique to design semilocal exchange energy functionals in two-dimensional density…

Materials Science · Physics 2018-05-09 Abhilash Patra , Subrata Jana , Prasanjit Samal

Density functional theory is the standard theory for computing the electronic structure of materials, which is based on a functional that maps the electron density to the energy. However, a rigorous form of the functional is not known and…

Materials Science · Physics 2021-12-02 Ryo Nagai , Ryosuke Akashi , Osamu Sugino

A widely used approximation to the exchange-correlation functional in density functional theory is the local density approximation (LDA), typically derived from the properties of the homogeneous electron gas (HEG). We previously introduced…

Other Condensed Matter · Physics 2018-06-27 Mike Entwistle , Michele Casula , Rex Godby

The performance of two modern density-functionals, HSE06 and TB-mBJ, on predicting electronic structures of metal oxides, chalcogenides and nitrides, is studied in terms of band gaps, band structure and projected density-of-states. Contrary…

Materials Science · Physics 2013-03-22 Wenqing Li , Christian F. J. Walther , Agnieszka Kuc , Thomas Heine

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

We propose a multiconfigurational hybrid density-functional theory which rigorously combines a multiconfiguration self-consistent-field calculation with a density-functional approximation based on a linear decomposition of the…

Chemical Physics · Physics 2012-08-20 Kamal Sharkas , Andreas Savin , Hans Jørgen Aa. Jensen , Julien Toulouse

Multiconfiguration pair-density functional theory (MC-PDFT) is a post-MCSCF multireference electronic-structure method that explicitly models strong electron correlation, and linearized pair-density functional theory (L-PDFT) is a recently…

Parameterized tight-binding models fit to first principles calculations can provide an efficient and accurate quantum mechanical method for predicting properties of molecules and solids. However, well-tested parameter sets are generally…

Materials Science · Physics 2023-04-28 Kevin F. Garrity , Kamal Choudhary

We have performed self-consistent calculations for first and second row atoms using a variant of density-functional theory, the optimized effective potential method, with an approximation due to Krieger, Li and Iafrate and a…

chem-ph · Physics 2009-10-28 Tobias Grabo , E. K. U. Gross

We perform calculations of the {3D} finite-temperature homogeneous electron gas (HEG) in the warm-dense regime ({r_{s} \equiv (3/4\pi n)^{1/3}a_{B}^{- 1} = 1.0- 40.0} and {\Theta \equiv T/T_{F} = 0.0625- 8.0}) using restricted path integral…

Strongly Correlated Electrons · Physics 2013-04-10 Ethan W. Brown , Bryan K. Clark , Jonathan L. DuBois , David M. Ceperley

We present a global hybrid meta-generalized gradient approximation (meta-GGA) with three empirical parameters, as well as its underlying semilocal meta-GGA and a meta-GGA with only one empirical parameter. All of them are based on the new…

We present the WCCR10 data set of ten ligand dissociation energies of large cationic transition metal complexes for the assessment of approximate exchange--correlation functionals. We analyze nine popular functionals, namely BP86, BP86-D3,…

Chemical Physics · Physics 2014-09-30 Thomas Weymuth , Erik P. A. Couzijn , Peter Chen , Markus Reiher

The derivative discontinuity of the exchange-correlation functional of density-functional theory is cast as the difference of two types of electron affinities. We show that standard Kohn-Sham calculations can be used to calculate both…

Chemical Physics · Physics 2007-12-13 F. P. Rosselli , A. B. F. da Silva , K. Capelle

High quality reference data from diffusion Monte Carlo calculations are presented for bulk sI methane hydrate, a complex crystal exhibiting both hydrogen-bond and dispersion dominated interactions. The performance of some commonly used…

Materials Science · Physics 2014-05-13 Stephen J. Cox , Michael D. Towler , Dario Alfè , Angelos Michaelides

Physically valid and numerically efficient approximations for the exchange and correlation energy are critical for reduced density-matrix functional theory to become a widely used method in electronic structure calculations. Here we examine…

Strongly Correlated Electrons · Physics 2016-03-23 A. Putaja , F. G. Eich , T. Baldsiefen , E. Rasanen
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