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Kohn-Sham spin-density functional theory provides an efficient and accurate model to study electron-electron interaction effects in quantum dots, but its application to large systems is a challenge. An efficient algorithm for the…

Mesoscale and Nanoscale Physics · Physics 2007-05-23 Hong Jiang , Harold U. Baranger , Weitao Yang

As a proof of principle, self-consistent Kohn--Sham calculations are performed with the exact exchange-correlation functional. Finding the exact functional for even one trial density requires solving the interacting Schr\"odinger equation…

Chemical Physics · Physics 2014-07-14 Lucas O. Wagner , Thomas E. Baker , E. M. Stoudenmire , Kieron Burke , Steven R. White

In the context of the density functional theory we consider the single particle excitation spectra of electron systems. As a result, we have related the single particle excitations with the eigenvalues of the corresponding Kohn-Sham…

Condensed Matter · Physics 2009-10-31 M. Ya. Amusia , V. R. Shaginyan

We study the accuracy of Kohn-Sham density functional theory (DFT) for warm- and hot-dense matter (WDM and HDM). Specifically, considering a wide range of systems, we perform accurate ab initio molecular dynamics simulations with…

Computational Physics · Physics 2024-11-21 Phanish Suryanarayana , Arpit Bhardwaj , Xin Jing , Shashikant Kumar , John E. Pask

We present an implementation of time-dependent density-functional theory (TDDFT) in the linear response formalism enabling the calculation of low energy optical absorption spectra for large molecules and nanostructures. The method avoids…

Spectroscopies that probe electronic excitations from core levels into unoccupied orbitals, such as X-ray absorption spectroscopy and electron energy loss spectroscopy, are widely used to gain insight into the electronic and chemical…

Materials Science · Physics 2022-09-12 Marcus Annegarn , Juhan Matthias Kahk , Johannes Lischner

We model the Hartree-exchange-correlation potential of Kohn-Sham density-functional theory adopting a novel strategy inspired by the strictly-correlated-electrons limit and relying on the exact decomposition of the potential based on the…

Chemical Physics · Physics 2024-09-09 Sara Giarrusso , Federica Agostini

We propose a way to improve energy density functionals (EDFs) in the density functional theory based on the combination of the inverse Kohn--Sham method and the density functional perturbation theory. Difference between the known EDF and…

Chemical Physics · Physics 2019-11-22 Tomoya Naito , Daisuke Ohashi , Haozhao Liang

This chapter presents controlled approximations of Kohn-Sham density functional theory (DFT) that enable very large scale simulations. The work is motivated by the study of defects in crystalline solids, though the ideas can be used in…

Materials Science · Physics 2021-12-14 Kaushik Bhattacharya , Vikram Gavini , Michael Ortiz , Mauricio Ponga , Phanish Suryanarayana

Kohn-Sham density functional theory (DFT) is a widely-used electronic structure theory for materials as well as molecules. DFT is needed especially for large systems, ab initio molecular dynamics, and high-throughput searches for functional…

The Kohn-Sham approach to time-dependent density-functional theory (TDDFT) can be formulated, in principle exactly, by invoking the force-balance equation for the density, which leads to an explicit expression for the exchange-correlation…

Chemical Physics · Physics 2021-09-15 Walter Tarantino , Carsten A. Ullrich

An optical absorption spectrum constitutes one of the most fundamental material characteristics, with relevant applications ranging from material identification to energy harvesting and optoelectronics. However, the database of both…

Materials Science · Physics 2022-09-20 Ruo Xi Yang , Matthew K. Horton , Jason Munro , Kristin A. Persson

We use the exact strong-interaction limit of the Hohenberg-Kohn energy density functional to approximate the exchange-correlation energy of the restricted Kohn-Sham scheme. Our approximation corresponds to a highly non-local density…

Strongly Correlated Electrons · Physics 2012-12-12 Francesc Malet , Paola Gori-Giorgi

Time-dependent density functional theory (TDDFT) simulations of transient core-level spectroscopies require a balanced treatment of both valence- and core-electron excitations. To this end, tuned range-separated hybrid exchange-correlation…

Materials Science · Physics 2020-06-04 C. D. Pemmaraju

Recently, Zacharias et al [Phys. Rev. Lett. 115, 177401 (2015)] developed a new ab initio theory of temperature-dependent optical absorption spectra and band gaps in semiconductors and insulators. In that work the zero-point renormalization…

Materials Science · Physics 2016-08-17 Marios Zacharias , Feliciano Giustino

We present a real-space formulation for coarse-graining Kohn-Sham Density Functional Theory that significantly speeds up the analysis of material defects without appreciable loss of accuracy. The approximation scheme consists of two steps.…

Computational Physics · Physics 2015-06-11 Phanish Suryanarayana , Kaushik Bhattacharya , Michael Ortiz

We use the exact strong-interaction limit of the Hohenberg-Kohn energy density functional to construct an approximation for the exchange-correlation term of the Kohn-Sham approach. The resulting exchange-correlation potential is able to…

Strongly Correlated Electrons · Physics 2013-04-05 Francesc Malet , André Mirtschink , Jonas C. Cremon , Stephanie M. Reimann , Paola Gori-Giorgi

We present a mixed basis-set approach to obtain optical absorption spectra within a generalized Kohn-Sham time-dependent density functional theory framework. All occupied valence molecular orbitals (MOs) are expanded in a plane-wave (PW)…

Chemical Physics · Physics 2025-08-13 Kyle Chen , Barry Y. Li , Tucker Allen , Daniel Neuhauser

Understanding, optimizing, and controlling the optical absorption process, exciton gemination, and electron-hole separation and conduction in low dimensional systems is a fundamental problem in materials science. However, robust and…

Mesoscale and Nanoscale Physics · Physics 2020-08-26 Keenan Lyon , María Rosa Preciado-Rivas , Duncan John Mowbray , Vito Despoja

Using the Kohn-Sham (KS) inversion method of Hollins et al. [J. Phys.: Condens. Matter 29, 04LT01 (2017)], we invert densities from variational and diffusion quantum Monte Carlo (QMC) calculations to obtain benchmark QMC-KS potentials for a…