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We study static correlation and delocalisation errors and show that even methods with good energies can yield significant delocalization errors that affect the density, leading to large errors in predicting {\em e.g.} dipole moments. We…

Chemical Physics · Physics 2020-06-01 Maria Hellgren , Tim Gould

Orbital-free density functional theory (OF-DFT) holds the promise to compute ground state molecular properties at minimal cost. However, it has been held back by our inability to compute the kinetic energy as a functional of the electron…

Chemical Physics · Physics 2023-10-25 Roman Remme , Tobias Kaczun , Maximilian Scheurer , Andreas Dreuw , Fred A. Hamprecht

We present a simplified density functional theory (DFT) method to com- pute vertical electron and hole attachment energies to frontier orbitals of molecules absorbed on insulating films supported by a metal substrate. The adsorbate and the…

Mesoscale and Nanoscale Physics · Physics 2017-08-29 Ivan Scivetti , Mats Persson

A new method for calculating optical absorption spectra within linear-scaling density-functional theory (LS-DFT) is presented, incorporating a scheme for optimizing a set of localized orbitals to accurately represent unoccupied Kohn-Sham…

Materials Science · Physics 2015-05-30 Laura E. Ratcliff , Nicholas D. M. Hine , Peter D. Haynes

We formulate the Kohn-Sham density functional theory (KS-DFT) as a statistical theory in which the electron density is deter-mined from an average of correlated stochastic densities in a trace formula. The key idea is that it is sufficient…

Materials Science · Physics 2015-06-15 Roi Baer , Daniel Neuhauser , Eran Rabani

This chapter presents the development of a density functional theory (DFT)-based method for accurate, reliable treatment of various resonances in atoms. Many of these are known to be notorious for their strong correlation, proximity to more…

Chemical Physics · Physics 2019-04-19 Amlan K. Roy

We present a rigorous formulation of the time-dependent density functional theory for interacting lattice electrons strongly coupled to cavity photons. We start with an example of one particle on a Hubbard dimer coupled to a single photonic…

Strongly Correlated Electrons · Physics 2015-06-22 Mehdi Farzanehpour , I. V. Tokatly

In the recent work of S. Sharma \emph{et al.}, (arxiv.org: arxiv:0912.1118), a single-electron spectrum associated with the natural orbitals was defined as the derivative of the total energy with respect to the occupation numbers at half…

Chemical Physics · Physics 2012-03-07 E. N. Zarkadoula , S. Sharma , J. K. Dewhurst , E. K. U. Gross , N. N. Lathiotakis

Quantum embedding approaches involve the self-consistent optimization of a local fragment of a strongly correlated system, entangled with the wider environment. The `energy-weighted' density matrix embedding theory (EwDMET) was established…

Strongly Correlated Electrons · Physics 2021-02-23 P. V. Sriluckshmy , Max Nusspickel , Edoardo Fertitta , George H. Booth

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 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

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

In this note, we show that the Local Molecular Field theory of Weeks et. al. can be re-derived as an extremum problem for an approximate Helmholtz free energy. Using the resulting free energy as a classical, fluid density functional yields…

Soft Condensed Matter · Physics 2025-07-15 David M. Rogers

As part of a project to obtain better optical response functions for nano materials and other systems with strong excitonic effects we here calculate the exchange-correlation (XC) potential of density-functional theory (DFT) at a level of…

Other Condensed Matter · Physics 2009-11-13 M. Hellgren , U. von Barth

Accurate and efficient theoretical descriptions of lanthanide systems based on ab initio electronic structure theory remain highly challenging due to the complex interplay of strong electronic correlation and significant relativistic…

Chemical Physics · Physics 2025-03-04 Yuhang Ai , Ze-Wei Li , Zhe-Bin Guan , Hong Jiang

We introduce real-time density matrix embedding theory (DMET), a dynamical quantum embedding theory for computing non-equilibrium electron dynamics in strongly correlated systems. As in the previously developed static DMET, real-time DMET…

Chemical Physics · Physics 2017-11-03 Joshua S. Kretchmer , Garnet Kin-Lic Chan

We present a method to make highly accurate pseudopotentials for use with orbital-free density functional theory (OF-DFT) with given exchange-correlation and kinetic energy functionals, which avoids the compounding of errors of Kohn-Sham…

Materials Science · Physics 2015-02-04 Fleur Legrain , Sergei Manzhos

Current-spin density functional theory (CSDFT) provides a framework to describe interacting many-electron systems in a magnetic field which couples to both spin- and orbital-degrees of freedom. Unlike in usual (spin-) density functional…

Materials Science · Physics 2015-06-25 S. Pittalis , S. Kurth , N. Helbig , E. K. U. Gross

We use projector operators to correct the Kohn-Sham Hamiltonian of density functional theory (KS-DFT) so that the resulting mean-field scheme yields, in finite systems, virtual orbitals and energy gaps in better agreement with those…

Other Condensed Matter · Physics 2008-06-26 Hector Mera

In pursuit of a colloidal analogue to quantum density functional theory (DFT) predictions of atomic crystal structures, we report a new, classical DFT that predicts the relative thermodynamic stability of colloidal crystals of hard, convex…

Soft Condensed Matter · Physics 2026-01-15 Kristi Pepa , Isaac R. Spivack , Trevor F. G. Teague , Ryn Y. Oliphant , Domagoj Fijan , Sharon C. Glotzer
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