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The van Leeuwen proof of linear-response time-dependent density functional theory (TDDFT) is generalized to thermal ensembles. This allows generalization to finite temperatures of the Gross-Kohn relation, the exchange-correlation kernel of…

Chemical Physics · Physics 2016-06-15 Aurora Pribram-Jones , Paul E. Grabowski , Kieron Burke

We investigate the construction of approximated exchange-correlation functionals by interpolating locally along the adiabatic connection between the weak- and the strong-coupling regimes, focussing on the effect of using approximate…

Chemical Physics · Physics 2017-04-05 Stefan Vuckovic , Lucas O. Wagner , Andrew M. Teale , Paola Gori-Giorgi

While the variational principle for excited-state energies leads to a route to obtaining excited-state densities from time-dependent density functional theory, relatively little attention has been paid to the quality of the resulting…

Chemical Physics · Physics 2025-09-12 Anna Baranova , Neepa T. Maitra

Time-dependent density functional theory (TDDFT) is a standard approach for calculating optical excitations of molecules and solids, while ensemble DFT (EDFT) is a promising alternative under development. We introduce ensemble TDDFT…

Chemical Physics · Physics 2026-05-22 Kimberly J. Daas , Steven Crisostomo , Kieron Burke

We have recently put forward a steady-state density functional theory (i-DFT) to calculate the transport coefficients of quantum junctions. Within i-DFT it is possible to obtain the steady density on and the steady current through an…

Mesoscale and Nanoscale Physics · Physics 2018-07-04 S. Kurth , G. Stefanucci

We present a new class of non-adiabatic approximations in time-dependent density functional theory derived from an exact expression for the time-dependent exchange-correlation potential. The approximations reproduce dynamical step and peak…

Chemical Physics · Physics 2018-12-21 Lionel Lacombe , Neepa T. Maitra

We identify peak and valley structures in the exact exchange-correlation potential of time-dependent density functional theory that are crucial for time-resolved electron scattering in a model one-dimensional system. These structures are…

Chemical Physics · Physics 2018-01-03 Yasumitsu Suzuki , Lionel Lacombe , Kazuyuki Watanabe , Neepa T. Maitra

The particle-hole interaction problem is longstanding within time-dependent density functional theory (TDDFT) and leads to extreme errors in the prediction of K-edge X-ray absorption spectra (XAS). We derive a linear-response formalism that…

Chemical Physics · Physics 2022-10-18 Kevin Carter-Fenk , Leonardo A. Cunha , Juan E. Arias-Martinez , Martin Head-Gordon

We develop a scheme for building the scalar exchange-correlation (xc) kernel of time-dependent density functional theory (TDDFT) from the tensorial kernel of time-dependent {\em current} density functional theory (TDCDFT) and the Kohn-Sham…

Materials Science · Physics 2009-11-13 V. U. Nazarov , J. M. Pitarke , Y. Takada , G. Vignale , Y. -C. Chang

Exact-exchange energy density and energy density of a semilocal density functional approximation are two key ingredients for modeling the static correlation, a strongly nonlocal functional of the density, through a local hybrid functional.…

Materials Science · Physics 2009-11-13 Jianmin Tao , Viktor N. Staroverov , Gustavo E. Scuseria , John P. Perdew

We discuss energy densities in the strong-interaction limit of density functional theory, deriving an exact expression within the definition (gauge) of the electrostatic potential of the exchange-correlation hole. Exact results for small…

Chemical Physics · Physics 2012-11-14 André Mirtschink , Michael Seidl , Paola Gori-Giorgi

We present a detailed study of the exact-exchange (EXX) kernel of time-dependent density functional theory with an emphasis on its discontinuity at integer particle numbers. It was recently found that this exact property leads to sharp…

Chemical Physics · Physics 2015-06-17 M. Hellgren , E. K. U. Gross

We present a detailed study of different exchange-correlation (xc) functionals in describing the dynamical properties of finite systems. For that purpose, we calculated the static polarizabilities, ionization potentials and optical…

Soft Condensed Matter · Physics 2009-11-07 M. A. L. Marques , Alberto Castro , Angel Rubio

The exchange-correlation hole and potential of the homogeneous electron gas have been investigated within the random-phase approximation, employing the plasmon-pole approximation for the linear density response function. The angular…

Strongly Correlated Electrons · Physics 2023-04-12 K. Karlsson , F. Aryasetiawan

Quantum-electrodynamical density-functional theory (QEDFT) provides a promising avenue for exploring complex light-matter interactions in optical cavities for real materials. Similar to conventional density-functional theory, the Kohn-Sham…

Computational Physics · Physics 2024-02-16 I-Te Lu , Michael Ruggenthaler , Nicolas Tancogne-Dejean , Simone Latini , Markus Penz , Angel Rubio

Ensemble density functional theory (EDFT) is a promising alternative to time-dependent density functional theory for computing electronic excitation energies. Using coordinate scaling, we prove several fundamental exact conditions in EDFT…

Strongly Correlated Electrons · Physics 2023-07-04 Thais R. Scott , John Kozlowski , Steven Crisostomo , Aurora Pribram-Jones , Kieron Burke

From a simplified version of the mathematical structure of the strong coupling limit of the exact exchange-correlation functional, we construct an approximation for the electronic repulsion energy at physical coupling strength, which is…

Chemical Physics · Physics 2017-05-11 Stefan Vuckovic , Paola Gori-Giorgi

An approximate solution to the time-dependent density functional theory (TDDFT) response equations for finite systems is developed, yielding corrections to the single-pole approximation. These explain why allowed Kohn-Sham transition…

Materials Science · Physics 2009-11-07 H. Appel , E. K. U. Gross , K. Burke

We demonstrate the capabilities of time-dependent density functional theory (TDDFT) for strong-field, short wavelength (soft X-ray) physics, as compared to a formalism based on rate equations. We find that TDDFT provides a very good…

Exchange-correlation potentials vxc and energy densities exc are derived for integer and fractional electron counts using an orbital-averaged Kohn-Sham inversion procedure. The reference densities for inversion come from full configuration…

Chemical Physics · Physics 2025-04-30 Vaibhav Khanna , Bikash Kanungo , Jeffrey Hatch , Joshua Kammeraad , Paul M. Zimmerman