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We show that as an electron transfers between closed-shell molecular fragments at large separation, the exact correlation potential of time-dependent density functional theory gradually develops a step and peak structure in the bonding…

Chemical Physics · Physics 2014-02-11 Johanna I. Fuks , Peter Elliott , Angel Rubio , Neepa T. Maitra

The polarization-dependence of the exchange-correlation (XC) energy functional of periodic insulators within Kohn-Sham (KS) density-functional theory requires a ${\cal O} (1/q^2)$ divergence in the XC kernel for small vectors q. This…

Materials Science · Physics 2009-10-30 Ph. Ghosez , X. Gonze , R. W. Godby

The most accurate theoretical method to describe excitons is the solution of the Bethe-Salpeter equation in the GW approximation (GW-BSE). However, because of its computation cost, time-dependent density functional theory (TDDFT) is…

Materials Science · Physics 2023-01-11 Rita Maji , Elena Degoli , Monica Calatayud , Valérie Véniard , Eleonora Luppi

We show that the analytic structure of the dynamical xc kernels of semiconductors and insulators can be sensed in terms of its poles which mark physically relevant frequencies of the system where the counter-phase motion of discrete…

Materials Science · Physics 2023-04-19 D. R. Gulevich , Ya. V. Zhumagulov , V. Kozin , I. V. Tokatly

Time-dependent (current) density functional theory for many-electron systems strongly coupled to quantized electromagnetic modes of a microcavity is proposed. It is shown that the electron-photon wave function is a unique functional of the…

Mesoscale and Nanoscale Physics · Physics 2013-12-10 I. V. Tokatly

We put forward new approach for the development of a non-local density functional by a direct modeling of the shape of exchange-correlation (xc) hole in inhomogeneous systems. The functional is aimed at giving an accurate xc-energy and an…

Other Condensed Matter · Physics 2013-08-05 Klaas J. H. Giesbertz , Robert van Leeuwen , Ulf von Barth

Parametric correlations are studied in several classes of covariant density functional theories (CDFTs) using a statistical analysis in a large parameter hyperspace. In the present manuscript, we investigate such correlations for two…

Nuclear Theory · Physics 2020-03-17 A. Taninah , S. E. Agbemava , A. V. Afanasjev , P. Ring

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

Adiabatic time-dependent density functional theory fails for excitations of a heteroatomic molecule composed of two open-shell fragments at large separation. Strong frequency-dependence of the exchange-correlation kernel is necessary for…

Other Condensed Matter · Physics 2009-11-11 Neepa T. Maitra , David G. Tempel

The near nucleus behavior of the exchange-correlation potential $v_{xc}({\bf r})$ in Hohenberg-Kohn-Sham density functional theory is investigated. It is shown that near the nucleus the linear term of $O(r)$ of the spherically averaged…

Materials Science · Physics 2009-11-13 Zhixin Qian

We propose a new conditional dependence measure and a statistical test for conditional independence. The measure is based on the difference between analytic kernel embeddings of two well-suited distributions evaluated at a finite set of…

Machine Learning · Statistics 2022-06-17 Meyer Scetbon , Laurent Meunier , Yaniv Romano

In order to assess the accuracy of commonly used approximate exchange-correlation density functionals, we present a comparison of accurate exchange and correlation potentials, exchange energy densities and energy components with the…

Condensed Matter · Physics 2007-05-23 Claudia Filippi , Xavier Gonze , C. J. Umrigar

A kernel-based framework for spatio-temporal data analysis is introduced that applies in situations when the underlying system dynamics are governed by a dynamic equation. The key ingredient is a representer theorem that involves…

Statistics Theory · Mathematics 2020-11-16 Oleg Szehr , Dario Azzimonti , Laura Azzimonti

We investigate a number of formal properties of the adiabatic strictly-correlated electrons (SCE) functional, relevant for time-dependent potentials and for kernels in linear response time-dependent density functional theory. Among the…

Strongly Correlated Electrons · Physics 2016-08-24 Giovanna Lani , Simone di Marino , Augusto Gerolin , Robert van Leeuwen , Paola Gori-Giorgi

Charge transfer plays a crucial role in many processes of interest in physics, chemistry, and bio-chemistry. In many applications the size of the systems involved calls for time-dependent density functional theory (TDDFT) to be used in…

Chemical Physics · Physics 2017-10-11 Neepa T. Maitra

We show that the exact exchange-correlation potential of time-dependent density-functional theory displays dynamical step structures that have a spatially non-local and time non-local dependence on the density. Using one-dimensional…

Chemical Physics · Physics 2015-06-12 Peter Elliott , Johanna I. Fuks , Angel Rubio , Neepa T. Maitra

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

Kernel adaptive filters, a class of adaptive nonlinear time-series models, are known by their ability to learn expressive autoregressive patterns from sequential data. However, for trivial monotonic signals, they struggle to perform…

Machine Learning · Statistics 2017-07-14 Felipe Tobar

In the context of inhomogeneous one-dimensional finite systems, recent numerical advances [Phys. Rev. B 103, 125155 (2021)] allow us to compute the exact coupling-constant dependent exchange-correlation kernel…

Materials Science · Physics 2021-09-22 Nick D. Woods , Michael T. Entwistle , Rex W. Godby

Time-dependent density functional theory (TDDFT) within the linear response regime provides a solid mathematical framework to capture excitations. The accuracy of the theory, however, largely depends on the approximations for the…

Strongly Correlated Electrons · Physics 2023-11-01 Aaron D. Kaplan , Adrienn Ruzsinszky