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A new density functional theory (DFT) exchange-correlation functional for the exploration of reaction mechanisms is proposed. This new functional, denoted BMK (Boese-Martin for Kinetics), has an accuracy in the 2 kcal/mol range for…

Chemical Physics · Physics 2007-05-23 A. Daniel Boese , Jan M. L. Martin

This work presents the formalism and implementation of excited state nuclear forces within density functional linear response theory (TDDFT) using a plane wave basis set. An implicit differentiation technique is developed for computing…

Other Condensed Matter · Physics 2009-11-11 Nikos L. Doltsinis , D. S. Kosov

We extend ground-state density-functional theory to excited states and provide the theoretical formulation for the widely used $\Delta SCF$ method for calculating excited-state energies and densities. As the electron density alone is…

Chemical Physics · Physics 2024-03-08 Weitao Yang , Paul W. Ayers

Excitation energies of light-emitting organic conjugated polymers have been investigated with time-dependent density functional theory (TDDFT) within the adiabatic approximation for the dynamical exchange-correlation potential. Our…

Materials Science · Physics 2009-07-06 Jianmin Tao , Sergei Tretiak , Jian-Xin Zhu

Kohn-Sham density functional theory (DFT) has long struggled with the accurate description of strongly correlated and open shell systems and improvements have been minor even in the newest hybrid functionals. In this Letter we treat the…

Chemical Physics · Physics 2021-04-01 Danny Gibney , Jan-Niklas Boyn , David A. Mazziotti

We analyze the various approaches to construct exchange-correlation functionals which are able to describe states of definite spin multiplicity in the DFT realm and outline the characteristics of possible functionals consistent with the…

Chemical Physics · Physics 2019-01-04 A. L. Tchougréeff , J. G. Ángyán

Density functional theory (DFT) is shown to provide a novel conceptual and computational framework for entanglement in interacting many-body quantum systems. DFT can, in particular, shed light on the intriguing relationship between quantum…

Quantum Physics · Physics 2009-11-11 L. -A. Wu , M. S. Sarandy , D. A. Lidar , L. J. Sham

We present a modification of the $\Delta$SCF method of calculating energies of excited states, in order to make it applicable to resonance calculations of molecules adsorbed on metal surfaces, where the molecular orbitals are highly…

Materials Science · Physics 2009-03-06 Jeppe Gavnholt , Thomas Olsen , Mads Engelund , Jakob Schiøtz

We present calculated, electronic and related properties of wurtzite cadmium sulfide (w-CdS). Our ab-initio, non-relativistic calculations employed a local density functional approximation (LDA) potential and the linear combination of…

Materials Science · Physics 2015-03-17 E. C. Ekuma , L. Franklin , G. L. Zhao , J. T. Wang , D. Bagayoko

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

Development of the electronic kinetic-energy density functional is a subject of major interest in theoretical physics and chemistry. In this work, the nonlocal kinetic-energy functional is developed in terms of the response function for the…

Chemical Physics · Physics 2022-06-17 Hideaki Takahashi

Within the framework of ab initio time-dependent density-functional theory (TD-DFT), we propose a static approximation to the exchange-correlation kernel based on the jellium-with-gap model. This kernel accounts for electron-hole…

A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…

Computational Physics · Physics 2022-11-09 Aleksei V. Ivanov , Gianluca Levi , Elvar Ö. Jónsson , Hannes Jónsson

We construct and apply an exchange-correlation functional for the one-dimensional Hubbard model. This functional has built into it the Luttinger-liquid and Mott-insulator correlations, present in the Hubbard model, in the same way in which…

Strongly Correlated Electrons · Physics 2007-05-23 K. Capelle , N. A. Lima , M. F. Silva , L. N. Oliveira

We present a time-dependent density functional theory (TDDFT) based approach to compute the light-matter couplings between two different manifolds of excited states relative to a common ground state. These quantities are the necessary…

Density functional theory (DFT) has emerged as one of the most versatile and lucrative approaches in electronic structure calculations of many-electron systems in past four decades. Here we give an account of the development of a…

Chemical Physics · Physics 2019-04-19 Abhisek Ghosal , Amlan K. Roy

Gross-Oliveira-Kohn density-functional theory (GOK-DFT) is an extension of DFT to excited states where the basic variable is the ensemble density, i.e. the weighted sum of ground- and excited-state densities. The ensemble energy (i.e. the…

Strongly Correlated Electrons · Physics 2018-07-17 Killian Deur , Laurent Mazouin , Bruno Senjean , Emmanuel Fromager

Density functional theory (DFT) and beyond-DFT methods are often used in combination with photoelectron spectroscopy to obtain physical insights into the electronic structure of molecules and solids. The Kohn-Sham eigenvalues are not…

Ensemble Density Functional Theory (EDFT) is a generalization of ground-state Density Functional Theory (GS DFT), which is based on an exact formal theory of finite collections of a system's ground and excited states. EDFT in various forms…

Materials Science · Physics 2024-08-27 Remi J. Leano , Aurora Pribram-Jones , David A. Strubbe

In this chapter, we provide a review of ground-state Kohn-Sham density-functional theory of electronic systems and some of its extensions, we present exact expressions and constraints for the exchange and correlation density functionals,…

Chemical Physics · Physics 2022-09-12 Julien Toulouse