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Reduced-density-matrix-functional theory is applied to open-shell systems. We introduce a spin-restricted formulation by appropriately expressing approximate correlation-energy functionals in terms of spin-dependent occupation numbers and…

Strongly Correlated Electrons · Physics 2007-05-23 N. N. Lathiotakis , N. Helbig , E. K. U. Gross

We present a novel method for calculating the fundamental gap. To this end, reduced-density-matrix-functional theory is generalized to fractional particle number. For each fixed particle number, $M$, the total energy is minimized with…

Strongly Correlated Electrons · Physics 2009-11-11 N. Helbig , N. N. Lathiotakis , M. Albrecht , E. K. U. Gross

The accurate description of open-shell molecules, in particular of transition metal complexes and clusters, is still an important challenge for quantum chemistry. While density-functional theory (DFT) is widely applied in this area, the…

Chemical Physics · Physics 2012-10-26 Christoph R. Jacob , Markus Reiher

The fundamental gap is a central quantity in the electronic structure of matter. Unfortunately, the fundamental gap is not generally equal to the Kohn-Sham gap of density functional theory (DFT), even in principle. The two gaps differ…

Materials Science · Physics 2015-09-01 Eli Kraisler , Leeor Kronik

We present a broadly-applicable, physically-motivated first-principles approach to determining the fundamental gap of finite systems. The approach is based on using a range-separated hybrid functional within the generalized Kohn-Sham…

Materials Science · Physics 2015-05-19 Tamar Stein , Helen Eisenberg , Leeor Kronik , Roi Baer

Energy gaps are crucial aspects of the electronic structure of finite and extended systems. Whereas much is known about how to define and calculate charge gaps in density-functional theory (DFT), and about the relation between these gaps…

Materials Science · Physics 2015-05-14 K. Capelle , G. Vignale , C. A. Ullrich

We present an approach based on density-functional theory for the calculation of fundamental gaps of both finite and periodic two-dimensional (2D) electronic systems. The computational cost of our approach is comparable to that of total…

Materials Science · Physics 2021-08-11 Alberto Guandalini , Alice Ruini , Esa Räsänen , Carlo Andrea Rozzi , Stefano Pittalis

We decompose the energy error of any variational DFT calculation into a contribution due to the approximate functional and that due to the approximate density. Typically, the functional error dominates, but in many interesting situations,…

Chemical Physics · Physics 2015-06-12 Min-Cheol Kim , Eunji Sim , Kieron Burke

We extend to strongly correlated molecular systems the recently introduced basis-set incompleteness correction based on density-functional theory (DFT) [E. Giner et al., J. Chem. Phys. 149, 194301 (2018)]. This basis-set correction relies…

Chemical Physics · Physics 2020-05-20 Emmanuel Giner , Anthony Scemama , Pierre-François Loos , Julien Toulouse

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

Reduced density matrix functional theory for the case of solids is presented and a new exchange correlation functional based on a fractional power of the density matrix is introduced. We show that compared to other functionals, this…

Materials Science · Physics 2009-11-13 S. Sharma , J. K. Dewhurst , N. N. Lathiotakis , E. K. U. Gross

Orbital-free Density Functional Theory (OF-DFT) has been used when studying atoms, molecules and solids. In nuclear physics, there has been basically no application of OF-DFT so far, as the Density Functional Theory (DFT) has been widely…

Nuclear Theory · Physics 2023-08-03 Gianluca Colo' , Kouichi Hagino

Reduced density-matrix functional theory (RDMFT) is a promising alternative approach to the problem of electron correlation. Like standard density functional theory, it contains an unknown exchange-correlation functional, for which several…

Chemical Physics · Physics 2017-03-03 N. N. Lathiotakis , Miguel A. L. Marques

Electrons in zero external magnetic field can be studied with density functional theory (DFT) or with spin-DFT (SDFT). The latter is normally used for open shell systems because its approximations appear to model better the exchange and…

Chemical Physics · Physics 2022-04-06 Timothy Callow , Benjamin Pearce , Nikitas Gidopoulos

We show that a lattice formulation of density-functional theory (DFT), guided by renormalization-group concepts, can be used to obtain numerical predictions of energy gaps, spin-density profiles, critical exponents, sound velocities,…

Strongly Correlated Electrons · Physics 2009-11-13 Francisco C. Alcaraz , Klaus Capelle

We propose a novel scheme to bring reduced density matrix functional theory (RDMFT) into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately…

Chemical Physics · Physics 2014-11-07 Nektarios N. Lathiotakis , Nicole Helbig , Angel Rubio , Nikitas I. Gidopoulos

The calculation of the band-gap by density-functional theory (DFT) methods is examined by considering the behavior of the energy as a function of number of electrons. It is found that the incorrect band-gap prediction with most approximate…

Materials Science · Physics 2009-11-13 Aron J. Cohen , Paula Mori-Sánchez , Weitao Yang

Density functional theory (DFT) is widely used to predict chemical properties, but its accuracy is limited by functional approximations and their approximate self-consistent densities. Density-corrected DFT (DC-DFT) is the study of the…

Chemical Physics · Physics 2023-07-21 Hayoung Yu , Suhwan Song , Seungsoo Nam , Kieron Burke , Eunji Sim

We prove the existence of the exact density-functional theory formalism for open electronic systems, and develop subsequently an exact time-dependent density-functional theory (TDDFT) formulation for the dynamic response. The TDDFT…

Chemical Physics · Physics 2007-05-23 Xiao Zheng , GuanHua Chen

Density functional theory (DFT) provides a theoretical framework for efficient and fairly accurate calculations of the electronic structure of molecules and crystals. The main features of density functional theory are described and DFT…

Chemical Physics · Physics 2012-06-12 Hauke Paulsen , Alfred Xaver Trautwein
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