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Electronic structure calculation of atoms and molecules, in the past few decades has largely been dominated by density functional methods. This is primarily due to the fact that this can account for electron correlation effects in a…

Chemical Physics · Physics 2013-07-12 Amlan K. Roy

DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

Chemical Physics · Physics 2022-03-15 Eunji Sim , Suhwan Song , Stefan Vuckovic , Kieron Burke

Warm dense matter (WMD) describes an intermediate phase, between condensed matter and classical plasmas, found in natural and man-made systems. In a laboratory setting, WDM needs to be created dynamically. It is typically laser or…

Plasma Physics · Physics 2022-03-14 Alexander J. White , Lee A. Collins , Katarina Nichols , S. X. Hu

In this paper, we investigate the energy minimization model of the ensemble Kohn-Sham density functional theory for metallic systems, in which a pseudo-eigenvalue matrix and a general smearing approach are involved. We study the invariance…

Numerical Analysis · Mathematics 2022-01-19 Xiaoying Dai , Stefano de Gironcoli , Bin Yang , Aihui Zhou

A stochastic approach to time-dependent density functional theory (TDDFT) is developed for computing the absorption cross section and the random phase approximation (RPA) correlation energy. The core idea of the approach involves…

Chemical Physics · Physics 2016-11-04 Yi Gao , Daniel Neuhauser , Roi Baer , Eran Rabani

Kohn-Sham density functional theory (KS-DFT) is a powerful method to obtain key materials' properties, but the iterative solution of the KS equations is a numerically intensive task, which limits its application to complex systems. To…

Materials Science · Physics 2023-05-29 Bruno Focassio , Michelangelo Domina , Urvesh Patil , Adalberto Fazzio , Stefano Sanvito

Time-dependent density functional theory (TDDFT) is rapidly emerging as a premier method for solving dynamical many-body problems in physics and chemistry. The mathematical foundations of TDDFT are established through the formal existence…

Quantum Physics · Physics 2014-08-22 J. D. Whitfield , M. -H. Yung , D. G. Tempel , S. Boixo , A. Aspuru-Guzik

We propose hybrid schemes incorporating exact exchange into thermally-assisted-occupation density functional theory (TAO-DFT) [J.-D. Chai, J. Chem. Phys. 136, 154104 (2012)] for an improved description of nonlocal exchange effects. With a…

Chemical Physics · Physics 2017-01-24 Jeng-Da Chai

We present a method to invert a given density and find the Kohn-Sham (KS) potential in Density Functional Theory (DFT) which shares that density. Our method employs the concept of screening density, which is naturally constrained by the…

Chemical Physics · Physics 2020-05-05 Timothy J. Callow , Nektarios N. Lathiotakis , Nikitas I. Gidopoulos

Linear-response time-dependent density functional theory (LR-TDDFT) simulations of disordered extended systems require averaging over different snapshots of ion configurations to minimize finite size effects due to the snapshot--dependence…

Computational Physics · Physics 2023-07-19 Zhandos A. Moldabekov , Jan Vorberger , Mani Lokamani , Tobias Dornheim

Accurately modeling dense plasmas over wide ranging conditions of pressure and temperature is a grand challenge critically important to our understanding of stellar and planetary physics as well as inertial confinement fusion. In this work,…

Linear scaling density functional theory approaches to electronic structure are often based on the tendency of electrons to localize even in large atomic and molecular systems. However, in many cases of actual interest, for example in…

Chemical Physics · Physics 2022-03-25 Marcel David Fabian , Ben Shpiro , Roi Baer

In this study, we propose a quantum-classical hybrid scheme for performing orbital-free density functional theory (OFDFT) using probabilistic imaginary-time evolution (PITE), designed for the era of fault-tolerant quantum computers (FTQC),…

Quantum Physics · Physics 2024-07-24 Yusuke Nishiya , Hirofumi Nishi , Taichi Kosugi , Yu-ichiro Matsushita

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

A generating coordinate is introduced into the exchange-correlation functional of density-functional theory (DFT). The many-body wave function is represented as a superposition of Kohn-Sham (KS) Slater determinants arising from different…

Materials Science · Physics 2009-11-07 K. Capelle

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

Local density approximation (LDA) to the density functional theory (DFT) has continuous derivative of total energy as a number of electrons function and continuous exchange-correlation potential, while in exact DFT both should be…

Strongly Correlated Electrons · Physics 2010-06-28 V. I. Anisimov , A. V. Kozhevnikov , M. A. Korotin , A. V. Lukoyanov , D. A. Khafizullin

Standard density functional approximations often give questionable results for odd-electron radical complexes, with the error typically attributed to self-interaction. In density corrected density functional theory (DC-DFT), certain classes…

Chemical Physics · Physics 2015-06-19 Min-Cheol Kim , Eunji Sim , Kieron Burke

We introduce a spectral density functional theory which can be used to compute energetics and spectra of real strongly--correlated materials using methods, algorithms and computer programs of the electronic structure theory of solids. The…

Strongly Correlated Electrons · Physics 2009-11-10 S. Y. Savrasov , G. Kotliar

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