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Using the optimized effective potential method in conjunction with the semi-analytical approximation due to Krieger, Li and Iafrate, we have performed fully self-consistent exact exchange-only density-functional calculations for diatomic…

chem-ph · Physics 2008-02-03 T. Grabo , E. K. U. Gross

We present a computationally efficient approach to perform systematically convergent real-space all-electron Kohn-Sham DFT calculations for solids using an enriched finite element (FE) basis. The enriched FE basis is constructed by…

Computational Physics · Physics 2021-08-18 Nelson D. Rufus , Bikash Kanungo , Vikram Gavini

We propose a quantum-classical hybrid variational algorithm, the quantum orbital minimization method (qOMM), for obtaining the ground state and low-lying excited states of a Hermitian operator. Given parameterized ansatz circuits…

Chemical Physics · Physics 2022-06-14 Joel Bierman , Yingzhou Li , Jianfeng Lu

We develop a generalization of the Kohn-Sham density functional theory (KS-DFT) + Hubbard $U$ (DFT+$U$) method to the excited-state regime. This has the form of Hubbard $U$ corrected linear-response time-dependent DFT, or `TDDFT+$U$'.…

Strongly Correlated Electrons · Physics 2019-04-24 Okan K. Orhan , David D. O'Regan

We develop a stochastic formulation of the optimally-tuned range-separated hybrid density functional theory which enables significant reduction of the computational effort and scaling of the non-local exchange operator at the price of…

Chemical Physics · Physics 2016-09-28 Daniel Neuhauser , Eran Rabani , Yael Cytter , Roi Baer

Solving the Euler equation which corresponds to the energy minimum of a density functional expressed in orbital-free form involves related but distinct computational challenges. One is the choice between all-electron and pseudo-potential…

Materials Science · Physics 2015-05-30 V. V. Karasiev , S. B. Trickey

We present an ``orbital'' free density functional theory for computing the quantum ground state of atomic clusters and liquids. Our approach combines the Bohm hydrodynamical description of quantum mechanics with an information theoretical…

Soft Condensed Matter · Physics 2016-08-31 Sean W. Derrickson , Eric R. Bittner

The optimized effective potential (OEP) is the exact Kohn-Sham potential for explicitly orbital-dependent energy functionals, e.g., the exact exchange energy. We give a proof for the OEP equation which does not depend on the chain rule for…

Materials Science · Physics 2009-11-10 Stephan Kümmel , John P. Perdew

We have developed and implemented a self-consistent density functional method using standard norm-conserving pseudopotentials and a flexible, numerical LCAO basis set, which includes multiple-zeta and polarization orbitals. Exchange and…

This paper derives and demonstrates a new, purely density-based ab initio approach for calculation of the energies and properties of many-electron systems. It is based upon the discovery of relationships that govern the "mechanics" of the…

Chemical Physics · Physics 2024-09-04 James C. Ellenbogen

The density-functional approach to quantum electrodynamics is extending traditional density-functional theory and opens the possibility to describe electron-photon interactions in terms of effective Kohn-Sham potentials. In this work, we…

Quantum Physics · Physics 2016-02-17 Johannes Flick , Michael Ruggenthaler , Heiko Appel , Angel Rubio

Accurate and efficient simulation of excited state properties is an important and much aspired cornerstone in the study of adsorbate dynamics on metal surfaces. To this end, the recently proposed linear expansion \Delta Self-Consistent…

Materials Science · Physics 2013-07-23 Reinhard J. Maurer , Karsten Reuter

Orbital-free density functional theory (OFDFT) offers a challenging way of electronic-structure calculations scaled as $\mathcal{O}(N)$ computation for system size $N$. We here develop a scheme of the OFDFT calculations based on the…

Computational Physics · Physics 2021-09-06 Fumihiro Imoto , Masatoshi Imada , Atsushi Oshiyama

We present excited states density functional theory (DFT) to calculate band gap for semiconductors and insulators. For the excited states exchange-correlation functional, we use a simple local density approximation (LDA) like functional and…

Kohn-Sham density functional theory calculations using conventional diagonalization based methods become increasingly expensive as temperature increases due to the need to compute increasing numbers of partially occupied states. We present…

Chemical Physics · Physics 2022-03-23 Qimen Xu , Xin Jing , Boqin Zhang , John E. Pask , Phanish Suryanarayana

Kohn-Sham Density Functional Theory (KS-DFT) has been traditionally solved by the Self-Consistent Field (SCF) method. Behind the SCF loop is the physics intuition of solving a system of non-interactive single-electron wave functions under…

Density functional theory is currently the most widely applied method in electronic structure theory. The Kohn-Sham method, based on a fictitious system of non-interacting particles, is the work horse of the theory. The particular form of…

Chemical Physics · Physics 2016-06-01 Hubertus J J van Dam

For exchange-correlation functionals that depend explicitly on the Kohn-Sham orbitals, the potential $V_{\mathrm{xc}\sigma}(\re)$ must be obtained as the solution of the optimized effective potential (OEP) integral equation. This is very…

Materials Science · Physics 2009-11-07 Stephan Kümmel , John P. Perdew

Occupation numbers of natural orbitals capture the physics of strong electron correlations in momentum space. A Natural Orbital Density Functional Theory based on the antisymmetrized geminal product provides these occupation numbers and the…

Strongly Correlated Electrons · Physics 2014-05-06 B. Barbiellini

A new, very fast, implementation of the exact (Fock) exchange operator for electronic structure calculations within the plane-wave pseudopotential method is described in detail for both molecular and periodic systems, and carefully…

Materials Science · Physics 2018-12-12 Ivan Carnimeo , Stefano Baroni , Paolo Giannozzi
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