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The alternative separation of exchange and correlation energies proposed by Toulouse et al. [Theor. Chem. Acc. 114, 305 (2005)] is explored in the context of multi-configuration range-separated density-functional theory. The new…

Within the finite-field Kohn-Sham framework, static electric response properties of diatomic molecules are presented. The electronic energy, dipole moment ({\boldmath$\mu$}), static dipole polarizability ({\boldmath$\alpha$}) and…

Chemical Physics · Physics 2019-04-26 Abhisek Ghosal , Tanmay Mandal , Amlan K. ~Roy

In orbital-free density functional theory the kinetic potential (KP), the functional derivative of the kinetic energy density functional, appears in the Euler equation for the electron density and may be more amenable to simple…

Other Condensed Matter · Physics 2015-05-13 Jeng-Da Chai , Vincent L. Ligneres , Gregory Ho , Emily A. Carter , John D. Weeks

The previously proposed ansatz for density cumulant theory that combines orbital-optimization and a parameterization of the 2-electron reduced density matrix cumulant in terms of unitary coupled cluster amplitudes (OUDCT) is carefully…

Chemical Physics · Physics 2020-12-23 Jonathon P. Misiewicz , Justin M. Turney , Henry F. Schaefer , Alexander Yu. Sokolov

We introduce an algorithm, the Orthogonal Operator Polynomial Expansion (OOPEX), to approximately compute expectation values in energy eigenstates at finite energy density of non-integrable quantum many-body systems with polynomial effort,…

Statistical Mechanics · Physics 2021-06-01 Pavan Hosur

We present a Gaussian-basis implementation of orbital-free density-functional theory (OF-DFT) in which the trust-region image method (TRIM) is used for optimization. This second-order optimization scheme has been constructed to provide…

Chemical Physics · Physics 2021-09-15 Matthew S. Ryley , Michael Withnall , Tom J. P. Irons , Trygve Helgaker , Andrew M. Teale

The optimized effective potential method is formulated as a convex minimization problem. This formulation does not require assumptions about $v$-representability nor functional differentiability. The formulation provides a natural framework…

Chemical Physics · Physics 2022-02-01 Erik I. Tellgren , Andre Laestadius , Markus Penz

We test the performance of a number of two- and one-parameter double-hybrid approximations, combining semilocal exchange-correlation density functionals with periodic local second-order M{\o}ller-Plesset (LMP2) perturbation theory, for…

Chemical Physics · Physics 2015-06-22 Kamal Sharkas , Julien Toulouse , Lorenzo Maschio , Bartolomeo Civalleri

We report the implementation of a cost-effective approximation method within the framework of time-dependent optimized coupled-cluster (TD-OCC) method [J. Chem. Phys. 148, 051101 (2018)] for real-time simulations of intense laser-driven…

Chemical Physics · Physics 2020-04-22 Himadri Pathak , Takeshi Sato , Kenichi L. Ishikawa

We present a general numerical approach to construct local Kohn-Sham potentials from orbital-dependent functionals within the all-electron full-potential linearized augmented-plane-wave (FLAPW) method, in which core and valence electrons…

Materials Science · Physics 2011-07-06 Markus Betzinger , Christoph Friedrich , Stefan Blügel , Andreas Görling

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

In this paper, we propose a parallel optimization method for electronic structure calculations based on a single orbital-updating approximation. It is shown by our numerical experiments that the method is efficient and reliable for atomic…

Numerical Analysis · Mathematics 2015-11-20 Xiaoying Dai , Zhuang Liu , Xin Zhang , Aihui Zhou

Low-scaling electron correlation theory based on the pair natural orbital approximation, PNO-CCSD(T), has become a powerful computational tool. Motivated by the recent discovery of large errors for organometallic molecules, we assess the…

Chemical Physics · Physics 2023-10-10 Reka A. Horvath , Kesha Sorathia , Isabelle Saint , David P. Tew

We showcase the advantages of orbital-free density-potential functional theory (DPFT), a more flexible variant of Hohenberg-Kohn density functional theory. DPFT resolves the usual trouble with the gradient-expanded kinetic energy functional…

Quantum Gases · Physics 2021-06-16 Martin-Isbjörn Trappe , Jun Hao Hue , Berthold-Georg Englert

Most approximate exchange-correlation functionals used within density functional theory are constructed as the sum of two distinct contributions for exchange and correlation. Separating the exchange component from the entire functional is…

Condensed Matter · Physics 2009-10-28 Claudia Filippi , C. J. Umrigar , Xavier Gonze

We present an optimized random phase approximation method (optRPA26) that significantly improves upon conventional RPA. The method employs an empirically constructed hybrid functional to generate DFT orbitals to evaluate the RPA correlation…

Chemical Physics · Physics 2026-02-06 Neung-Kyung Yu , Johannes Voss , Andrew J. Medford

A natural orbital functional for electronic systems with any value of the spin is proposed. This energy functional is based on a new reconstruction for the two-particle reduced density matrix (2RDM) of the multiplet, that is, of the mixed…

Chemical Physics · Physics 2019-10-02 Mario Piris

In order for methods combining ab initio density-functional theory and many-body techniques to become routinely used, a flexible, fast, and easy-to-use implementation is crucial. We present an implementation of a general charge…

Arguments showing that exchange-only optimized effective potential (xOEP) methods, with finite basis sets, cannot in general yield the Hartree-Fock (HF) ground state energy, but a higher one, are given. While the orbital products of a…

Chemical Physics · Physics 2007-05-23 Andreas Goerling , Andreas Hesselmann , Martin Jones , Mel Levy

We present a perturbative approach within the scope of Kohn-Sham density functional theory (DFT). The method is based on the exact exchange-only optimized effective potential method, and correlation is included via perturbation expansion…

Chemical Physics · Physics 2007-05-23 P. Sule
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