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Orbital-free density functional theory promises to deliver linear-scaling electronic structure calculations. This requires the knowledge of the non-interacting kinetic-energy density functional (KEDF), which should be accurate and must…

Materials Science · Physics 2024-12-12 Michael A. J. Mitchell , Teresa Del Aguila Ferrandis , Stefano Sanvito

Dyson orbitals play an important role in understanding quasi-particle effects in the correlated ground state of a many-particle system and are relevant for describing the Compton scattering cross section beyond the frameworks of the impulse…

Materials Science · Physics 2007-10-11 B. Barbiellini , A. Bansil

Exchange-correlation potentials vxc and energy densities exc are derived for integer and fractional electron counts using an orbital-averaged Kohn-Sham inversion procedure. The reference densities for inversion come from full configuration…

Chemical Physics · Physics 2025-04-30 Vaibhav Khanna , Bikash Kanungo , Jeffrey Hatch , Joshua Kammeraad , Paul M. Zimmerman

Recently, we have proposed the adaptive local basis set for electronic structure calculations based on Kohn-Sham density functional theory in a pseudopotential framework. The adaptive local basis set is efficient and systematically…

Computational Physics · Physics 2015-10-23 Gaigong Zhang , Lin Lin , Wei Hu , Chao Yang , John E. Pask

Methods for calculating an electron density of a periodic crystal constructed using non-orthogonal localised orbitals are discussed. We demonstrate that an existing method based on the matrix expansion of the inverse of the overlap matrix…

Computational Physics · Physics 2009-11-10 Lev Kantorovich , Oleh Danyliv

We introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using…

Recently, an approximate theoretical framework was introduced, called local reduced density matrix functional theory (local-RDMFT), where functionals of the one-body reduced density matrix (1-RDM) are minimized under the additional…

In practical implementations of density-functional theory, the only term where an orbital description is needed is the kinetic one. Even this term in principle depends on the density only, but its explicit form is unknown. We provide a…

Materials Science · Physics 2007-05-23 L. De Santis , R. Resta

We derive a non-empirical, orbital-free density functional for the total energy of interacting electrons in two dimensions. The functional consists of a local formula for the interaction energy, where we follow the lines introduced by Parr…

Strongly Correlated Electrons · Physics 2009-10-09 S. Pittalis , E. Rasanen

We introduce affordable computational strategies for calculating orbital and pair-orbital energies in atomic and molecular systems. Our methods are based on the pair Coupled Cluster Doubles (pCCD) ansatz and its orbital-optimized variant.…

Chemical Physics · Physics 2025-02-06 Seyedehdelaram Jahani , Somayeh Ahmadkhani , Katharina Boguslawski , Paweł Tecmer

We present an Augmented Lagrangian formulation and its real-space implementation for non-periodic orbital-free Density Functional Theory (OF-DFT) calculations. In particular, we rewrite the constrained minimization problem of OF-DFT as a…

Computational Physics · Physics 2015-06-19 Phanish Suryanarayana , Deepa Phanish

The energy minimization involved in density functional calculations of electronic systems can be carried out using an exponential transformation that preserves the orthonormality of the orbitals. The energy of the system is then represented…

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

We show that using complex, spin-restricted orbitals (cR) in Kohn-Sham density functional theory (KS-DFT) allows one to access a new class of densities that is not accessible by either spin-restricted (RKS) or spin-unrestricted (UKS)…

Chemical Physics · Physics 2019-09-13 Joonho Lee , Luke W. Bertels , Martin Head-Gordon

We report a direct scheme calculation of kinetic energy functional derivative using Machine Learning. Support Vector Regression and Kernel Ridge Regression techniques were independently employed to estimate the kinetic energy functional and…

Computational Physics · Physics 2021-03-16 H. Saidaoui , S. Kais , S. Rashkeev , FH. Alharbi

Electron density prediction stands as a cornerstone challenge in molecular systems, pivotal for various applications such as understanding molecular interactions and conducting precise quantum mechanical calculations. However, the scaling…

Chemical Physics · Physics 2024-10-10 Ilan Mitnikov , Joseph Jacobson

Methods of the explicitly correlated F12 approach are applied to the problem of calculating the uncoupled second-order dispersion energy in symmetry-adapted perturbation theory. The accuracy of the new method is tested for noncovalently…

Chemical Physics · Physics 2018-05-15 Michal Przybytek

Variational quantum eigensolver ans\"atze hold considerable promise for ground-state energy calculations on near-term quantum hardware, yet most promising ansatz designs currently strongly depend on how well the molecular orbital basis…

A conceptual difficulty in formulating the density functional theory of the fractional quantum Hall effect is that while in the standard approach the Kohn-Sham orbitals are either fully occupied or unoccupied, the physics of the fractional…

Strongly Correlated Electrons · Physics 2017-05-12 Jianyun Zhao , Manisha Thakurathi , Manish Jain , Diptiman Sen , J. K. Jain

We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…

Chemical Physics · Physics 2015-06-23 Ralph Gebauer , Morrel H. Cohen , Roberto Car

We present a $\Delta$-machine learning model for obtaining Kohn-Sham accuracy from orbital-free density functional theory (DFT) calculations. In particular, we employ a machine learned force field (MLFF) scheme based on the kernel method to…

Chemical Physics · Physics 2023-10-11 Shashikant Kumar , Xin Jing , John E. Pask , Andrew J. Medford , Phanish Suryanarayana
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