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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

An O(N) algorithm is proposed for calculating linear response functions of non-interacting electrons in arbitray potential. This algorithm is based on numerical solution of the time-dependent Schroedinger equation discretized in space, and…

Condensed Matter · Physics 2009-10-30 Toshiaki Iitaka , Shintaro Nomura , Hideki Hirayama , Xinwei Zhao , Yoshinobu Aoyagi , Takuo Sugano

Natural orbital functional (NOF) theory offers a promising approach for studying strongly correlated systems at an affordable computational cost, with an accuracy comparable to highly demanding wavefunction-based methods. However, its…

Strongly Correlated Electrons · Physics 2025-01-31 Juan Felipe Huan Lew-Yee , Jorge M. del Campo , Mario Piris

We demonstrate that, rather than resorting to high-cost dynamic correlation methods, qualitative failures in excited-state potential energy surface predictions can often be remedied at no additional cost by ensuring that optimal molecular…

Chemical Physics · Physics 2020-06-18 Lan Nguyen Tran , Eric Neuscamman

Due to efficient scaling with electron number N, density functional theory (DFT) is widely used for studies of large molecules and solids. Restriction of an exact mean-field theory to local potential functions has recently been questioned.…

Other Condensed Matter · Physics 2015-06-24 Robert K. Nesbet

We investigate the suitability of natural orbitals as a basis for describing many-body excitations. We analyze to which extend the natural orbitals describe both bound as well as ionized excited states and show that depending on the…

Other Condensed Matter · Physics 2011-01-14 N. Helbig , I. V. Tokatly , A. Rubio

The nuclear many-body problem for medium-mass systems is commonly addressed using wave-function expansion methods that build upon a second-quantized representation of many-body operators with respect to a chosen computational basis. While…

Nuclear Theory · Physics 2021-02-02 J. Hoppe , A. Tichai , M. Heinz , K. Hebeler , A. Schwenk

We have derived orbital basis sets from scattering theory. They are expressed as polynomial approximations to the energy dependence of a set of partial waves, in quantized form. The corresponding matrices, as well as the Hamiltonian and…

Condensed Matter · Physics 2009-10-31 O. K. Andersen , T. Saha-Dasgupta

We present a new linear scaling method for the energy minimization step of semiempirical and first-principles Hartree-Fock and Kohn-Sham calculations. It is based on the self-consistent calculation of the optimum localized orbitals of any…

Materials Science · Physics 2009-11-10 Luis Seijo , Zoila Barandiaran

Variational optimization of orbitals in time-independent density functional calculations of excited electronic states presents a significant challenge, as excited states typically correspond to saddle points on the electronic energy…

Chemical Physics · Physics 2026-04-02 Yorick L. A. Schmerwitz , Elli Selenius , Gianluca Levi

This chapter provides a comprehensive review of fundamental concepts related to approximate natural orbital functionals (NOFs), emphasizing their significance in quantum chemistry and physics. Focusing on fermions, the discussion excludes…

Chemical Physics · Physics 2023-12-13 Mario Piris

We present a real-space formulation and higher-order finite-difference implementation of periodic Orbital-free Density Functional Theory (OF-DFT). Specifically, utilizing a local reformulation of the electrostatic and kernel terms, we…

Computational Physics · Physics 2015-12-23 Swarnava Ghosh , Phanish Suryanarayana

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

Orbital-free density functional theory (OF-DFT) provides an alternative approach for calculating the molecular electronic energy, relying solely on the electron density. In OF-DFT, both the ground-state density is optimized variationally to…

Chemical Physics · Physics 2023-11-23 Alexandre de Camargo , Ricky T. Q. Chen , Rodrigo A. Vargas-Hernández

We prove the general chemical potential theorem: the noninteracting one-electron orbital energies in DFT ground states and $\Delta$SCF excited states are corresponding chemical potentials of electron addition or removal, from an…

Chemical Physics · Physics 2024-08-20 Weitao Yang , Yichen Fan

In the recent work of S. Sharma \emph{et al.}, (arxiv.org: arxiv:0912.1118), a single-electron spectrum associated with the natural orbitals was defined as the derivative of the total energy with respect to the occupation numbers at half…

Chemical Physics · Physics 2012-03-07 E. N. Zarkadoula , S. Sharma , J. K. Dewhurst , E. K. U. Gross , N. N. Lathiotakis

We develop a technique for generating a set of optimized local basis functions to solve models in the Kohn-Sham density functional theory for both insulating and metallic systems. The optimized local basis functions are obtained by solving…

Computational Physics · Physics 2015-05-30 Lin Lin , Jianfeng Lu , Lexing Ying , E. Weinan

We present and motivate an efficient way to include orbital dependent many--body correlations in trial wave function of real--space Quantum Monte Carlo methods for use in electronic structure calculations. We apply our new…

Computational Physics · Physics 2019-10-17 Markus Holzmann , Saverio Moroni

The grand potential of a system of interacting electrons is considered as a stationary point of a self-energy functional. It is shown that a rigorous evaluation of the functional is possible for self-energies that are representable within a…

Strongly Correlated Electrons · Physics 2009-11-10 Michael Potthoff

Determination of \emph{optimal} arrangements of $N$ particles on a sphere is a well-known problem in physics. A famous example of such is the Thomson problem of finding equilibrium configurations of electrical charges on a sphere. More…

Computational Physics · Physics 2019-11-06 Wesley J. M. Ridgway , Alexei F. Cheviakov