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Localized orbitals are important for modeling and interpreting complicated electronic structures of atoms and molecules in a chemically meaningful way. Here, we present the parameter-free procedure for transforming delocalized molecular…

Chemical Physics · Physics 2018-04-12 Tymofii Yu. Nikolaienko , Leonid A. Bulavin

Recently, we have demonstrated that the problems finding a suitable adiabatic approximation in time-dependent one-body reduced density matrix functional theory can be remedied by introducing an additional degree of freedom to describe the…

Chemical Physics · Physics 2014-03-10 Klaas J. H. Giesbertz , Oleg V. Gritsenko , Evert Jan Baerends

We investigated the reliability and applicability of so-called magnetic force linear response method to calculate spin-spin interaction strengths from first-principles. We examined the dependence on the numerical parameters including the…

Strongly Correlated Electrons · Physics 2018-03-28 Hongkee Yoon , Taek Jung Kim , Jae-Hoon Sim , Seung Woo Jang , Taisuke Ozaki , Myung Joon Han

We present SPARC-atomSFE, a spectral finite-element package for accurate and efficient atomic structure calculations within the framework of Kohn-Sham density functional theory. The package supports both all-electron and norm conserving…

Computational Physics · Physics 2026-05-19 Qihao Cheng , Shubhang Krishnakant Trivedi , Phanish Suryanarayana

We have developed a Scalable Linear Augmented Slater-Type Orbital (LASTO) method for electronic-structure calculations on free-standing atomic clusters. As with other linear methods we solve the Schr\"odinger equation using a mixed basis…

Materials Science · Physics 2008-06-11 K. S. Kang , J. W. Davenport , James Glimm , David Keyes , Michael McGuigan

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

Starting from the observation that one of the most successful methods for solving the Kohn-Sham equations for periodic systems -- the plane-wave method -- is a spectral method based on eigenfunction expansion, we formulate a spectral method…

Computational Physics · Physics 2016-03-08 Amartya S. Banerjee , Ryan S. Elliott , Richard D. James

Creating soft-Coulomb-type (SC) molecular potential within single-active-electron approximation (SAE) is essential since it allows solving time-dependent Schr\"odinger equations with fewer computational resources compared to other…

Chemical Physics · Physics 2024-09-17 Duong D. Hoang-Trong , Khang Tran , Doan-An Trieu , Quan-Hao Truong , Van-Hoang Le , Ngoc-Loan Phan

We present a novel route to constructing cost-efficient semi-empirical approximations for the non-additive kinetic energy in subsystem density functional theory. The developed methodology is based on the use of Slater determinants composed…

Chemical Physics · Physics 2025-01-13 Larissa Sophie Eitelhuber , Denis G. Artiukhin

We propose a lattice density-functional theory for {\it ab initio} quantum chemistry or physics as a route to an efficient approach that approximates the full configuration interaction energy and orbital occupations for molecules with…

Strongly Correlated Electrons · Physics 2019-04-19 J. P. Coe

We develop and analyze a fault-tolerant quantum algorithm for computing $n$-th order response properties necessary for analysis of non-linear spectroscopies of molecular and condensed phase systems. We use a semi-classical description in…

Quantum Physics · Physics 2024-04-23 Tyler Kharazi , Torin F. Stetina , Liwen Ko , Guang Hao Low , K. Birgitta Whaley

It is demonstrated that the reaction path for a polyatomic molecule (applied to the HCO molecule) is easily calculated via ab-initio configuration interaction (CI) total energies. This Hamiltonian not only reproduces the CI calculations…

Chemical Physics · Physics 2007-05-23 N. C. Bacalis , A. Metropoulos , D. A. Papaconstantopoulos

We propose a real-time time-dependent ab__initio approach within a configuration-interaction-singles ansatz to decompose the high-harmonic generation (HHG) signal of molecules in terms of individual molecular-orbital (MO) contributions.…

Chemical Physics · Physics 2025-12-11 Marco Marchetta , Chiara Morassut , Julien Toulouse , Emanuele Coccia , Eleonora Luppi

We introduce a new approach to density functional theory based on kinetic theory, showing that the Kohn-Sham equations can be derived as a macroscopic limit of a suitable Boltzmann kinetic equation in the limit of small mean free path…

Chemical Physics · Physics 2015-06-15 M. Mendoza , S. Succi , H. J. Herrmann

The optical response functions and band structures of LiCoO$_2$ are studied at different levels of approximation, from density functional theory (DFT) in the generalized gradient approximation (GGA) to quasiparticle self-consistent QS$GW$…

Kohn-Sham density functional theory is one of the most widely used electronic structure theories. In the pseudopotential framework, uniform discretization of the Kohn-Sham Hamiltonian generally results in a large number of basis functions…

Numerical Analysis · Mathematics 2015-05-27 Lin Lin , Jianfeng Lu , Lexing Ying , E. Weinan

A two-electron one-dimensional model of a heteroatomic molecule composed of two open-shell atoms is considered. Including only two electrons isolates and examines the effect that the highest occupied molecular orbital has on the Kohn-Sham…

Materials Science · Physics 2010-03-22 David G. Tempel , Todd J. Martinez , Neepa T. Maitra

In the density functional (DF) theory of Kohn and Sham, the kinetic energy of the ground state of a system of noninteracting electrons in a general external field is calculated using a set of orbitals. Orbital free methods attempt to…

Strongly Correlated Electrons · Physics 2009-11-13 Jeng-Da Chai , John D Weeks

Accurate local Kohn-Sham potentials have been constructed for the ground $1s^2 ^1S$ state and, in particular, for the lowest triplet $1s2s ^{3}S$ state of the helium atom, using electron densities from many-body calculations and the…

Atomic Physics · Physics 2016-08-16 I. Lindgren , S. Salomonson , F. Möller

Density functional calculations are performed for twelve $2l2l'$n$l"$ (n$\geq$2) triply excited hollow resonance series of Li, {\em viz.,} 2s$^2$ns $^2$S$^e$, 2s$^2$np $^2$P$^o$, 2s$^2$nd $^2$D$^e$, 2p$^2$ns $^2$D$^e$,$^4$P$^e$, 2s2pns…

Chemical Physics · Physics 2015-06-16 Amlan K. Roy