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We report the derivation and implementation of orbital optimization algorithms for the active space decomposition (ASD) model, which are extensions of complete active space self-consistent field (CASSCF) and its occupation-restricted…

Chemical Physics · Physics 2015-08-17 Inkoo Kim , Shane M. Parker , Toru Shiozaki

Nuclear matter is studied within the Density Functional Theory (DFT) framework. Our method employs a finite number of nucleons in a box subject to periodic boundary conditions, in order to simulate infinite matter and study its response to…

Nuclear Theory · Physics 2023-04-26 Francesco Marino , Gianluca Colò , Xavier Roca-Maza , Enrico Vigezzi

This work presents a detailed mathematical derivation of the hierarchically correlated orbital functional theory (HCOFT), a framework based on hypercomplex orbitals. Recent study [Phys. Rev. Lett. 133, 206402] has demonstrated that…

Chemical Physics · Physics 2025-03-04 Ting Zhang , Neil Qiang Su

Analytical nuclear gradients for fully internally contracted complete active space second-order perturbation theory (CASPT2) are reported. This implementation has been realized by an automated code generator that can handle spin-free…

Chemical Physics · Physics 2015-02-11 Matthew K. MacLeod , Toru Shiozaki

The occupation of d-orbitals controls the magnitude and anisotropy of the inter-atomic electron transfer in transition metal oxides and hence exerts a key influence on their chemical bonding and physical properties. Atomic-scale modulations…

An energy functional for orbital based $O(N)$ calculations is proposed, which depends on a number of non orthogonal, localized orbitals larger than the number of occupied states in the system, and on a parameter, the electronic chemical…

mtrl-th · Physics 2016-09-07 Jeongnim Kim , Francesco Mauri , Giulia Galli

The isoelectronic series of Be, Ne and Si are investigated using a variational determination of the second-order density matrix. A semidefinite program was developed that exploits all rotational and spin symmetries in the atomic system. We…

Strongly Correlated Electrons · Physics 2009-09-14 Brecht Verstichel , Helen van Aggelen , Dimitri Van Neck , Paul W. Ayers , Patrick Bultinck

We introduce an orbital free electron density functional approximation based on alchemical perturbation theory. Given convergent perturbations of a suitable reference system, the accuracy of popular self-consistent Kohn-Sham density…

Chemical Physics · Physics 2020-05-27 Guido Falk von Rudorff , O. Anatole von Lilienfeld

A detailed exploration of the $f$-atomic orbital occupancy space for UO$_2$ is performed using a first principles approach based on density functional theory (DFT), employing a full hybrid functional within a systematic basis set.…

Strongly Correlated Electrons · Physics 2022-01-05 Laura E. Ratcliff , Luigi Genovese , Hyowon Park , Peter B. Littlewood , Alejandro Lopez-Bezanilla

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

For a large class of variational quantum circuits, we show how arbitrary-order derivatives can be analytically evaluated in terms of simple parameter-shift rules, i.e., by running the same circuit with different shifts of the parameters. As…

Quantum Physics · Physics 2021-03-03 Andrea Mari , Thomas R. Bromley , Nathan Killoran

The ground state of atoms from H to Ar was calculated using a self-interaction correction to local and gradient dependent density functionals. The correction can significantly improve the total energy and makes the orbital energies…

Atomic and Molecular Clusters · Physics 2013-08-29 Simon Klüpfel , Peter Klüpfel , Hannes Jonsson

Here, we report orbital-free density-functional theory (OF DFT) molecular dynamics simulations of the displacement cascade in aluminum. The electronic effect is our main concern. The displacement threshold energies are calculated using OF…

Materials Science · Physics 2017-09-26 Ruizhi Qiu

Scientific studies often require the precise calculation of derivatives. In many cases an analytical calculation is not feasible and one resorts to evaluating derivatives numerically. These are error-prone, especially for higher-order…

High Energy Physics - Phenomenology · Physics 2010-05-28 Mathias Wagner , Andrea Walther , Bernd-Jochen Schaefer

Following a recent work [Gal, Phys. Rev. A 64, 062503 (2001)], a simple derivation of the density-functional correction of the Hartree-Fock equations, the Hartree-Fock-Kohn-Sham equations, is presented, completing an integrated view of…

Chemical Physics · Physics 2008-09-11 Tamas Gal

Describing systems with non-Hermitian (NH) operators remains a challenge in quantum theory due to instabilities (e.g., exceptional points and decoherence) arising from interactions with the environment. We propose a framework to express the…

Quantum Physics · Physics 2025-03-31 Priyanshi Bhasin , Tanmoy Das

New energy-density functionals (EDFs) inspired by effective-field theories (EFTs) have been recently proposed. The present work focuses on three of such functionals which were developed to produce satisfactory equations of state for nuclear…

Nuclear Theory · Physics 2018-09-26 Jérémy Bonnard , Marcella Grasso , Denis Lacroix

Second-order structured deformations of continua provide an extension of the multiscale geometry of first-order structured deformations by taking into account the effects of submacroscopic bending and curving. We derive here an integral…

Optimization and Control · Mathematics 2017-05-24 Ana Cristina Barroso , José Matias , Marco Morandotti , David R. Owen

An explicitly orbital-dependent correlation energy functional is proposed, which is to be used in combination with the orbital-dependent exchange energy functional in energy-band calculations. It bears a close resemblance to the…

Strongly Correlated Electrons · Physics 2009-11-10 Masahiko Higuchi , Hiroshi Yasuhara

When using atom-centered integration grids, the portion of the grid that belongs to a certain atom also moves when this atom is displaced. In the paper, we investigate the moving-grid effect in the calculation of the harmonic vibrational…

Computational Physics · Physics 2020-03-20 Honghui Shang , Jinlong Yang