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Molecule-optimized basis sets, based on approximate natural orbitals, are developed for accelerating the convergence of quantum calculations with strongly correlated (multi-referenced) electrons. We use a low-cost approximate solution of…

Chemical Physics · Physics 2014-02-12 Gergely Gidofalvi , David A. Mazziotti

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 study the long-time self-diffusion of a single conjugated organic para-sexiphenyl (p-6P) molecule physisorbed on the inorganic ZnO $\left(10\overline{1}0\right)$ surface by means of all-atom molecular dynamics computer simulations. We…

Materials Science · Physics 2014-08-20 Karol Palczynski , Joachim Dzubiella

We introduce an efficient finite-element approach for large-scale real-space pseudopotential density functional theory (DFT) calculations incorporating noncollinear magnetism and spin-orbit coupling. The approach, implemented within the…

Materials Science · Physics 2025-06-11 Nikhil Kodali , Phani Motamarri

A new, very fast, implementation of the exact (Fock) exchange operator for electronic structure calculations within the plane-wave pseudopotential method is described in detail for both molecular and periodic systems, and carefully…

Materials Science · Physics 2018-12-12 Ivan Carnimeo , Stefano Baroni , Paolo Giannozzi

An ab initio Wannier-function-based approach to electronic ground-state calculations for crystalline solids is outlined. In the framework of the linear combination of atomic orbitals method the infinite character of the solid is rigorously…

Condensed Matter · Physics 2009-10-31 Martin Albrecht , Alok Shukla , Michael Dolg , Peter Fulde , Hermann Stoll

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

The reliability of the recently proposed natural orbital functional supplemented with second-order M{\o}ller-Plesset calculations, (NOF-MP2), has been assessed for the mechanistic studies of elementary reactions of transition metal…

Chemical Physics · Physics 2020-12-25 Jose M. Mercero , Jesus M. Ugalde , Mario Piris

We present a basis set correction scheme for the coupled-cluster singles and doubles (CCSD) method. The scheme is based on employing frozen natural orbitals (FNOs) and diagrammatically decomposed contributions to the electronic correlation…

Materials Science · Physics 2021-06-18 Andreas Irmler , Alejandro Gallo , Andreas Grüneis

The convergence of self-consistent field equations in mean-field nuclear-electronic orbital methods strongly depends on the choice of initial guesses for quantum nuclei. Although several such guesses have been proposed in the literature, a…

Chemical Physics · Physics 2026-02-18 Denis G. Artiukhin

Variational quantum eigensolvers (VQE) are among the most promising approaches for solving electronic structure problems on near-term quantum computers. A critical challenge for VQE in practice is that one needs to strike a balance between…

We extend the natural orbital impurity solver [PRB 90, 085102 (2014)] to finite temperatures and apply it to calculate spectral and transport properties of correlated electrons within the dynamical mean-field theory. First, we benchmark our…

Strongly Correlated Electrons · Physics 2024-08-23 Motoharu Kitatani , Shiro Sakai , Ryotaro Arita

Approximate natural orbitals are investigated as a way to improve a Monte Carlo configuration interaction (MCCI) calculation. We introduce a way to approximate the natural orbitals in MCCI and test these and approximate natural orbitals…

Chemical Physics · Physics 2013-04-12 J. P. Coe , M. J. Paterson

We compute $\mathcal O(\alpha^2 Z)$ radiative corrections to superallowed $\beta$ decays with a heavy-particle effective field theory that systematically describes the interactions of low-energy ultrasoft photons with nuclei. We calculate…

High Energy Physics - Phenomenology · Physics 2025-11-27 Òscar L. Crosas , Emanuele Mereghetti

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

We propose a local real-space formulation for orbital-free DFT with density dependent kinetic energy functionals and a unified variational framework for computing the configurational forces associated with geometry optimization of both…

Materials Science · Physics 2015-06-15 Sambit Das , Mrinal Iyer , Vikram Gavini

Most widely used density functional approximations suffer from self-interaction (SI) error, which can be corrected using the Perdew-Zunger (PZ) self-interaction correction (SIC). We implement the recently proposed size-extensive formulation…

Chemical Physics · Physics 2021-12-07 Carlos M. Diaz , Phanish Suryanarayana , Qimen Xu , Tunna Baruah , John Pask , Rajendra Zope

The self-consistent field method utilized for solving the Hartree-Fock (HF) problem and the closely related Kohn-Sham problem, is typically thought of as one of the cheapest methods available to quantum chemists. This intuition has been…

Quantum Physics · Physics 2015-06-22 James D. Whitfield , Zoltán Zimborás

We compare three different models of rotating neutron star spacetimes: the Hartle-Thorne (HT) slow-rotation approximation at second order in rotation, the exact analytic vacuum solution of Manko et al. and a numerical solution of the full…

General Relativity and Quantum Cosmology · Physics 2011-05-23 Emanuele Berti , Frances White , Asimina Maniopoulou , Marco Bruni

We identify the dominant computational cost within the recently introduced stochastic and internally contracted FCIQMC-NEVPT2 method for large active space sizes. This arises from the contribution to the four-body intermediates arising from…

Chemical Physics · Physics 2020-10-05 James J. Halson , Robert J. Anderson , George H. Booth