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Density-potential functional theory (DPFT) is an alternative formulation of orbital-free density functional theory that may be suitable for modeling the electronic structure of large systems. To date, DPFT has been applied mainly to quantum…

Materials Science · Physics 2023-04-21 Martin-Isbjörn Trappe , William C. Witt , Sergei Manzhos

We extend to strongly correlated molecular systems the recently introduced basis-set incompleteness correction based on density-functional theory (DFT) [E. Giner et al., J. Chem. Phys. 149, 194301 (2018)]. This basis-set correction relies…

Chemical Physics · Physics 2020-05-20 Emmanuel Giner , Anthony Scemama , Pierre-François Loos , Julien Toulouse

We present a novel implementation of the complete active space self-consistent field (CASSCF) method that makes use of the many-body expanded full configuration interaction (MBE-FCI) method to incrementally approximate electronic structures…

The semistochastic heat-bath configuration interaction (SHCI) method is a selected configuration interaction plus perturbation theory method that has provided near-full configuration interaction (FCI) levels of accuracy for many systems…

Chemical Physics · Physics 2021-11-30 Yuan Yao , Emmanuel Giner , Tyler A. Anderson , Julien Toulouse , C. J. Umrigar

Density functional theory (DFT) is the most promising method for calculating quantum properties of molecules and materials at moderate and large scales. However, commonly used density functional approximations (DFAs) have systematic…

Chemical Physics · Physics 2026-03-24 Yichen Fan , Jacob Z. Williams , Weitao Yang

Orbital-free density functional theory (OF-DFT) runs at low computational cost that scales linearly with the number of simulated atoms, making it suitable for large-scale material simulations. It is generally considered that OF-DFT strictly…

Materials Science · Physics 2022-04-05 Qiang Xu , Cheng Ma , Wenhui Mi , Yanchao Wang , Yanming Ma

Fermi operator expansion (FOE) methods are powerful alternatives to diagonalization type methods for solving Kohn-Sham density functional theory (KSDFT). One example is the pole expansion and selected inversion (PEXSI) method, which…

Computational Physics · Physics 2017-10-25 Weile Jia , Lin Lin

The implementation of an efficient self-consistent field (SCF) method including both scalar relativistic effects and spin-orbit interaction in density functional theory (DFT) is presented. We make use of Gaussian-type orbitals (GTOs) and…

Chemical Physics · Physics 2024-05-03 Yannick J. Franzke , Werner M. Schosser , Fabian Pauly

The energy and analytic gradient are developed for FMO combined with the Hartree-Fock method augmented with three empirical corrections (HF-3c). The auxiliary basis set approach to FMO is extended to perform pair interaction energy…

Chemical Physics · Physics 2018-08-01 Dmitri G. Fedorov , Jimmy C. Kromann , Jan H. Jensen

We introduce a size-consistent and orbital-invariant formalism for constructing correlation functionals based on the adiabatic connection for density functional theory (DFT). By constructing correlation energy matrices for the weak and…

Chemical Physics · Physics 2025-11-05 Kyle Bystrom , Timothy C. Berkelbach

We showcase the advantages of orbital-free density-potential functional theory (DPFT), a more flexible variant of Hohenberg-Kohn density functional theory. DPFT resolves the usual trouble with the gradient-expanded kinetic energy functional…

Quantum Gases · Physics 2021-06-16 Martin-Isbjörn Trappe , Jun Hao Hue , Berthold-Georg Englert

In [Phys. Rev. Lett. 128, 013001 (2022)] a novel ground state method was proposed. It has been suggested that this $i$-DMFT would be a method within one-particle reduced density matrix functional theory (DMFT), capable of describing…

Quantum Physics · Physics 2022-02-14 Lexin Ding , Julia Liebert , Christian Schilling

The accurate resolution of the chemical properties of strongly correlated systems, such as biradicals, requires the use of electronic structure theories that account for both multi-reference as well as dynamic correlation effects. A variety…

Chemical Physics · Physics 2023-01-03 Jan-Niklas Boyn , David A. Mazziotti

The Perdew-Zunger(PZ) self-interaction correction (SIC) was designed to correct the one-electron limit of any approximate density functional for the exchange-correlation (xc) energy, while yielding no correction to the exact functional.…

Accurate prediction of spin-state energy difference is crucial for understanding the spin crossover (SCO) phenomena and is very challenging for the density functional approximations, especially for the local and semi-local approximations,…

Chemical Physics · Physics 2023-02-22 Selim Romero , Tunna Baruah , Rajendra R. Zope

Precisely measuring molecular orientation is key to understanding how molecules organize and interact in soft matter, but the maximum theoretical limit of measurement precision has yet to be quantified. We use quantum estimation theory and…

Optics · Physics 2020-07-23 Oumeng Zhang , Matthew D. Lew

Many modern semiempirical molecular orbital models are built on the neglect of diatomic differential overlap (NDDO) approximation. An in-depth understanding of this approximation is therefore indispensable to rationalize the success of…

Chemical Physics · Physics 2018-10-30 Tamara Husch , Markus Reiher

We introduce 1-RDMFT in the canonical ensemble and then proceed to approximate the interacting ensemble by a non-interacting ensemble that maximizes the entropy, independently of temperature. Bosonic and Fermionic Sinkhorn algorithms are…

Chemical Physics · Physics 2022-05-31 Derk P. Kooi

Interacting one-dimensional quantum systems play a pivotal role in physics. Exact solutions can be obtained for the homogeneous case using the Bethe ansatz and bosonisation techniques. However, these approaches are not applicable when…

Quantum Physics · Physics 2016-07-12 M. E. S. Andersen , A. S. Dehkharghani , A. G. Volosniev , E. J. Lindgren , N. T. Zinner

Density fitting (DF), also known as the resolution of the identity (RI), is a widely used technique in quantum chemical calculations with various types of atomic basis sets - Gaussian-type orbitals, Slater-type orbitals, as well as…

Chemical Physics · Physics 2021-12-22 Susi Lehtola
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