相关论文: Strongly localised molecular orbitals for $\alpha$…

Quantum-chemical multi-configurational methods are required for a proper description of static electron correlation, a phenomenon inherent to the electronic structure of molecules with multiple (near-)degenerate frontier orbitals. Here, we…

We present a natural orbital-based implementation of the intermediate Hamiltonian Fock space coupled-cluster method for (1,1) sector of Fock space. The use of natural orbital significantly reduces the computational cost and can…

We demonstrate how to determine numerically nearly exact orthonormal orbitals that are optimal for evaluation of the energy of arbitrary (correlated) states of atoms and molecules by minimization of the energy Lagrangian. Orbitals are…

We present a general formula for the tight-binding representation of momentum matrix elements needed for calculating the conductivity based on the Kubo-Greenwood formula using atomic orbitals, which are in general not orthogonal to other…

Here, we investigate the fractal-lattice Hubbard model using various numerical methods: exact diagonalization, the self-consistent diagonalization of a (mean-field) Hartree-Fock Hamiltonian and state-of-the-art Auxiliary-Field Quantum Monte…

It is shown that four-component (4C), quasi-four-component (Q4C), and exact two-component (X2C) relativistic Hartree-Fock (HF) equations can be implemented in an unified manner, by making use of the atomic nature of the small components of…

Density functional theory with plane-wave basis sets is widely employed in computational materials science, including applications to isolated molecular systems. However, the inadequate description of electron correlation remains a…

We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…

We have performed Linearized Augmented Plane Wave (LAPW) calculations for five crystal structures (alpha, dhcp, sc, fcc, bcc) of Boron which we then fitted to a non-orthogonal tight-binding model following the Naval Research Laboratory…

Natural orbitals, defined in electronic structure and quantum chemistry as the (molecular) orbitals diagonalizing the one-particle reduced density matrix of the ground state, have been conjectured for decades to be the perfect reference…

We use a novel approach to analyze the one dimensional spinless Falicov-Kimball model. We derive a simple effective model for the occupation of the localized orbitals which clearly reveals the origin of the known ordering. Our study is…

The series expansion formulae are established for the one- and two-center charge densities over complete orthonormal sets of exponential type orbitals introduced by the author. Three-center overlap integrals of appearing in these relations…

We use first-principles computational methods to examine hole trapping in organic molecular crystals. We present a computational scheme based on the tuning of the fraction of exact exchange in hybrid density functional theory to eliminate…

Perturbative approaches are methods to efficiently tackle many-body problems, offering both intuitive insights and analysis of correlation effects. However, their application to systems where light and matter are strongly coupled is…

Localized orbital-based quantum embedding, as originally formulated in the context of density matrix embedding theory (DMET), is revisited from the perspective of lattice density functional theory (DFT). An in-principle exact (in the sense…

Localized orbital coupled cluster theory has recently emerged as an nonempirical alternative to DFT for large systems. Intuitively, one might expect such methods to perform less well for highly delocalized systems. In the present work, we…

We present an efficient scheme for accurate electronic structure interpolations based on the systematically improvable optimized atomic orbitals. The atomic orbitals are generated by minimizing the spillage value between the atomic basis…

We study a one-dimensional quantum system with an arbitrary number of hard-core particles on the lattice, which are subject to a deterministic attractive interaction as well as a random potential. Our choice of interaction is suggested by…

We are reinvestigating the hyperfine structure of sodium using a fully relativistic multiconfiguration approach. In the fully relativistic approach, the computational strategy somewhat differs from the original nonrelativistic counterpart…

In the present work, we investigate the computational efficiency afforded by higher-order finite-element discretization of the saddle-point formulation of orbital-free density functional theory. We first investigate the robustness of viable…