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A previously proposed computational procedure for constructing a set of nonorthogonal strongly localised one-electron molecular orbitals (O. Danyliv, L. Kantorovich - physics/0401107) is applied to a perfect $\alpha$-quartz crystal…

Chemical Physics · Physics 2009-11-10 Oleh Danyliv , Lev Kantorovich

We present a new linear scaling method for the energy minimization step of semiempirical and first-principles Hartree-Fock and Kohn-Sham calculations. It is based on the self-consistent calculation of the optimum localized orbitals of any…

Materials Science · Physics 2009-11-10 Luis Seijo , Zoila Barandiaran

Spatially localized one-electron orbitals, orthogonal and nonorthogonal, are widely used in electronic structure theory to describe chemical bonding and speed up calculations. In order to avoid linear dependencies of localized orbitals, the…

Chemical Physics · Physics 2020-03-04 Ziling Luo , Rustam Z. Khaliullin

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…

Chemical Physics · Physics 2016-12-04 Ralph Gebauer , Morrel H. Cohen , Roberto Car

With the aim of future applications in quantum mechanical embedding in extended systems such as crystals, we suggest a simple and computationally efficient method which enables construction of a set of nonorthogonal highly localized…

Computational Physics · Physics 2009-11-10 Oleh Danyliv , Lev Kantorovich

Localized molecular orbitals are often used for the analysis of chemical bonds, but they can also serve to efficiently and comprehensibly compute linear response properties. While conventional canonical molecular orbitals provide an…

Chemical Physics · Physics 2023-02-08 Souloke Sen , Bruno Senjean , Lucas Visscher

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…

Chemical Physics · Physics 2021-09-07 Soumi Haldar , Achintya Kumar Dutta

We present a new methodology to analyze complicated multi-physics simulations by introducing a fictitious parameter. Using the method, we study quantum mechanical aspects of an organic molecule in water. The simulation is variationally…

Chaotic Dynamics · Physics 2007-05-23 Toshiya Takami , Jun Maki , Jun-ichi Ooba , Taizo Kobayashi , Rie Nogita , Mutsumi Aoyagi

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

We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…

Chemical Physics · Physics 2015-06-23 Ralph Gebauer , Morrel H. Cohen , Roberto Car

The general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…

Chemical Physics · Physics 2017-03-16 Alain C. Vaucher , Markus Reiher

A Hamiltonian based approach using spatially localized projection operators is introduced to give precise meaning to the chemically intuitive idea of the electronic energy on a quantum subsystem. This definition facilitates the study of…

Quantum Physics · Physics 2015-06-11 Yaser R. Khan , Paul Brumer

A comprehensive theoretical understanding of electron-photon correlation is essential for describing the reshaping of molecular orbitals in quantum electrodynamics (QED) environments. The strong coupling QED Hartree-Fock (SC-QED-HF) theory…

Chemical Physics · Physics 2024-09-04 Yassir El Moutaoukal , Rosario R. Riso , Matteo Castagnola , Henrik Koch

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

Energy decomposition analysis (EDA) based on absolutely localized molecular orbitals provides detailed insights into intermolecular bonding by decomposing the total molecular binding energy into physically meaningful components. Here, we…

Chemical Physics · Physics 2025-09-25 Hossein Tahmasbi , Michael Beerbaum , Bartosz Brzoza , Attila Cangi , Thomas D. Kühne

An approximation to the many-body London dispersion energy in molecular systems is expressed as a functional of the occupied orbitals only. The method is based on the local-RPA theory. The occupied orbitals are localized molecular orbitals…

Chemical Physics · Physics 2015-12-25 Bastien Mussard , Janos Angyan

A new electronic structure model is developed in which the ground state energy of a molecular system is given by a Hartree-Fock-like expression with parametrized one- and two-electron integrals over an extended (minimal + polarization) set…

Chemical Physics · Physics 2014-02-11 Dimitri N. Laikov

Local electronic-structure methods in quantum chemistry operate on the ability to compress electron correlations more efficiently in a basis of spatially localized molecular orbitals than in a parent set of canonical orbitals. However, many…

Chemical Physics · Physics 2024-08-01 Jonas Greiner , Jürgen Gauss , Janus J. Eriksen

We investigate the coupling of different quantum-embedding approaches with a third molecular-mechanics layer, which can be either polarizable or non-polarizable. In particular, such a coupling is discussed for the multilevel families of…

Chemical Physics · Physics 2020-12-11 Linda Goletto , Tommaso Giovannini , Sarai D. Folkestad , Henrik Koch

We present an implementation and analysis of a stochastic high performance algorithm to calculate the correlation energy of three dimensional periodic systems in second-order M{\o}ller-Plesset perturbation theory (MP2). In particular we…

Chemical Physics · Physics 2018-02-12 Tobias Schäfer , Benjamin Ramberger , Georg Kresse
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