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We introduce and benchmark a systematically improvable route for excited-state calculations, state-specific configuration interaction ($\Delta$CI), \alert{which is a particular realization of multiconfigurational self-consistent field and…

Chemical Physics · Physics 2023-08-31 Fábris Kossoski , Pierre-François Loos

We introduce affordable computational strategies for calculating orbital and pair-orbital energies in atomic and molecular systems. Our methods are based on the pair Coupled Cluster Doubles (pCCD) ansatz and its orbital-optimized variant.…

Chemical Physics · Physics 2025-02-06 Seyedehdelaram Jahani , Somayeh Ahmadkhani , Katharina Boguslawski , Paweł Tecmer

A configuration-interaction model is presented for the barrier region of induced fission. The configuration space is composed of seniority-zero configurations constructed from self-consistent mean-field wave functions. The Hamiltonian…

Nuclear Theory · Physics 2023-02-03 G. F. Bertsch , K. Hagino

We show that systematic full configuration-interaction (FCI) calculations enable prediction of the energy spectra and the intrinsic spatial and spin structures of the many-body wave functions as a function of the detuning parameter for the…

Mesoscale and Nanoscale Physics · Physics 2022-05-05 Constantine Yannouleas , Uzi Landman

The idea of adaptive perturbation theory is to divide a Hamiltonian into a solvable part and a perturbation part. The solvable part contains the non-interacting sector and the diagonal elements of Fock space from the interacting terms. The…

Quantum Physics · Physics 2021-06-14 Xin Guo

Quantum mechanical calculations of core electron binding energies (CEBEs) leading to 2p hole states are relevant to interpreting L-edge x-ray photo-electron spectroscopy (XPS), as well as higher edges. Orbital-optimized density functional…

Chemical Physics · Physics 2025-07-31 Richard Kang , Leonardo A. Cunha , Diptarka Hait , Martin Head-Gordon

Coupled cluster (CC) methods are among the most accurate methods in quantum chemistry. However, the standard CC linear response formulation is not gauge invariant resulting in errors when modelling properties like optical rotation and…

Chemical Physics · Physics 2018-03-13 Rolf H. Myhre

We study the Kondo effect of a quantum dot placed in a complex mesoscopic structure. Assuming that electronic interactions are taking place solely on the dot, and focusing on the infinite Hubbard interaction limit, we use a decoupling…

Mesoscale and Nanoscale Physics · Physics 2009-11-10 O. Entin-Wohlman , A. Aharony , Y. Meir

Since in coupled-cluster (CC) theory ground-state and excitation energies are eigenvalues of a non-Hermitian matrix, these energies can in principle take on complex values. In this paper we discuss the appearance of complex energy values in…

Chemical Physics · Physics 2022-01-12 Simon Thomas , Florian Hampe , Stella Stopkowicz , Jürgen Gauss

We introduce single and double particle-hole excitations in the recently revived spin-projected Hartree-Fock. Our motivation is to treat static correlation with spin-projection and recover the residual correlation, mostly dynamic in nature,…

Chemical Physics · Physics 2016-01-20 Takashi Tsuchimochi , Seiichiro Ten-no

An accurate description of electron correlation is one of the most challenging problems in quantum chemistry. The exact electron correlation can be obtained by means of full configuration interaction (FCI). A simple strategy for…

Chemical Physics · Physics 2021-05-14 Jae Woo Park

Neutral uranium (U I) is a very difficult atom for theoretical calculations due to a large number of valence electrons, six, strong valence-valence and valence-core correlations, high density of states, and relativistic effects.…

Atomic Physics · Physics 2020-10-14 Igor M. Savukov

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

We give a thorough analysis of the convergence properties of the configuration-interaction method as applied to parabolic quantum dots among other systems, including \emph{a priori} error estimates. The method converges slowly in general,…

Computational Physics · Physics 2013-05-29 Simen Kvaal

High-order topological insulators (HOTIs), as generalized from topological crystalline insulators (TCIs), are characterized with lower-dimensional metallic boundary states protected by spatial symmetries of a crystal, whose theoretical…

Materials Science · Physics 2022-08-02 Citian Wang , Feng Liu , Huaqing Huang

Multi-configurational wave functions are known to describe electronic structure across a Born-Oppenheimer surface qualitatively correct. However, for quantitative reaction energies, dynamical correlation originating from the many…

Chemical Physics · Physics 2020-04-16 Christopher J. Stein , Markus Reiher

The fundamental non-Hermitian nature of the forms of coupled-cluster (CC) theory widely used in quantum chemistry has usually been viewed as a negative, but the present letter shows how this can be used to advantage. Specifically, the…

Finite-Hamiltonian impurity solvers provide direct real-frequency spectra and a natural route to enlarged impurity Hamiltonians, but their applicability is limited by the rapid Hilbert-space growth with the number of bath or other added…

Strongly Correlated Electrons · Physics 2026-05-11 Jeongmoo Lee , Ara Go

We present a program for solving exactly the general pairing Hamiltonian based on diagonalization. The program generates the seniority-zero shell-model-like basis vectors via the `01' inversion algorithm. The Hamiltonian matrix is…

Nuclear Theory · Physics 2020-01-08 Xiaoyu Liu , Chong Qi

The congruent transformation of the electronic Hamiltonian is developed to address the electron correlation problem in many-electron systems. The central strategy presented in this method is to perform transformation on the electronic…

Chemical Physics · Physics 2012-12-21 Jennifer M. Elward , Johannes Hoja , Arindam Chakraborty