Hybrid Treatments Based on Determinant Seniority Numbers and Spatial Excitation Levels in the Configuration Interaction Framework

In this work we project the Hamiltonian of an N-electron system onto a set of N-electron determinants cataloged by their seniority numbers and their excitation levels with respect to a reference determinant. We show that, in open-shell systems, the diagonalization of the N-electron Hamiltonian matri...

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Detalles Bibliográficos
Autores: Alcoba, Diego Ricardo, Torre, Alicia, Lain, Luis, Oña, Ofelia Beatriz, Massaccesi, Gustavo Ernesto, Capuzzi, Pablo
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2018
País:Argentina
Institución:Consejo Nacional de Investigaciones Científicas y Técnicas
Repositorio:CONICET Digital (CONICET)
Idioma:inglés
OAI Identifier:oai:ri.conicet.gov.ar:11336/96717
Acceso en línea:http://hdl.handle.net/11336/96717
Access Level:acceso abierto
Palabra clave:CONFIGURATION INTERACTION METHODOLOGY
EXCITATION LEVEL OPERATORS
EXCITATION LEVELS IN N-ELECTRON DETERMINANTS
HYBRID METHODS IN CI TREATMENTS
SENIORITY NUMBER OF N-ELECTRON DETERMINANTS
SENIORITY NUMBER OPERATORS
SPIN CONTAMINATION OF WAVE FUNCTIONS
https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
Descripción
Sumario:In this work we project the Hamiltonian of an N-electron system onto a set of N-electron determinants cataloged by their seniority numbers and their excitation levels with respect to a reference determinant. We show that, in open-shell systems, the diagonalization of the N-electron Hamiltonian matrix leads to eigenstates of the operator Ŝ2 when the excitation levels are counted in terms of spatial orbitals instead of spin-orbitals. Our proposal is based on the commutation relations between the N-electron operators seniority number and spatial excitation level, as well as between these operators and the spin operators Ŝ2 and Ŝz. Energy and 〈Ŝ2〉 expectation values of molecular systems obtained from our procedure are compared with those arising from the standard hybrid configuration interaction methods based on seniority numbers and spin-orbital-excitation levels. We analyze the behavior of these methods, evaluating their computational costs and establishing their usefulness.