(Hyper)polarizability density analysis for open-shell molecular systems based on natural orbitals and occupation numbers

Masayoshi Nakano, Hitoshi Fukui, Takuya Minami, Kyohei Yoneda, Yasuteru Shigeta, Ryohei Kishi, Benoît Champagne, Edith Botek, Takashi Kubo, Koji Ohta, Kenji Kamada

Résultats de recherche: Contribution à un journal/une revueArticle

Résumé

We have developed a method for analyzing the (hyper)polarizabilities of open-shell molecular systems. This method employs the (hyper)polarizability densities based on the natural orbitals and occupation numbers, which enables us to analyze the contributions of odd electrons having various open-shell (diradical) characters. Within broken-symmetry, i. e., spin-unrestricted, single-determinant molecular orbital and density functional theory approaches, we can also remove the spin contamination effects on these quantities through spin projection. To do that, an approximate spin projected method has been elaborated and applied to the analysis of the (hyper)polarizability of multi-radical systems. As examples, typical open-shell singlet systems, 1,3-dipoles and rectangular graphene nanoflakes, are examined.

langueAnglais
Pages711-724
Nombre de pages14
journalTheoretical Chemistry Accounts
Volume130
Numéro4-6
Les DOIs
étatPublié - 1 déc. 2011

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Graphite
Molecular orbitals
occupation
Density functional theory
Contamination
orbitals
Electrons
determinants
broken symmetry
molecular orbitals
graphene
contamination
projection
dipoles
density functional theory
electrons

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    Nakano, Masayoshi ; Fukui, Hitoshi ; Minami, Takuya ; Yoneda, Kyohei ; Shigeta, Yasuteru ; Kishi, Ryohei ; Champagne, Benoît ; Botek, Edith ; Kubo, Takashi ; Ohta, Koji ; Kamada, Kenji. / (Hyper)polarizability density analysis for open-shell molecular systems based on natural orbitals and occupation numbers. Dans: Theoretical Chemistry Accounts. 2011 ; Vol 130, Numéro 4-6. p. 711-724
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    abstract = "We have developed a method for analyzing the (hyper)polarizabilities of open-shell molecular systems. This method employs the (hyper)polarizability densities based on the natural orbitals and occupation numbers, which enables us to analyze the contributions of odd electrons having various open-shell (diradical) characters. Within broken-symmetry, i. e., spin-unrestricted, single-determinant molecular orbital and density functional theory approaches, we can also remove the spin contamination effects on these quantities through spin projection. To do that, an approximate spin projected method has been elaborated and applied to the analysis of the (hyper)polarizability of multi-radical systems. As examples, typical open-shell singlet systems, 1,3-dipoles and rectangular graphene nanoflakes, are examined.",
    keywords = "Broken-symmetry method, Diradical, Hyperpolarizability, Natural orbital, Open-shell molecule, Spin projection",
    author = "Masayoshi Nakano and Hitoshi Fukui and Takuya Minami and Kyohei Yoneda and Yasuteru Shigeta and Ryohei Kishi and Beno{\^i}t Champagne and Edith Botek and Takashi Kubo and Koji Ohta and Kenji Kamada",
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    (Hyper)polarizability density analysis for open-shell molecular systems based on natural orbitals and occupation numbers. / Nakano, Masayoshi; Fukui, Hitoshi; Minami, Takuya; Yoneda, Kyohei; Shigeta, Yasuteru; Kishi, Ryohei; Champagne, Benoît; Botek, Edith; Kubo, Takashi; Ohta, Koji; Kamada, Kenji.

    Dans: Theoretical Chemistry Accounts, Vol 130, Numéro 4-6, 01.12.2011, p. 711-724.

    Résultats de recherche: Contribution à un journal/une revueArticle

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    T1 - (Hyper)polarizability density analysis for open-shell molecular systems based on natural orbitals and occupation numbers

    AU - Nakano,Masayoshi

    AU - Fukui,Hitoshi

    AU - Minami,Takuya

    AU - Yoneda,Kyohei

    AU - Shigeta,Yasuteru

    AU - Kishi,Ryohei

    AU - Champagne,Benoît

    AU - Botek,Edith

    AU - Kubo,Takashi

    AU - Ohta,Koji

    AU - Kamada,Kenji

    PY - 2011/12/1

    Y1 - 2011/12/1

    N2 - We have developed a method for analyzing the (hyper)polarizabilities of open-shell molecular systems. This method employs the (hyper)polarizability densities based on the natural orbitals and occupation numbers, which enables us to analyze the contributions of odd electrons having various open-shell (diradical) characters. Within broken-symmetry, i. e., spin-unrestricted, single-determinant molecular orbital and density functional theory approaches, we can also remove the spin contamination effects on these quantities through spin projection. To do that, an approximate spin projected method has been elaborated and applied to the analysis of the (hyper)polarizability of multi-radical systems. As examples, typical open-shell singlet systems, 1,3-dipoles and rectangular graphene nanoflakes, are examined.

    AB - We have developed a method for analyzing the (hyper)polarizabilities of open-shell molecular systems. This method employs the (hyper)polarizability densities based on the natural orbitals and occupation numbers, which enables us to analyze the contributions of odd electrons having various open-shell (diradical) characters. Within broken-symmetry, i. e., spin-unrestricted, single-determinant molecular orbital and density functional theory approaches, we can also remove the spin contamination effects on these quantities through spin projection. To do that, an approximate spin projected method has been elaborated and applied to the analysis of the (hyper)polarizability of multi-radical systems. As examples, typical open-shell singlet systems, 1,3-dipoles and rectangular graphene nanoflakes, are examined.

    KW - Broken-symmetry method

    KW - Diradical

    KW - Hyperpolarizability

    KW - Natural orbital

    KW - Open-shell molecule

    KW - Spin projection

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