(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

Research output: Contribution to journalArticle

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.

Original languageEnglish
Pages (from-to)711-724
Number of pages14
JournalTheoretical Chemistry Accounts
Volume130
Issue number4-6
DOIs
Publication statusPublished - 1 Dec 2011

Keywords

  • Broken-symmetry method
  • Diradical
  • Hyperpolarizability
  • Natural orbital
  • Open-shell molecule
  • Spin projection

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