Relationship between second hyperpolarizability and diradical character in open-shell singlet metal-metal multiply bonded systems

Hitoshi Fukui, Edith Botek, Benoît Champagne, Yasuteru Shigeta, Masayoshi Nakano

Research output: Contribution in Book/Catalog/Report/Conference proceedingConference contribution

Abstract

Using the coupled-cluster method with single and double excitations (CCSD), we investigate the relationship between the second hyperpolarizability (γ) and the diradical characters of dσ, dπ and dδ orbitals for the open-shell singlet Cr(II)-Cr(II) quadruply bonded model system, in which d 4 -d 4 interactions make one dσ, two equivalent dπ and one dδ molecular orbitals, and then these orbitals exhibit different diradical characters. The γ value is divided into the contributions of natural orbitals in order to reveal the contributions of dσ, dπ and dδ orbitals to γ. From these results, we elucidate a relationship among the orbital symmetry, diradical character and γ value, and thus we propose a guiding principle for designing open-shell singlet metal-metal multiply bonded complexes with highly efficient third-order nonlinear optical properties.

Original languageEnglish
Title of host publicationProceedings of the International Conference of Computational Methods in Sciences and Engineering 2010, ICCMSE 2010
EditorsTheodore E. Simos, Theodore E. Simos, George Maroulis, Theodore E. Simos, Theodore E. Simos
PublisherAmerican institute of physics
Pages245-248
Number of pages4
ISBN (Electronic)9780735412828
DOIs
Publication statusPublished - 1 Jan 2015
EventInternational Conference of Computational Methods in Sciences and Engineering 2010, ICCMSE 2010 - Psalidi, Kos, Greece
Duration: 3 Oct 20108 Oct 2010

Publication series

NameAIP Conference Proceedings
Volume1642
ISSN (Print)0094-243X
ISSN (Electronic)1551-7616

Conference

ConferenceInternational Conference of Computational Methods in Sciences and Engineering 2010, ICCMSE 2010
CountryGreece
CityPsalidi, Kos
Period3/10/108/10/10

Fingerprint

metal shells
orbitals
metals
molecular orbitals
optical properties
symmetry
excitation

Keywords

  • dichromium complex
  • metal-metal multiple bond
  • multi-diradical
  • nonlinear optics
  • open-shell
  • second hyperpolarizability

Cite this

Fukui, H., Botek, E., Champagne, B., Shigeta, Y., & Nakano, M. (2015). Relationship between second hyperpolarizability and diradical character in open-shell singlet metal-metal multiply bonded systems. In T. E. Simos, T. E. Simos, G. Maroulis, T. E. Simos, & T. E. Simos (Eds.), Proceedings of the International Conference of Computational Methods in Sciences and Engineering 2010, ICCMSE 2010 (pp. 245-248). [4906663] (AIP Conference Proceedings; Vol. 1642). American institute of physics. https://doi.org/10.1063/1.4906663
Fukui, Hitoshi ; Botek, Edith ; Champagne, Benoît ; Shigeta, Yasuteru ; Nakano, Masayoshi. / Relationship between second hyperpolarizability and diradical character in open-shell singlet metal-metal multiply bonded systems. Proceedings of the International Conference of Computational Methods in Sciences and Engineering 2010, ICCMSE 2010. editor / Theodore E. Simos ; Theodore E. Simos ; George Maroulis ; Theodore E. Simos ; Theodore E. Simos. American institute of physics, 2015. pp. 245-248 (AIP Conference Proceedings).
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abstract = "Using the coupled-cluster method with single and double excitations (CCSD), we investigate the relationship between the second hyperpolarizability (γ) and the diradical characters of dσ, dπ and dδ orbitals for the open-shell singlet Cr(II)-Cr(II) quadruply bonded model system, in which d 4 -d 4 interactions make one dσ, two equivalent dπ and one dδ molecular orbitals, and then these orbitals exhibit different diradical characters. The γ value is divided into the contributions of natural orbitals in order to reveal the contributions of dσ, dπ and dδ orbitals to γ. From these results, we elucidate a relationship among the orbital symmetry, diradical character and γ value, and thus we propose a guiding principle for designing open-shell singlet metal-metal multiply bonded complexes with highly efficient third-order nonlinear optical properties.",
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Fukui, H, Botek, E, Champagne, B, Shigeta, Y & Nakano, M 2015, Relationship between second hyperpolarizability and diradical character in open-shell singlet metal-metal multiply bonded systems. in TE Simos, TE Simos, G Maroulis, TE Simos & TE Simos (eds), Proceedings of the International Conference of Computational Methods in Sciences and Engineering 2010, ICCMSE 2010., 4906663, AIP Conference Proceedings, vol. 1642, American institute of physics, pp. 245-248, International Conference of Computational Methods in Sciences and Engineering 2010, ICCMSE 2010, Psalidi, Kos, Greece, 3/10/10. https://doi.org/10.1063/1.4906663

Relationship between second hyperpolarizability and diradical character in open-shell singlet metal-metal multiply bonded systems. / Fukui, Hitoshi; Botek, Edith; Champagne, Benoît; Shigeta, Yasuteru; Nakano, Masayoshi.

Proceedings of the International Conference of Computational Methods in Sciences and Engineering 2010, ICCMSE 2010. ed. / Theodore E. Simos; Theodore E. Simos; George Maroulis; Theodore E. Simos; Theodore E. Simos. American institute of physics, 2015. p. 245-248 4906663 (AIP Conference Proceedings; Vol. 1642).

Research output: Contribution in Book/Catalog/Report/Conference proceedingConference contribution

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T1 - Relationship between second hyperpolarizability and diradical character in open-shell singlet metal-metal multiply bonded systems

AU - Fukui, Hitoshi

AU - Botek, Edith

AU - Champagne, Benoît

AU - Shigeta, Yasuteru

AU - Nakano, Masayoshi

PY - 2015/1/1

Y1 - 2015/1/1

N2 - Using the coupled-cluster method with single and double excitations (CCSD), we investigate the relationship between the second hyperpolarizability (γ) and the diradical characters of dσ, dπ and dδ orbitals for the open-shell singlet Cr(II)-Cr(II) quadruply bonded model system, in which d 4 -d 4 interactions make one dσ, two equivalent dπ and one dδ molecular orbitals, and then these orbitals exhibit different diradical characters. The γ value is divided into the contributions of natural orbitals in order to reveal the contributions of dσ, dπ and dδ orbitals to γ. From these results, we elucidate a relationship among the orbital symmetry, diradical character and γ value, and thus we propose a guiding principle for designing open-shell singlet metal-metal multiply bonded complexes with highly efficient third-order nonlinear optical properties.

AB - Using the coupled-cluster method with single and double excitations (CCSD), we investigate the relationship between the second hyperpolarizability (γ) and the diradical characters of dσ, dπ and dδ orbitals for the open-shell singlet Cr(II)-Cr(II) quadruply bonded model system, in which d 4 -d 4 interactions make one dσ, two equivalent dπ and one dδ molecular orbitals, and then these orbitals exhibit different diradical characters. The γ value is divided into the contributions of natural orbitals in order to reveal the contributions of dσ, dπ and dδ orbitals to γ. From these results, we elucidate a relationship among the orbital symmetry, diradical character and γ value, and thus we propose a guiding principle for designing open-shell singlet metal-metal multiply bonded complexes with highly efficient third-order nonlinear optical properties.

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PB - American institute of physics

ER -

Fukui H, Botek E, Champagne B, Shigeta Y, Nakano M. Relationship between second hyperpolarizability and diradical character in open-shell singlet metal-metal multiply bonded systems. In Simos TE, Simos TE, Maroulis G, Simos TE, Simos TE, editors, Proceedings of the International Conference of Computational Methods in Sciences and Engineering 2010, ICCMSE 2010. American institute of physics. 2015. p. 245-248. 4906663. (AIP Conference Proceedings). https://doi.org/10.1063/1.4906663