Third-order nonlinear optical properties of one-dimensional quinoidal oligothiophene derivatives involving phenoxyl groups

Ryohei Kishi, Tsubasa Katsurayama, Shoki Ochi, Akihiro Makino, Naoyuki Matsushita, Michika Saito, Takanori Nagami, Jun Ya Fujiyoshi, Masayoshi Nakano

Research output: Contribution to journalArticlepeer-review

3 Citations (Scopus)

Abstract

The diradical characters (y) and third-order nonlinear optical (NLO) properties of open-shell quinoidal oligothiophene derivatives with phenoxyl groups, and the corresponding reduced (hydrogenated)-state oligomers, are investigated by using the broken-symmetry density functional theory method. The oxidized (dehydrogenated) states are predicted to have an openshell singlet ground state and their y values increase with the number of units. Static second hyperpolarizabilities (γ) of the open-shell oligomers with intermediate y are shown to be enhanced significantly compared with those of the closed-shell analogues. Furthermore, owing to the effective diradical distances, the γ values of open-shell oligomers are found to exceed that of s-indaceno[1,2,3-cd;5,6,7-c’d’]diphenalene, which is known as an organic molecule with the largest twophoton absorption cross-section in this size of the pure hydrocarbons. This feature extends the range of efficient open-shell third-order NLO materials to a novel class of one-dimensional conjugated oligomers with redox-based high tunability of third-order NLO properties.

Original languageEnglish
Pages (from-to)506-513
Number of pages8
JournalChemistryOpen
Volume6
Issue number4
DOIs
Publication statusPublished - 2017 Aug
Externally publishedYes

Keywords

  • Density functional calculations
  • Diradicals
  • Nonlinear optics
  • Oligomers
  • Redox systems

ASJC Scopus subject areas

  • Chemistry(all)

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