Second-order nonlinear optical properties of Λ-shaped pyrazine derivatives

Frédéric Castet, Adrien Gillet, Filip Bureš, Aurélie Plaquet, Vincent Rodriguez, Benoît Champagne

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The linear and nonlinear optical (NLO) properties of a series of Λ-shaped derivatives containing a 4,5-dicyanopyrazine acceptor unit, N,N-dimethylamino donor groups and systematically enlarged π-conjugated linkers are investigated by means of UV/Visible and Hyper-Rayleigh scattering spectroscopies. Density functional theory calculations are also carried out to rationalize the magnitude and symmetry of the NLO responses. The results demonstrate that these compounds possess two low-lying excited electronic states close to each other in energy, which are accessible through one-photon optical transitions respectively polarized perpendicular and parallel to the two-fold molecular axis. These two states contribute additively to the first hyperpolarizability, which exhibits a dominant dipolar character. We also show that the NLO responses significantly deviate from Kleinman's index permutation symmetry.

Original languageEnglish
Article number108850
JournalDyes and pigments
Publication statusPublished - 1 Jan 2021


  • Density functional theory
  • First hyperpolarizability
  • Hyper-Rayleigh scattering
  • Kleinman symmetry
  • Nonlinear optics
  • Pyrazines


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