Theoretical investigation of the second-order nonlinear optical properties of helical pyridine-pyrimidine oligomers

Edith Botek, Frédéric Castet, Benoît Champagne

Research output: Contribution to journalArticle

Abstract

The structure and second-order nonlinear optical properties of a series of helical pyridine-pyrimidine oligqmers recently synthesized by Barboiu and Lehn have been investigated theoretically by combining molecular mechanics and quantum chemistry approaches. In the absence of substituents, the hyper-Rayleigh scattering response (βHRS) and the projection of the first hyperpolarizability on the dipole moment (β) exhibit periodic variations with chain length, but these non-linear optical responses remain small. The first hyperpolarizabilities can, however, be enhanced by adding sub-stituents. The greatest enhancement is obtained by substituting the pyrimidine groups by donor groups. Moreover, regular distributions of the donor groups around the helices enable thedesign of supramolecular structures exhibiting dipolar, octupolar or Λ-shaped nonlinear optical characters, evident from the values of the depolarization ratios in hyper-Rayleigh scattering. Therefore this theoretical investigation demonstrates the potential of helical structures for the organization of chromophores in such a way that they exhibit large and specific second-order nonlinear optical responses.

Original languageEnglish
Pages (from-to)8687-8695
Number of pages9
JournalChemistry: A European Journal
Volume12
Issue number34
DOIs
Publication statusPublished - 24 Nov 2006

Fingerprint

Rayleigh scattering
Oligomers
Pyridine
Optical properties
Quantum chemistry
Molecular mechanics
Dipole moment
Depolarization
Chromophores
Chain length
pyridine
pyrimidine

Keywords

  • Helical structures
  • Nitrogen heterocycles
  • Nonlinear optics
  • Substituent effects

Cite this

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Theoretical investigation of the second-order nonlinear optical properties of helical pyridine-pyrimidine oligomers. / Botek, Edith; Castet, Frédéric; Champagne, Benoît.

In: Chemistry: A European Journal, Vol. 12, No. 34, 24.11.2006, p. 8687-8695.

Research output: Contribution to journalArticle

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AU - Champagne, Benoît

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