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

Edith Botek, Frédéric Castet, Benoît Champagne

Résultats de recherche: Contribution à un journal/une revueArticle

Résumé

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.

langue originaleAnglais
Pages (de - à)8687-8695
Nombre de pages9
journalChemistry: A European Journal
Volume12
Numéro de publication34
Les DOIs
étatPublié - 24 nov. 2006

Empreinte digitale

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

Citer ceci

@article{9d2c250b630042f39c0c8151a6cb659c,
title = "Theoretical investigation of the second-order nonlinear optical properties of helical pyridine-pyrimidine oligomers",
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.",
keywords = "Helical structures, Nitrogen heterocycles, Nonlinear optics, Substituent effects",
author = "Edith Botek and Fr{\'e}d{\'e}ric Castet and Beno{\^i}t Champagne",
year = "2006",
month = "11",
day = "24",
doi = "10.1002/chem.200600551",
language = "English",
volume = "12",
pages = "8687--8695",
journal = "Chemistry: A European Journal",
issn = "0947-6539",
publisher = "Wiley Online Library",
number = "34",

}

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

Dans: Chemistry: A European Journal, Vol 12, Numéro 34, 24.11.2006, p. 8687-8695.

Résultats de recherche: Contribution à un journal/une revueArticle

TY - JOUR

T1 - Theoretical investigation of the second-order nonlinear optical properties of helical pyridine-pyrimidine oligomers

AU - Botek, Edith

AU - Castet, Frédéric

AU - Champagne, Benoît

PY - 2006/11/24

Y1 - 2006/11/24

N2 - 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.

AB - 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.

KW - Helical structures

KW - Nitrogen heterocycles

KW - Nonlinear optics

KW - Substituent effects

UR - http://www.scopus.com/inward/record.url?scp=33845223895&partnerID=8YFLogxK

U2 - 10.1002/chem.200600551

DO - 10.1002/chem.200600551

M3 - Article

AN - SCOPUS:33845223895

VL - 12

SP - 8687

EP - 8695

JO - Chemistry: A European Journal

JF - Chemistry: A European Journal

SN - 0947-6539

IS - 34

ER -