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Proceedings Paper

Hyperpolar multichromophoric nanoassembly for molecular nonlinear optics
Author(s): Mireille H. Blanchard-Desce; M. Ait Amer Meziane; El Djouhar Rekai; Jean-Bernard Baudin; Ludovic Jullien; Isabelle N. Ledoux; Joseph Zyss
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Paper Abstract

A multichromophoric nanoassembly was designed by gathering seven push-pull chromophores on a β-cyclodextrin assembling unit via covalent linkers. Such supermolecule provides a valuable model for the investigation of confinement effects on the linear and nonlinear optical properties of push-pull chromophores in the condensed phase. Push-pull chromophores display a significant ground-state dipole, thus promoting dipolar interactions that are expected to influence both the conformation and the optical properties of the multichromophoric assembly. In this perspective, the photophysical and nonlinear optical properties of the mutichromophoric bundle were investigated and compared to those of the monomeric chromophore. The absorption, circular dichroism and fluorescence investigations provide evidence that the push-pull chromophores do not behave as isolated independent chromophores within the multichromophoric assembly. The nanoscale supermolecule is hypsochromically and significantly hypochromically shifted with respect to its monomeric analogue. In addition, the close proximity promotes excitonic coupling, as well as excimer formation phenomena. The nanoscopic assembly also shows a very large dipolar moment (μ = 38 D), and a significant molecular first-order hyperpolarisability, which reveal a spontaneous sheaf-type self-arrangement of the dipolar chromophores within the supermolecule. Such chiral hyperpolar nanoassemblies are promising candidates as model systems for nanophotonics.

Paper Details

Date Published: 18 December 2002
PDF: 10 pages
Proc. SPIE 4798, Linear and Nonlinear Optics of Organic Materials II, (18 December 2002); doi: 10.1117/12.452066
Show Author Affiliations
Mireille H. Blanchard-Desce, Univ. de Rennes I (France)
M. Ait Amer Meziane, Univ. de Rennes I (France)
El Djouhar Rekai, Ecole Normale Superieure Paris (France)
Jean-Bernard Baudin, Ecole Normale Superieure Paris (France)
Ludovic Jullien, Ecole Normale Superieure Paris (France)
Isabelle N. Ledoux, Ecole Normale Superieure de Cachan (France)
Joseph Zyss, Ecole Normale Superieure de Cachan (France)

Published in SPIE Proceedings Vol. 4798:
Linear and Nonlinear Optics of Organic Materials II
Manfred Eich; Mark G. Kuzyk, Editor(s)

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