Title: Combined molecular and supramolecular bottom-up nanoengineering for enhanced nonlinear optical response: experiments, modeling, and approaching the fundamental limit
Authors: Pérez-Moreno, Javier ×
Asselberghs, Inge
Song, Kai
Clays, Koen
Zhao, Yuxia
Nakanishi, Hachiro
Okada, Shuji
Nogi, Kyoko
Kim, Oh-Kil
Je, Jongtae
Matrai, Janka
De Maeyer, Marc
Kuzyk, Mark G #
Issue Date: 21-Feb-2007
Series Title: Journal of Chemical Physics vol:126 issue:7
Article number: 074705
Abstract: The authors study the combination of two independent strategies that enhance the hyperpolarizability of ionic organic chromophores. The first molecular-level strategy is the extension of the conjugation path in the active chromophore. The second supramolecular-level strategy is the bottom-up nanoengineering of an inclusion complex of the chromophore in an amylose helix by self-assembly. The authors study a series of five (dimethylamino)stilbazolium-type chromophores with increasing conjugation length between the (dimethylamino)phenyl donor ring and the pyridinium acceptor ring in conjunction with four amylose helices of differing molecular weights. The first hyperpolarizabilities of the self-assembled inclusion complexes, as determined with frequency-resolved femtosecond hyper-Rayleigh scattering at 800 and 1300 nm, are compared with experimental values for the free chromophores in solution and with theoretical values. While the experimental values for the hyperpolarizability in solution are lower than the theoretically predicted values, an enhancement upon inclusion is observed, with the longest chromophore in the best amylose helix showing an enhancement by one order of magnitude. Molecular modeling of the inclusion of the chromophore suggests that the coplanarity of the two rings is more important than all-trans configuration in the conjugation path. The fundamental limit analysis indicates that the inclusion inside the amylose helix results in an optimal excited-level energy spacing that is responsible for breaching the apparent limit.
ISSN: 0021-9606
Publication status: published
KU Leuven publication type: IT
Appears in Collections:Biochemistry, Molecular and Structural Biology Section
Molecular Imaging and Photonics
Vesalius Research Centre (-)
× corresponding author
# (joint) last author

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