Journal article
Combined molecular and supramolecular bottom-up nanoengineering for enhanced nonlinear optical response: experiments, modeling, and approaching the fundamental limit
The Journal of chemical physics, Vol.126(7), pp.074705-074705
02/21/2007
Handle:
https://hdl.handle.net/2376/115528
PMID: 17328625
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.
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Details
- Title
- Combined molecular and supramolecular bottom-up nanoengineering for enhanced nonlinear optical response: experiments, modeling, and approaching the fundamental limit
- Creators
- Javier Pérez-Moreno - Department of Chemistry, University of Leuven, Celestijnenlaan 200D, B-3001 Leuven, BelgiumInge AsselberghsKai SongKoen ClaysYuxia ZhaoHachiro NakanishiShuji OkadaKyoko NogiOh-Kil KimJongtae JeJanka MátraiMarc De MaeyerMark G Kuzyk
- Publication Details
- The Journal of chemical physics, Vol.126(7), pp.074705-074705
- Academic Unit
- Physics and Astronomy, Department of
- Publisher
- United States
- Identifiers
- 99900548223201842
- Language
- English
- Resource Type
- Journal article