Statements in which the resource exists as a subject.
PredicateObject
rdf:type
lifeskim:mentions
pubmed:issue
7
pubmed:dateCreated
2007-3-1
pubmed:abstractText
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.
pubmed:language
eng
pubmed:journal
pubmed:citationSubset
IM
pubmed:chemical
pubmed:status
MEDLINE
pubmed:month
Feb
pubmed:issn
0021-9606
pubmed:author
pubmed:issnType
Print
pubmed:day
21
pubmed:volume
126
pubmed:owner
NLM
pubmed:authorsComplete
Y
pubmed:pagination
074705
pubmed:dateRevised
2008-11-21
pubmed:meshHeading
pubmed:year
2007
pubmed:articleTitle
Combined molecular and supramolecular bottom-up nanoengineering for enhanced nonlinear optical response: experiments, modeling, and approaching the fundamental limit.
pubmed:affiliation
Department of Chemistry, University of Leuven, Celestijnenlaan 200D, B-3001 Leuven, Belgium.
pubmed:publicationType
Journal Article, Research Support, U.S. Gov't, Non-P.H.S., Research Support, Non-U.S. Gov't