Title:
Resonant enhancement of two-photon absorption in substituted fluorene molecules

dc.contributor.author Hales, Joel M. en_US
dc.contributor.author Hagan, David J. en_US
dc.contributor.author Van Stryland, Eric W. en_US
dc.contributor.author Schafer, K. J. en_US
dc.contributor.author Morales, A. R. en_US
dc.contributor.author Belfield, Kevin D. en_US
dc.contributor.author Pacher, P. en_US
dc.contributor.author Kwon, O. en_US
dc.contributor.author Zojer, Egbert en_US
dc.contributor.author Brédas, Jean-Luc en_US
dc.contributor.corporatename Georgia Institute of Technology. Center for Organic Photonics and Electronics en_US
dc.contributor.corporatename University of Central Florida. School of Optics en_US
dc.contributor.corporatename CREOL (Research center) en_US
dc.contributor.corporatename University of Central Florida. Dept. of Chemistry en_US
dc.contributor.corporatename University of Arizona. Dept. of Chemistry en_US
dc.contributor.corporatename Georgia Institute of Technology. School of Chemistry and Biochemistry en_US
dc.date.accessioned 2013-04-11T20:22:44Z
dc.date.available 2013-04-11T20:22:44Z
dc.date.issued 2004-08
dc.description © 2004 American Institute of Physics. The electronic version of this article is the complete one and can be found at: http://dx.doi.org/10.1063/1.1770726 en_US
dc.description DOI: 10.1063/1.1770726 en_US
dc.description.abstract The degenerate and nondegenerate two-photon absorption (2PA) spectra for a symmetric and an asymmetric fluorene derivative were experimentally measured in order to determine the effect of intermediate state resonance enhancement (ISRE) on the 2PA cross section δ. The ability to tune the individual photon energies in the nondegenerate 2PA (ND-2PA) process afforded a quantitative study of the ISRE without modifying the chemical structure of the investigated chromophores. Both molecules exhibited resonant enhancement of the nonlinearity with the asymmetric compound showing as much as a twentyfold increase in δ. Furthermore, the possibility of achieving over a one order of magnitude enhancement of the nonlinearity reveals the potential benefits of utilizing ND-2PA for certain applications. To model ISRE, we have used correlated quantum-chemical methods together with the perturbative sum-over-states (SOS) expression. We find strong qualitative and quantitative correlation between the experimental and theoretical results. Finally, using a simplified three-level model for the SOS expression, we provide intuitive insight into the process of ISRE for ND-2PA. en_US
dc.identifier.citation Hales, Joel M. and Hagan, D. J. and Van Stryland, E. W. and Schafer, K. J. and Morales, A. R. and Belfield, K. D. and Pacher, P. and Kwon, O. and Zojer, Egbert and Brédas, Jean-Luc, "Resonant enhancement of two-photon absorption in substituted fluorene molecules," Journal of Chemical Physics, 121, 7, 3152-3160 (August 15 2004) en_US
dc.identifier.doi 10.1063/1.1770726
dc.identifier.issn 0021-9606
dc.identifier.uri http://hdl.handle.net/1853/46788
dc.publisher Georgia Institute of Technology en_US
dc.publisher.original American Institute of Physics en_US
dc.subject Two-photon processes en_US
dc.subject Quantum chemistry en_US
dc.subject Chemical structure en_US
dc.subject Nonlinear optics en_US
dc.subject Excited states en_US
dc.subject Molecular configurations en_US
dc.subject Fluorine en_US
dc.title Resonant enhancement of two-photon absorption in substituted fluorene molecules en_US
dc.type Text
dc.type.genre Article
dspace.entity.type Publication
local.contributor.author Brédas, Jean-Luc
local.contributor.corporatename Center for Organic Photonics and Electronics
relation.isAuthorOfPublication 4d846669-7bb3-480a-8267-9b1cd9ff38d2
relation.isOrgUnitOfPublication 43f8dc5f-0678-4f07-b44a-edbf587c338f
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