Title
Practical model for first hyperpolarizability dispersion accounting for both homogeneous and inhomogeneous broadening effects Practical model for first hyperpolarizability dispersion accounting for both homogeneous and inhomogeneous broadening effects
Author
Faculty/Department
Faculty of Sciences. Physics
Publication type
article
Publication
Washington, D.C :American Chemical Society ,
Subject
Physics
Chemistry
Engineering sciences. Technology
Source (journal)
The journal of physical chemistry letters / American Chemical Society. - Washington, D.C, 2010, currens
Volume/pages
3(2012) :16 , p. 2248-2252
ISSN
1948-7185
ISI
000307697300024
Carrier
E
Target language
English (eng)
Full text (Publishers DOI)
Affiliation
University of Antwerp
Abstract
A practical yet accurate dispersion model for the molecular first hyperpolarizability beta is presented, incorporating both homogeneous and inhomogeneous line broadening because these affect the beta dispersion differently, even if they are indistinguishable in linear absorption. Consequently, combining the absorption spectrum with one free shape-determining parameter G(inhom), the inhomogeneous line width, turns out to be. necessary and sufficient to obtain a reliable description of the beta dispersion, requiring no information on the homogeneous (including vibronic) and inhomogeneous line broadening mechanisms involved, providing an ideal model for practical use in extrapolating experimental nonlinear optical (NLO) data. The model is applied to the efficient NLO chromophore picolinium quinodimethane, yielding an excellent fit of the two photon resonant wavelength dependent data and a dependable static, value beta(0) = 316 x 10(-30) esu. Furthermore, we show that including a second electronic excited state in the model does yield an improved description of the NLO data at shorter wavelengths but has only limited influence on beta(0).
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