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Proceedings Paper

Analysis of the unusual wavelength dependence of the first hyperpolarizability of porphyrin derivatives
Author(s): K. De Mey; K. Clays; Michael J. Therien; David N. Beratan; Inge Asselberghs
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Paper Abstract

Successfully predicting the frequency dispersion of electronic hyperpolarizabilities is an unresolved challenge in materials science and electronic structure theory. It has been shown1 that the generalized Thomas-Kuhn sum rules combined with linear absorption data and measured hyperpolarizabilities at one or two frequencies, may be used to predict the entire frequency-dependent electronic hyperpolarizability spectrum. This treatment includes two- and threelevel contributions that arise from the lowest two or three excited state manifolds, enabling us to describe the unusual observed frequency dispersion of the dynamic hyperpolarizability in high oscillator strength M-PZn chromophores, where (porphinato)zinc(II) (PZn) and metal(II)polypyridyl (M) units are connected via an ethyne unit that aligns the high oscillator strength transition dipoles of these components in a head-to-tail arrangement. Importantly, this approach provides a quantitative scheme to use linear optical absorption spectra and very few individual hyperpolarizability values to predict the entire frequency-dependent nonlinear optical response. In addition we provide here experimental dynamic hyperpolarizability values determined by hyper-Rayleigh scattering that underscore the validity of our approach.

Paper Details

Date Published: 17 August 2010
PDF: 10 pages
Proc. SPIE 7774, Linear and Nonlinear Optics of Organic Materials X, 777403 (17 August 2010); doi: 10.1117/12.859819
Show Author Affiliations
K. De Mey, Katholieke Univ. Leuven (Belgium)
K. Clays, Katholieke Univ. Leuven (Belgium)
Michael J. Therien, Duke Univ. (United States)
David N. Beratan, Duke Univ. (United States)
Inge Asselberghs, Katholieke Univ. Leuven (Belgium)


Published in SPIE Proceedings Vol. 7774:
Linear and Nonlinear Optics of Organic Materials X
Manfred Eich; Jean-Michel Nunzi; Rachel Jakubiak; Theodore G. Goodson, Editor(s)

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