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Frequency-Dependent Second Harmonic Generation in Acentric Chromophoric Self-Assembled NLO Materials

Published online by Cambridge University Press:  15 February 2011

Shlomo Yitzchaik ,
Paul M. Lundquist ,
Weiping Lin ,
David R. Kanis ,
Mark A. Ratner ,
Tobin J. Marks  and
George K. Wong
Shlomo Yitzchaik
Affiliation:
Department of Chemistry, the Materials Research Center, Northwestern University, Evanston, Illinois 60208-3113 (USA)
Paul M. Lundquist
Affiliation:
Physics and Astronomyt and the Materials Research Center, Northwestern University, Evanston, Illinois 60208-3113 (USA)
Weiping Lin
Affiliation:
Physics and Astronomyt and the Materials Research Center, Northwestern University, Evanston, Illinois 60208-3113 (USA)
David R. Kanis
Affiliation:
Department of Chemistry, the Materials Research Center, Northwestern University, Evanston, Illinois 60208-3113 (USA)
Mark A. Ratner
Affiliation:
Department of Chemistry, the Materials Research Center, Northwestern University, Evanston, Illinois 60208-3113 (USA)
Tobin J. Marks
Affiliation:
Department of Chemistry, the Materials Research Center, Northwestern University, Evanston, Illinois 60208-3113 (USA)
George K. Wong
Affiliation:
Department of Chemistry, the Materials Research Center, Northwestern University, Evanston, Illinois 60208-3113 (USA) Physics and Astronomyt and the Materials Research Center, Northwestern University, Evanston, Illinois 60208-3113 (USA)
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Abstract

An attractive and challenging approach to the construction of robust, thin film materials with large second-order optical nonlinearities is the covalent self-assembly of aligned arrays of high-β molecular chromophores into multilayer superlattices. In this paper, we describe the dispersion of second harmonic generation (SHG) in a self-assembled (SA) monolayer containing a stilbazolium chromophore. The frequency-dependent measurements were performed on 25 Å thick monolayers on glass using a tunable (0.4–2 μm) light source based on optical parametric amplification (OPA). The SHG spectrum contains a clear two-photon resonance at hω = 1.3eV. The maximum in the second-order susceptibility coincides with a low energy chromophore-centered charge-transfer excitation at 480 nm. The experimental SHG dispersion values compare favorably with theoretical results computed using a sum-over-states (SOS) formalism. However, the measured values exhibit a somewhat broader band response than the theoretical curve, and the origin of this behavior is discussed.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 351: Symposium V – Molecularly Designed Ultrafine/Nanostructured Materials , 1994 , 119
Copyright
Copyright © Materials Research Society 1994

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References

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