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

  • Shlomo Yitzchaik (a1), Paul M. Lundquist (a2), Weiping Lin (a2), David R. Kanis (a1), Mark A. Ratner (a1), Tobin J. Marks (a1) and George K. Wong (a1) (a2)...


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.



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