Frequency-dependent second harmonic generation in acentric chromophoric self-assembled NLO materials

Shlomo Yitzchaik*, Paul M. Lundquist, Weiping Lin, David R. Kanis, Mark A. Ratner, Tobin J. Marks, George K. Wong

*Corresponding author for this work

Research output: Contribution to journalConference articlepeer-review

1 Scopus citations


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 angstrom 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 ℏω = 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.

Original languageEnglish (US)
Pages (from-to)119-125
Number of pages7
JournalMaterials Research Society Symposium - Proceedings
StatePublished - 1994
EventProceedings of the 1994 MRS Symposium - San Francisco, CA, USA
Duration: Apr 4 1994Apr 8 1994

ASJC Scopus subject areas

  • General Materials Science
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering


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