Hostname: page-component-cd9895bd7-fscjk Total loading time: 0 Render date: 2024-12-27T02:02:36.299Z Has data issue: false hasContentIssue false
  • English
  • Français

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)
Get access

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

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1. (a) Yitzchaik, S., Roscoe, S.B., Kakkar, A.K., Allan, D.S., Marks, T.J., Xu, Z., Zhang, T., Lin, W. and Wong, G.K., J. Phys. Chem. 97, 6958 (1993). (b) A.K. Kakkar, S. Yitzchaik, S.B. Roscoe, F. Kubota, D.S. Allan, T.J. Marks, W. Lin and G.K. Wong, Langmuir 9, 388 (1993). (c) D. Li, M.A. Ratner, T.J. Marks, C. Zhang, J. Yang and G.K. Wong, J. Am. Chem. Soc. 112, 7389 (1990). (d) S.B. Roscoe, S. Yitzchaik, A.K. Kakkar, T.J. Marks, W. Lin and G.K. Wong, Langmuir -in press. (e) P. Lundquist, S. Yitzchaik, T. Zhang, D.R. Kanis, M.A. Ratner, T.J. Marks and G.K. Wong, Appl. Phys. Lett. - in press.Google Scholar
2. (a) Marder, S.R., Sohn, J.E. and Stucky, G.D. (Eds.) Materials for Nonlinear Optics: Chemical Perspectives, ACS Symposium Series 455, American Chemical Society, Washington, DC (1991). (b) P.N. Prasad and D.J. Williams, Introduction to Nonlinear Optical Effects in Molecules and Polymers, Wiley, New York (1991).Google Scholar
3. Ashwell, G.J., Hargreaves, R.C., Baldwin, C.E., Bahra, G.S., Brown, C.R., Nature 357, 393 (1992).Google Scholar
4. Ulman, A., An Introduction to Ultrathin Organic Films, Academic Press, New York, (1991), and references therein.Google Scholar
5. Zhang, T.G., Zhang, C.H. and Wong, G.K. J. Opt. Soc. Am. B. 7, 902 (1990).Google Scholar
6. Schatz, G.C. and Ratner, M.A., Ouantum Mechanics in Chemistry, Prentice-Hall (1993) p.297.Google Scholar
7. (a) Yam, R., Berkovic, G., Langmuir 9, 2109 (1993). (b) W.M.K.P. Wijekoon, Z.Z. Ho, M.W. Mull, G.G. Padmabandu, W.M. Hethrington, J. Phys. Chem. 96, 10450 (1992). (c) D.A. Higgins, M.B. Abrams, S.K. Byerly, R.M. Corn, Langmuir 8, 1994 (1992).Google Scholar
8. Kanis, D.R., Ratner, M.A. and Marks, T.J., Chem. Mat. 3, 19 (1991).Google Scholar
9. Kanis, D.R., Ratner, M.A. and Marks, T.J., Int. J. Quantum Chem. 43, 61 (1992).Google Scholar
10. Kanis, D.R., Ratner, M.A. and Marks, T.J., Chem. Rev. 94, 195 (1994)Google Scholar
11. Heinz, T.F., Tom, H.W.K., and Shen, Y.R., Phys. Rev. A. 28, 1883 (1983).Google Scholar
12. Zhang, T.G., Zhang, C.H., and Wong, G.K., J. Opt. Soc. Am. B 7, 902 (1990).Google Scholar
13. Oudar, J.L., J. Chem. Phys. 67, 446 (1977).Google Scholar
14. Oudar, J.L. and Chemla, D.S., J. Chem. Phys. 66, 2664 (1977).Google Scholar