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Negative Third Order Optical Susceptibilities of Squaraines

Published online by Cambridge University Press:  16 February 2011

R. F. Shi
Affiliation:
Department of Physics, University of Pennsylvania, Philadelphia, PA 19104
Q. L. Zhou
Affiliation:
Department of Physics, University of Pennsylvania, Philadelphia, PA 19104
A. F. Garito
Affiliation:
Department of Physics, University of Pennsylvania, Philadelphia, PA 19104
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Abstract

Quantum Many-electron calculations based on Multiple-excited configuration interaction have been implemented on squaraine Molecules. It is found that certain squaraines possess negative third order optical susceptibilities (γ) even in the zero frequency limit. Our calculations agree well with the experimental results obtained by Dirk and co-workers[1] for anilinium squarylium (BSQ) in terms of the sign and Magnitude. High-lying two-photon states in squaraines are found to be always critically important. The sign of γ is found to depend on the electron donating ability of the two side groups in squaraines.

Type
Research Article
Copyright
Copyright © Materials Research Society 1994

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References

REFERENCES

[1] Dirk, C.W., Cheng, L-T., and Kuzyk, M.G., Mat. Res. Soc. Proc. 247, 73 (1992);Google Scholar
Dirk, C.W., Cheng, L-T., and Kuzyk, M.G., Int. J. Quant. Chem. 43, 27 (1992).Google Scholar
[2] Heflin, J.R., Wong, K.Y., Zamani-Khamiri, O., and Garito, A.F., Phys. Rev. B 38, 1573 (1988).Google Scholar
[3] Bigelow, R.W., and Freund, H., Chem. Phys. 107, 159 (1986).Google Scholar
[4] Kuzyk, M.G., Sohn, J.E., and Dirk, C.W., J.Opt. Soc. Am. B 7, 842 (1990); M.G. Kuzyk (Personal Communications).CrossRefGoogle Scholar
[5] Law, K.Y., J. Phys. Chem. 91, 5185 (1987).Google Scholar
[6] Heflin, J.R. and Garito, A.F., in Polymers for Lightwave and Integrated Optics, Hornak, L.A. ed., Marcel Dekker, 501 (1992).Google Scholar
[7] Zhou, Q.L., Shi, R.F., Zamani-Khamiri, O. and Garito, A.F., Nonlinear Optics (to appear Nov. 1993).Google Scholar
[8] Yu, Y.Z., Grossman, C.H., and Garito, A.F. (submitted).Google Scholar
[9] Singer, K.D., Kuzyk, M.K., and Sohn, J.E., Opt, J.. Soc. Am. B 6, 968 (1987).Google Scholar
[10] Marder, S.R., Perry, J.W., Bourhill, G., Gorman, C.B., Tiemann, B.G., and Mansour, K., Science, 261, 186 (1993).Google Scholar