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  • Vol. 19, Iss. 11 — Jun. 1, 1994
  • pp: 786–788

Origin of negative χ(3) in squaraines: experimental observation of two-photon states

Y. Z. Yu, R. F. Shi, A. F. Garito, and C. H. Grossman  »View Author Affiliations


Optics Letters, Vol. 19, Issue 11, pp. 786-788 (1994)
http://dx.doi.org/10.1364/OL.19.000786


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Abstract

Femtosecond pump–probe experiments performed on squaraines demonstrate strong couplings between the first excited state and high-lying two-photon states. The experimental data agree well with our earlier quantum many-electron calculations based on multiple-excited configuration interactions. We show that high-lying two-photon states in squaraines are critically important to understanding the observed third-order optical properties and that two-level models are inadequate even for molecules with negative third-order optical susceptibilities.

© 1994 Optical Society of America

History
Original Manuscript: January 3, 1994
Published: June 1, 1994

Citation
Y. Z. Yu, C. H. Grossman, R. F. Shi, and A. F. Garito, "Origin of negative χ(3) in squaraines: experimental observation of two-photon states," Opt. Lett. 19, 786-788 (1994)
http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-19-11-786


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References

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