OSA's Digital Library

Journal of the Optical Society of America B

Journal of the Optical Society of America B

| OPTICAL PHYSICS

  • Vol. 12, Iss. 12 — Dec. 1, 1995
  • pp: 2360–2371

Characterization of excited states of centrosymmetric and noncentrosymmetric squaraines by third-harmonic spectral dispersion

James H. Andrews, John D. V. Khaydarov, Kenneth D. Singer, Diana L. Hull, and Kathy C. Chuang  »View Author Affiliations


JOSA B, Vol. 12, Issue 12, pp. 2360-2371 (1995)
http://dx.doi.org/10.1364/JOSAB.12.002360


View Full Text Article

Enhanced HTML    Acrobat PDF (531 KB)





Browse Journals / Lookup Meetings

Browse by Journal and Year


   


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools

Share
Citations

Abstract

We measured the third-harmonic spectrum for each of four squaraine dyes in chloroform. By fitting the experimental dispersion of the third-order susceptibility, γ, to a four-level sum-over-states model, we determine the strength and the location of the lowest-lying two-photon-like transition. In each case, we find that the lowest two-photon-like state appears just above the dominant linear absorption peak in energy and that the transition moment to that state makes a significant contribution to the nonlinearity, as do transition moments to one or more higher-lying two-photon-like states in the ultraviolet. The spectra of two of these dyes contain additional features, evidencing a nonzero dipole moment difference between the ground and the first excited-state dipole moments that we attribute to asymmetry in their structures. From our measurements, we also predict the dispersion of the real and the imaginary optical Kerr susceptibilities in the near infrared for two of these dyes.

© 1995 Optical Society of America

Citation
James H. Andrews, John D. V. Khaydarov, Kenneth D. Singer, Diana L. Hull, and Kathy C. Chuang, "Characterization of excited states of centrosymmetric and noncentrosymmetric squaraines by third-harmonic spectral dispersion," J. Opt. Soc. Am. B 12, 2360-2371 (1995)
http://www.opticsinfobase.org/josab/abstract.cfm?URI=josab-12-12-2360


Sort:  Author  |  Year  |  Journal  |  Reset  

References

  1. K. D. Singer and J. H. Andrews, "Quadratic nonlinear optics in poled polymer films: From physics to devices," in Molecular Nonlinear Optics: Materials, Physics, and Devices, J. Zyss, ed. (Academic, New York, 1994), pp. 245–298.
  2. K. D. Singer, J. E. Sohn, L. A. King, H. M. Gordon, H. E. Katz, and C. W. Dirk, "Second-order nonlinear-optical properties of donor- and acceptor-substituted aromatic compounds," J. Opt. Soc. Am. B 6, 1339–1350 (1989). [CrossRef]
  3. J. W. Wu, J. R. Heflin, R. A. Norwood, K. Y. Wong, O. Zamani-Khamiri, A. F. Garito, P. Kalyanaraman, and J. Sounik, "Nonlinear-optical processes in lower-dimensional conjugated structures," J. Opt. Soc. Am. B 6, 707–720 (1989). [CrossRef]
  4. B. M. Pierce, "A theoretical analysis of the third-order nonlinear optical properties of linear cyanines and polyenes," in Nonlinear Optical Properties of Organic Materials IV, K. D. Singer, ed., Proc. Soc. Photo-Opt. Instrum. Eng. 1560, 148–161 (1991). [CrossRef]
  5. M. G. Kuzyk and C. W. Dirk, "Effects of centrosymmetry on the nonresonant electronic third-order nonlinear optical susceptibility," Phys. Rev. A 41, 5098–5109 (1990). [CrossRef] [PubMed]
  6. C. W. Dirk, W. C. Herndon, F. Cervantes-Lee, H. Selnau, S. Martinez, P. Kalamegham, A. Tan, G. Campos, M. Velez, J. Zyss, I. Ledoux, and L.-T. Cheng, "Squarilium dyes: structural factors pertaining to the negative third-order nonlinear optical response," J. Am. Chem. Soc. 117, 2214–2225 (1995). [CrossRef]
  7. J. R. Heflin, Y. M. Cai, and A. F. Garito, "Dispersion measurements of electric-field-induced second-harmonic generation and third-harmonic generation in conjugated linear chains," J. Opt. Soc. Am. B 8, 2132–2147 (1991). [CrossRef]
  8. J. R. Heflin, D. C. Rodenberger, R. F. Shi, M. Wu, N. Q. Wang, Y. M. Cai, and A. F. Garito, "Experimental observation of enhanced nonresonant nonlinear optical responses from optically pumped electronic excited states," Phys. Rev. A 45, R4233–R4236 (1992). [CrossRef]
  9. Y. Z. Yu, R. F. Shi, A. F. Garito, and C. H. Grossman, "Origin of negative x(3) in squaraines: experimental observation of two-photon state," Opt. Lett. 19, 786–788 (1994). [CrossRef] [PubMed]
  10. S. Aramaki, W. Torruellas, R. Zanoni, and G. I. Stegeman, "Tunable third harmonic generation of trans-β–carotene," Opt. Commun. 85, 527–535 (1991). [CrossRef]
  11. M. G. Kuzyk, J. E. Sohn, and C. W. Dirk, "Mechanisms of quadratic electro-optic modulation of dye doped polymer systems," J. Opt. Soc. Am. B 7, 842–858 (1990). [CrossRef]
  12. C. W. Dirk and M. G. Kuzyk, "Squarilium dye-doped polymer systems as quadratic electrooptic materials," Chem. Mater. 2, 4–6 (1990). [CrossRef]
  13. J. H. Andrews, J. D. V. Khaydarov, and K. D. Singer, "Contribution of the 2Ag state to the third-order optical nonlinearity in a squaraine dye," Opt. Lett. 19, 984–986, "Errata," 19, 1909 (1994).
  14. J. H. Andrews, J. D. V. Khaydarov, K. D. Singer, D. L. Hull, and K. C. Chuang, "Spectral dispersion of third harmonic generation in squaraines," Nonlinear Opt. 10, 227 (1995).
  15. Q. L. Zhou, R. F. Shi, O. Zamani-Khamari, and A. F. Garito, "Negative third-order optical responses in squaraines," Nonlinear Opt. 6, 145–154 (1993).
  16. D. Guo, S. Mazumdar, G. I. Stegeman, M. Cha, D. Neher, S. Aramaki, W. Torruellas, and R. Zanoni, "Nonlinear optics of linear conjugated polymers," in Vol. 247 of Symposium Proceedings of the Materials Research Society (Materials Research Society, Pittsburgh, Pa., 1992), pp. 151–162. [CrossRef]
  17. F. Meyers, S. R. Marder, B. M. Pierce, and J. L. Bredas, "Electric field modulated nonlinear optical properties of donor-acceptor polyenes: sum-over-states investigation of the relationship between molecular polarizabilities (α, β, and ϒ) and bond length alternation," J. Am. Chem. Soc. 116, 10703–10714 (1994). [CrossRef]
  18. S. Etemad, G. L. Baker, and Z. G. Soos, "Third-order NLO processes in polydiacetylenes: physics, materials, and devices," in Molecular Nonlinear Optics: Materials, Physics, and Devices (Academic, New York, 1994), 433–465.
  19. S. R. Marder, C. B. Gorman, L.-T. Cheng, and B. G. Tiemann, "Optimizing the second-order optical nonlinearities of organic molecules: asymmetric cyanines and highly polarized polyenes," in Nonlinear Optical Properties of Organic Materials V, D. J. Williams, ed., Proc. Soc. Photo-Opt. Instrum. Eng. 1775, 19–31 (1992). [CrossRef]
  20. R. W. Bigelow and H.-J. Freund, "An MNDO and CNDO/S(S+ DES CI) study of the structural and electronic properties of a model squaraine dye and related cyanine," Chem. Phys. 107, 159–174 (1986). [CrossRef]
  21. C. W. Dirk, H. E. Katz, M. L. Schilling, and L. A. King, "Use of thiazole rings to enhance molecular second-order nonlinear optical susceptibilities," Chem. Mater. 2, 700–705 (1990); "Errata," 3, 207 (1991). [CrossRef]
  22. C. Poga, M. G. Kuzyk, S. Martinez, and C. W. Dirk, "Quadratic electroabsorption spectroscopy as a probe of x(3) mechanisms in dye-doped polymers," in Nonlinear Optical Properties of Organic Materials VI, G. R. Moehlmann, ed., Proc. Soc. Photo-Opt. Instrum. Eng. 2025, 363–372 (1993). [CrossRef]
  23. C. Poga, T. M. Brown, M. G. Kuzyk, and C. W. Dirk, "Characterization of the excited states of a squaraine molecule with quadratic electroabsorption spectroscopy," J. Opt. Soc. Am. B 12, 531–543 (1995). [CrossRef]
  24. A. Agnesi, G. C. Reali, V. Kubecek, S. Kumazaki, Y. Takagi, and K. Yoshihara, "β-barium borate and lithium triborate picosecond parametric oscillators pumped by a frequencytripled passive negative-feedback mode-locked Nd:YAG laser," J. Opt. Soc. Am. B 10, 2211–2217 (1993). [CrossRef]
  25. J. D. V. Khaydarov, J. H. Andrews, and K. D. Singer, "Pulse compression in a synchronously pumped optical parametric oscillator due to group velocity mismatch," Opt. Lett. 19, 831–833 (1994). [CrossRef] [PubMed]
  26. J. D. V. Khaydarov, J. H. Andrews, and K. D. Singer, "20-fold pulse compression in a synchronously pumped optical parametric oscillator," Appl. Phys. Lett. 65, 1614–1616 (1994). [CrossRef]
  27. J. D. V. Khaydarov, J. H. Andrews, and K. D. Singer, "Pulse-compression mechanism in a synchronously pumped optical parametric oscillator," J. Opt. Soc. Am. B 2199–2208 (1995). [CrossRef]
  28. F. Kajzar and J. Messier, "Original technique for third-harmonic-generation measurements in liquids," Rev. Sci. Instrum. 58, 2081–2085 (1987). [CrossRef]
  29. Optical Glass, Schott Glass Technologies Inc. catalog (Schott Glass, Duryea, Pa., 1990).
  30. V. Mizrahi, K. W. DeLong, G. I. Stegeman, M. A. Saifi, and M. J. Andrejco, "Two-photon absorption as a limitation to all-optical switching," Opt. Lett. 14, 1140–1142 (1989). [CrossRef] [PubMed]
  31. F. Kajzar, S. Etemad, G. L. Baker, and J. Messier, "Frequency dependence of the large, electronic x(3) in polyacetylene," Solid State Commun. 63, 1113–1117 (1987). [CrossRef]
  32. S. R. Marder, J. W. Perry, G. Bourhill, C. B. Gorman, B. G. Tiemann, and K. Mansour, "Relation between bond-length alternation and second electronic hyperpolarizability of conjugated organic molecules," Science 261, 186–189 (1993). [CrossRef] [PubMed]
  33. S. R. Marder, J. W. Perry, B. G. Tiemann, S. Gilmour, S. L. Biddle, G. Bourhill, and C. B. Gorman, "Direct observation of reduced bond length alternation in donor/acceptor polyenes," J. Am. Chem. Soc. 115, 2524–2526 (1993). [CrossRef]
  34. S. R. Marder, C. B. Gorman, B. G. Tiemann, and L.-T. Cheng, "Stronger acceptors can diminish nonlinear optical response in simple donor-acceptor polyenes," J. Am. Chem. Soc. 115, 3006–3007 (1993). [CrossRef]
  35. C. C. Teng and A. F. Garito, "Dispersion of the second-order optical susceptibility of organic systems," Phys. Rev. B 28, 6766–6773 (1983). [CrossRef]

Cited By

Alert me when this paper is cited

OSA is able to provide readers links to articles that cite this paper by participating in CrossRef's Cited-By Linking service. CrossRef includes content from more than 3000 publishers and societies. In addition to listing OSA journal articles that cite this paper, citing articles from other participating publishers will also be listed.


« Previous Article  |  Next Article »

OSA is a member of CrossRef.

CrossCheck Deposited