Abstract

Picosecond measurements of the optical response of chloroaluminum phthalocyanine in solutions are presented. The observed nonlinearities are modeled and interpreted theoretically by rate-equation and density-matrix techniques within a three-level model. Single-pulse power limiting is observed at 532 nm, and the absorption cross section of the first excited state is determined to be 15 times that of the ground state. From time-resolved excitation–probe measurements we determine an excited-state recombination time of 7 ns and a reorientational time of 7 ps. Further, the observation of the associated optical coherence effects, which are manifested as a negative coherent artifact, allow us to obtain an 8ps coherence time.

© 1997 Optical Society of America

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  1. D. R. Coulter, V. M. Miskowski, J. W. Perry, T. Wei, E. W. Van Stryland, and D. J. Hagan, “Optical limiting in solutions of metallo-phthalocyanines and naphthalocyanines,” in Materials for Optical Switches, Isolators, and Limiters, M. J. Soileau, ed., Proc. SPIE1105, 42 (1989).
    [CrossRef]
  2. J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.
  3. Y. B. Band, “Optical properties and applications of reverse saturable absorbers,” in Proceedings of Fritz Harz International Symposium (Plenum, New York, 1985), p. 23.
  4. D. J. Harter, M. L. Shand, and Y. B. Band, “Power/energy limiter using reverse saturable absorption,” J. Appl. Phys. 56, 865 (1984).
    [CrossRef]
  5. G. R. Allan, D. R. Labergerie, S. J. Rychnovsky, T. F. Boggess, A. L. Smirl, and L. Tutt, “Picosecond reverse saturable absorption in King’s complex (C5H5Fe(CO))4,” J. Phys. Chem. 96, 631 (1992).
    [CrossRef]
  6. M. P. Joshi, S. R. Mishra, H. S. Rawat, S. C. Mehendale, and K. C. Rustagi, “Investigation of optical limiting in C 60 solution,” Appl. Phys. Lett. 62, 1763 (1993).
    [CrossRef]
  7. W. Blau, H. Byrne, W. M. Dennis, and J. Kelly, “Reverse saturable absorption in tetraphenyporphyrins,” Opt. Commun. 56, 1985 (1993).
  8. J. M. Burzler, S. Hughes, and B. S. Wherrett, “Split-step Fourier methods applied to model nonlinear refractive effects in optically thick media,” Appl. Phys. B 62, 389 (1996).
    [CrossRef]
  9. T. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, “Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines,” Appl. Phys. B 46–51, 46 (1992).
    [CrossRef]
  10. A. A. Said, T. H. Wei, R. Desalvo, Z. Wang, M. Sheik-Bahae, D. J. Hagan, and E. W. Van Stryland, “Self-protecting optical limiters using cascading geometries,” in Nonlinear and Electro-Optic Materials for Optical Switching, M. Soileau, ed., Proc. SPIE1692, 37 (1992).
    [CrossRef]
  11. S. Hughes, J. M. Burzler, G. Spruce, and B. S. Wherrett, “Fast Fourier transform techniques for efficient simulation of Z-scan measurements,” J. Opt. Soc. Am. B 12, 1888 (1995).
    [CrossRef]
  12. S. Hughes, “A novel computational technique for propagating picosecond, intense laser pulses through a multi-level system,” Opt. Commun. 132, 236 (1996).
    [CrossRef]
  13. S. Hughes, G. Spruce, B. S. Wherrett, K. R. Welford, and A. D. Lloyd, “The saturation limit to picosecond, induced absorption in dyes,” Opt. Commun. 100, 113 (1993).
    [CrossRef]
  14. S. Hughes and B. S. Wherrett, “Multi-level rate-equation analysis to explain the recent observations to optical limiting dyes,” Phys. Rev. A 54, 3546 (1996).
    [CrossRef] [PubMed]
  15. J. P. Lavoine, A. Boeglin, S. H. Lin, and A. A. Villaeys, “Coherence–population interdependence in nonlinear optics,” Phys. Rev. A 38, 2896 (1988).
    [CrossRef] [PubMed]
  16. B. S. Wherrett, A. L. Smirl, and T. F. Boggess, “Theory of degenerate four-wave mixing in picosecond excitation-probe experiments,” IEEE J. Quantum Electron. 19, 680 (1983).
    [CrossRef]
  17. R. Bavli and Y. B. Band, “Optical properties of a homogeneously broadened two-level system,” Phys. Rev. A 36, 5200 (1987).
    [CrossRef] [PubMed]
  18. S. Hughes, B. S. Wherrett, and G. Spruce, “Theory and analysis of excitation-probe measurements for induced absorptive three-level molecular systems,” J. Opt. Soc. Am. B (to be published).
  19. Z. Vardeny and J. Tauc, “Picosecond coherence coupling in the pump and probe technique,” Opt. Commun. 39, 396 (1981).
    [CrossRef]
  20. A. V. Jena and H. E. Lessing, “Coherent coupling in picosecond absorption experiments,” Appl. Phys. 19, 131 (1979).
    [CrossRef]
  21. B. Wilhelmi and J. Hermann, “Coherent interaction effects in probe pulse experiments,” Sov. J. Quantum Electron. 10, 1082 (1980).
    [CrossRef]

1996 (3)

J. M. Burzler, S. Hughes, and B. S. Wherrett, “Split-step Fourier methods applied to model nonlinear refractive effects in optically thick media,” Appl. Phys. B 62, 389 (1996).
[CrossRef]

S. Hughes, “A novel computational technique for propagating picosecond, intense laser pulses through a multi-level system,” Opt. Commun. 132, 236 (1996).
[CrossRef]

S. Hughes and B. S. Wherrett, “Multi-level rate-equation analysis to explain the recent observations to optical limiting dyes,” Phys. Rev. A 54, 3546 (1996).
[CrossRef] [PubMed]

1995 (1)

1993 (3)

S. Hughes, G. Spruce, B. S. Wherrett, K. R. Welford, and A. D. Lloyd, “The saturation limit to picosecond, induced absorption in dyes,” Opt. Commun. 100, 113 (1993).
[CrossRef]

M. P. Joshi, S. R. Mishra, H. S. Rawat, S. C. Mehendale, and K. C. Rustagi, “Investigation of optical limiting in C 60 solution,” Appl. Phys. Lett. 62, 1763 (1993).
[CrossRef]

W. Blau, H. Byrne, W. M. Dennis, and J. Kelly, “Reverse saturable absorption in tetraphenyporphyrins,” Opt. Commun. 56, 1985 (1993).

1992 (2)

G. R. Allan, D. R. Labergerie, S. J. Rychnovsky, T. F. Boggess, A. L. Smirl, and L. Tutt, “Picosecond reverse saturable absorption in King’s complex (C5H5Fe(CO))4,” J. Phys. Chem. 96, 631 (1992).
[CrossRef]

T. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, “Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines,” Appl. Phys. B 46–51, 46 (1992).
[CrossRef]

1988 (1)

J. P. Lavoine, A. Boeglin, S. H. Lin, and A. A. Villaeys, “Coherence–population interdependence in nonlinear optics,” Phys. Rev. A 38, 2896 (1988).
[CrossRef] [PubMed]

1987 (1)

R. Bavli and Y. B. Band, “Optical properties of a homogeneously broadened two-level system,” Phys. Rev. A 36, 5200 (1987).
[CrossRef] [PubMed]

1984 (1)

D. J. Harter, M. L. Shand, and Y. B. Band, “Power/energy limiter using reverse saturable absorption,” J. Appl. Phys. 56, 865 (1984).
[CrossRef]

1983 (1)

B. S. Wherrett, A. L. Smirl, and T. F. Boggess, “Theory of degenerate four-wave mixing in picosecond excitation-probe experiments,” IEEE J. Quantum Electron. 19, 680 (1983).
[CrossRef]

1981 (1)

Z. Vardeny and J. Tauc, “Picosecond coherence coupling in the pump and probe technique,” Opt. Commun. 39, 396 (1981).
[CrossRef]

1980 (1)

B. Wilhelmi and J. Hermann, “Coherent interaction effects in probe pulse experiments,” Sov. J. Quantum Electron. 10, 1082 (1980).
[CrossRef]

1979 (1)

A. V. Jena and H. E. Lessing, “Coherent coupling in picosecond absorption experiments,” Appl. Phys. 19, 131 (1979).
[CrossRef]

Allan, G. R.

G. R. Allan, D. R. Labergerie, S. J. Rychnovsky, T. F. Boggess, A. L. Smirl, and L. Tutt, “Picosecond reverse saturable absorption in King’s complex (C5H5Fe(CO))4,” J. Phys. Chem. 96, 631 (1992).
[CrossRef]

Alverez, J. D.

J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.

Band, Y. B.

R. Bavli and Y. B. Band, “Optical properties of a homogeneously broadened two-level system,” Phys. Rev. A 36, 5200 (1987).
[CrossRef] [PubMed]

D. J. Harter, M. L. Shand, and Y. B. Band, “Power/energy limiter using reverse saturable absorption,” J. Appl. Phys. 56, 865 (1984).
[CrossRef]

Y. B. Band, “Optical properties and applications of reverse saturable absorbers,” in Proceedings of Fritz Harz International Symposium (Plenum, New York, 1985), p. 23.

Bavli, R.

R. Bavli and Y. B. Band, “Optical properties of a homogeneously broadened two-level system,” Phys. Rev. A 36, 5200 (1987).
[CrossRef] [PubMed]

Blau, W.

W. Blau, H. Byrne, W. M. Dennis, and J. Kelly, “Reverse saturable absorption in tetraphenyporphyrins,” Opt. Commun. 56, 1985 (1993).

Boeglin, A.

J. P. Lavoine, A. Boeglin, S. H. Lin, and A. A. Villaeys, “Coherence–population interdependence in nonlinear optics,” Phys. Rev. A 38, 2896 (1988).
[CrossRef] [PubMed]

Boggess, T. F.

G. R. Allan, D. R. Labergerie, S. J. Rychnovsky, T. F. Boggess, A. L. Smirl, and L. Tutt, “Picosecond reverse saturable absorption in King’s complex (C5H5Fe(CO))4,” J. Phys. Chem. 96, 631 (1992).
[CrossRef]

B. S. Wherrett, A. L. Smirl, and T. F. Boggess, “Theory of degenerate four-wave mixing in picosecond excitation-probe experiments,” IEEE J. Quantum Electron. 19, 680 (1983).
[CrossRef]

Burzler, J. M.

J. M. Burzler, S. Hughes, and B. S. Wherrett, “Split-step Fourier methods applied to model nonlinear refractive effects in optically thick media,” Appl. Phys. B 62, 389 (1996).
[CrossRef]

S. Hughes, J. M. Burzler, G. Spruce, and B. S. Wherrett, “Fast Fourier transform techniques for efficient simulation of Z-scan measurements,” J. Opt. Soc. Am. B 12, 1888 (1995).
[CrossRef]

Byrne, H.

W. Blau, H. Byrne, W. M. Dennis, and J. Kelly, “Reverse saturable absorption in tetraphenyporphyrins,” Opt. Commun. 56, 1985 (1993).

Coulter, D. R.

T. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, “Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines,” Appl. Phys. B 46–51, 46 (1992).
[CrossRef]

J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.

D. R. Coulter, V. M. Miskowski, J. W. Perry, T. Wei, E. W. Van Stryland, and D. J. Hagan, “Optical limiting in solutions of metallo-phthalocyanines and naphthalocyanines,” in Materials for Optical Switches, Isolators, and Limiters, M. J. Soileau, ed., Proc. SPIE1105, 42 (1989).
[CrossRef]

Dennis, W. M.

W. Blau, H. Byrne, W. M. Dennis, and J. Kelly, “Reverse saturable absorption in tetraphenyporphyrins,” Opt. Commun. 56, 1985 (1993).

Desalvo, R.

A. A. Said, T. H. Wei, R. Desalvo, Z. Wang, M. Sheik-Bahae, D. J. Hagan, and E. W. Van Stryland, “Self-protecting optical limiters using cascading geometries,” in Nonlinear and Electro-Optic Materials for Optical Switching, M. Soileau, ed., Proc. SPIE1692, 37 (1992).
[CrossRef]

Hagan, D.

J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.

Hagan, D. J.

T. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, “Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines,” Appl. Phys. B 46–51, 46 (1992).
[CrossRef]

A. A. Said, T. H. Wei, R. Desalvo, Z. Wang, M. Sheik-Bahae, D. J. Hagan, and E. W. Van Stryland, “Self-protecting optical limiters using cascading geometries,” in Nonlinear and Electro-Optic Materials for Optical Switching, M. Soileau, ed., Proc. SPIE1692, 37 (1992).
[CrossRef]

D. R. Coulter, V. M. Miskowski, J. W. Perry, T. Wei, E. W. Van Stryland, and D. J. Hagan, “Optical limiting in solutions of metallo-phthalocyanines and naphthalocyanines,” in Materials for Optical Switches, Isolators, and Limiters, M. J. Soileau, ed., Proc. SPIE1105, 42 (1989).
[CrossRef]

Harter, D. J.

D. J. Harter, M. L. Shand, and Y. B. Band, “Power/energy limiter using reverse saturable absorption,” J. Appl. Phys. 56, 865 (1984).
[CrossRef]

Hermann, J.

B. Wilhelmi and J. Hermann, “Coherent interaction effects in probe pulse experiments,” Sov. J. Quantum Electron. 10, 1082 (1980).
[CrossRef]

Hughes, S.

J. M. Burzler, S. Hughes, and B. S. Wherrett, “Split-step Fourier methods applied to model nonlinear refractive effects in optically thick media,” Appl. Phys. B 62, 389 (1996).
[CrossRef]

S. Hughes, “A novel computational technique for propagating picosecond, intense laser pulses through a multi-level system,” Opt. Commun. 132, 236 (1996).
[CrossRef]

S. Hughes and B. S. Wherrett, “Multi-level rate-equation analysis to explain the recent observations to optical limiting dyes,” Phys. Rev. A 54, 3546 (1996).
[CrossRef] [PubMed]

S. Hughes, J. M. Burzler, G. Spruce, and B. S. Wherrett, “Fast Fourier transform techniques for efficient simulation of Z-scan measurements,” J. Opt. Soc. Am. B 12, 1888 (1995).
[CrossRef]

S. Hughes, G. Spruce, B. S. Wherrett, K. R. Welford, and A. D. Lloyd, “The saturation limit to picosecond, induced absorption in dyes,” Opt. Commun. 100, 113 (1993).
[CrossRef]

S. Hughes, B. S. Wherrett, and G. Spruce, “Theory and analysis of excitation-probe measurements for induced absorptive three-level molecular systems,” J. Opt. Soc. Am. B (to be published).

Jena, A. V.

A. V. Jena and H. E. Lessing, “Coherent coupling in picosecond absorption experiments,” Appl. Phys. 19, 131 (1979).
[CrossRef]

Joshi, M. P.

M. P. Joshi, S. R. Mishra, H. S. Rawat, S. C. Mehendale, and K. C. Rustagi, “Investigation of optical limiting in C 60 solution,” Appl. Phys. Lett. 62, 1763 (1993).
[CrossRef]

Kelly, J.

W. Blau, H. Byrne, W. M. Dennis, and J. Kelly, “Reverse saturable absorption in tetraphenyporphyrins,” Opt. Commun. 56, 1985 (1993).

Khundkar, L. R.

J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.

Labergerie, D. R.

G. R. Allan, D. R. Labergerie, S. J. Rychnovsky, T. F. Boggess, A. L. Smirl, and L. Tutt, “Picosecond reverse saturable absorption in King’s complex (C5H5Fe(CO))4,” J. Phys. Chem. 96, 631 (1992).
[CrossRef]

Lavoine, J. P.

J. P. Lavoine, A. Boeglin, S. H. Lin, and A. A. Villaeys, “Coherence–population interdependence in nonlinear optics,” Phys. Rev. A 38, 2896 (1988).
[CrossRef] [PubMed]

Lessing, H. E.

A. V. Jena and H. E. Lessing, “Coherent coupling in picosecond absorption experiments,” Appl. Phys. 19, 131 (1979).
[CrossRef]

Lin, S. H.

J. P. Lavoine, A. Boeglin, S. H. Lin, and A. A. Villaeys, “Coherence–population interdependence in nonlinear optics,” Phys. Rev. A 38, 2896 (1988).
[CrossRef] [PubMed]

Lloyd, A. D.

S. Hughes, G. Spruce, B. S. Wherrett, K. R. Welford, and A. D. Lloyd, “The saturation limit to picosecond, induced absorption in dyes,” Opt. Commun. 100, 113 (1993).
[CrossRef]

Marder, S. R.

J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.

Mehendale, S. C.

M. P. Joshi, S. R. Mishra, H. S. Rawat, S. C. Mehendale, and K. C. Rustagi, “Investigation of optical limiting in C 60 solution,” Appl. Phys. Lett. 62, 1763 (1993).
[CrossRef]

Mishra, S. R.

M. P. Joshi, S. R. Mishra, H. S. Rawat, S. C. Mehendale, and K. C. Rustagi, “Investigation of optical limiting in C 60 solution,” Appl. Phys. Lett. 62, 1763 (1993).
[CrossRef]

Miskowski, V. M.

D. R. Coulter, V. M. Miskowski, J. W. Perry, T. Wei, E. W. Van Stryland, and D. J. Hagan, “Optical limiting in solutions of metallo-phthalocyanines and naphthalocyanines,” in Materials for Optical Switches, Isolators, and Limiters, M. J. Soileau, ed., Proc. SPIE1105, 42 (1989).
[CrossRef]

Perry, J. W.

T. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, “Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines,” Appl. Phys. B 46–51, 46 (1992).
[CrossRef]

D. R. Coulter, V. M. Miskowski, J. W. Perry, T. Wei, E. W. Van Stryland, and D. J. Hagan, “Optical limiting in solutions of metallo-phthalocyanines and naphthalocyanines,” in Materials for Optical Switches, Isolators, and Limiters, M. J. Soileau, ed., Proc. SPIE1105, 42 (1989).
[CrossRef]

J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.

Rawat, H. S.

M. P. Joshi, S. R. Mishra, H. S. Rawat, S. C. Mehendale, and K. C. Rustagi, “Investigation of optical limiting in C 60 solution,” Appl. Phys. Lett. 62, 1763 (1993).
[CrossRef]

Rustagi, K. C.

M. P. Joshi, S. R. Mishra, H. S. Rawat, S. C. Mehendale, and K. C. Rustagi, “Investigation of optical limiting in C 60 solution,” Appl. Phys. Lett. 62, 1763 (1993).
[CrossRef]

Rychnovsky, S. J.

G. R. Allan, D. R. Labergerie, S. J. Rychnovsky, T. F. Boggess, A. L. Smirl, and L. Tutt, “Picosecond reverse saturable absorption in King’s complex (C5H5Fe(CO))4,” J. Phys. Chem. 96, 631 (1992).
[CrossRef]

Said, A. A.

A. A. Said, T. H. Wei, R. Desalvo, Z. Wang, M. Sheik-Bahae, D. J. Hagan, and E. W. Van Stryland, “Self-protecting optical limiters using cascading geometries,” in Nonlinear and Electro-Optic Materials for Optical Switching, M. Soileau, ed., Proc. SPIE1692, 37 (1992).
[CrossRef]

Sence, M.

J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.

Sence, M. J.

T. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, “Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines,” Appl. Phys. B 46–51, 46 (1992).
[CrossRef]

Shand, M. L.

D. J. Harter, M. L. Shand, and Y. B. Band, “Power/energy limiter using reverse saturable absorption,” J. Appl. Phys. 56, 865 (1984).
[CrossRef]

Sheik-Bahae, M.

A. A. Said, T. H. Wei, R. Desalvo, Z. Wang, M. Sheik-Bahae, D. J. Hagan, and E. W. Van Stryland, “Self-protecting optical limiters using cascading geometries,” in Nonlinear and Electro-Optic Materials for Optical Switching, M. Soileau, ed., Proc. SPIE1692, 37 (1992).
[CrossRef]

Smirl, A. L.

G. R. Allan, D. R. Labergerie, S. J. Rychnovsky, T. F. Boggess, A. L. Smirl, and L. Tutt, “Picosecond reverse saturable absorption in King’s complex (C5H5Fe(CO))4,” J. Phys. Chem. 96, 631 (1992).
[CrossRef]

B. S. Wherrett, A. L. Smirl, and T. F. Boggess, “Theory of degenerate four-wave mixing in picosecond excitation-probe experiments,” IEEE J. Quantum Electron. 19, 680 (1983).
[CrossRef]

Spruce, G.

S. Hughes, J. M. Burzler, G. Spruce, and B. S. Wherrett, “Fast Fourier transform techniques for efficient simulation of Z-scan measurements,” J. Opt. Soc. Am. B 12, 1888 (1995).
[CrossRef]

S. Hughes, G. Spruce, B. S. Wherrett, K. R. Welford, and A. D. Lloyd, “The saturation limit to picosecond, induced absorption in dyes,” Opt. Commun. 100, 113 (1993).
[CrossRef]

S. Hughes, B. S. Wherrett, and G. Spruce, “Theory and analysis of excitation-probe measurements for induced absorptive three-level molecular systems,” J. Opt. Soc. Am. B (to be published).

Stryland, E. W. Van

T. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, “Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines,” Appl. Phys. B 46–51, 46 (1992).
[CrossRef]

Tauc, J.

Z. Vardeny and J. Tauc, “Picosecond coherence coupling in the pump and probe technique,” Opt. Commun. 39, 396 (1981).
[CrossRef]

Tutt, L.

G. R. Allan, D. R. Labergerie, S. J. Rychnovsky, T. F. Boggess, A. L. Smirl, and L. Tutt, “Picosecond reverse saturable absorption in King’s complex (C5H5Fe(CO))4,” J. Phys. Chem. 96, 631 (1992).
[CrossRef]

Van Stryland, E. W.

J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.

D. R. Coulter, V. M. Miskowski, J. W. Perry, T. Wei, E. W. Van Stryland, and D. J. Hagan, “Optical limiting in solutions of metallo-phthalocyanines and naphthalocyanines,” in Materials for Optical Switches, Isolators, and Limiters, M. J. Soileau, ed., Proc. SPIE1105, 42 (1989).
[CrossRef]

A. A. Said, T. H. Wei, R. Desalvo, Z. Wang, M. Sheik-Bahae, D. J. Hagan, and E. W. Van Stryland, “Self-protecting optical limiters using cascading geometries,” in Nonlinear and Electro-Optic Materials for Optical Switching, M. Soileau, ed., Proc. SPIE1692, 37 (1992).
[CrossRef]

Vardeny, Z.

Z. Vardeny and J. Tauc, “Picosecond coherence coupling in the pump and probe technique,” Opt. Commun. 39, 396 (1981).
[CrossRef]

Villaeys, A. A.

J. P. Lavoine, A. Boeglin, S. H. Lin, and A. A. Villaeys, “Coherence–population interdependence in nonlinear optics,” Phys. Rev. A 38, 2896 (1988).
[CrossRef] [PubMed]

Wang, Z.

A. A. Said, T. H. Wei, R. Desalvo, Z. Wang, M. Sheik-Bahae, D. J. Hagan, and E. W. Van Stryland, “Self-protecting optical limiters using cascading geometries,” in Nonlinear and Electro-Optic Materials for Optical Switching, M. Soileau, ed., Proc. SPIE1692, 37 (1992).
[CrossRef]

Wei, T.

T. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, “Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines,” Appl. Phys. B 46–51, 46 (1992).
[CrossRef]

D. R. Coulter, V. M. Miskowski, J. W. Perry, T. Wei, E. W. Van Stryland, and D. J. Hagan, “Optical limiting in solutions of metallo-phthalocyanines and naphthalocyanines,” in Materials for Optical Switches, Isolators, and Limiters, M. J. Soileau, ed., Proc. SPIE1105, 42 (1989).
[CrossRef]

J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.

Wei, T. H.

A. A. Said, T. H. Wei, R. Desalvo, Z. Wang, M. Sheik-Bahae, D. J. Hagan, and E. W. Van Stryland, “Self-protecting optical limiters using cascading geometries,” in Nonlinear and Electro-Optic Materials for Optical Switching, M. Soileau, ed., Proc. SPIE1692, 37 (1992).
[CrossRef]

Welford, K. R.

S. Hughes, G. Spruce, B. S. Wherrett, K. R. Welford, and A. D. Lloyd, “The saturation limit to picosecond, induced absorption in dyes,” Opt. Commun. 100, 113 (1993).
[CrossRef]

Wherrett, B. S.

S. Hughes and B. S. Wherrett, “Multi-level rate-equation analysis to explain the recent observations to optical limiting dyes,” Phys. Rev. A 54, 3546 (1996).
[CrossRef] [PubMed]

J. M. Burzler, S. Hughes, and B. S. Wherrett, “Split-step Fourier methods applied to model nonlinear refractive effects in optically thick media,” Appl. Phys. B 62, 389 (1996).
[CrossRef]

S. Hughes, J. M. Burzler, G. Spruce, and B. S. Wherrett, “Fast Fourier transform techniques for efficient simulation of Z-scan measurements,” J. Opt. Soc. Am. B 12, 1888 (1995).
[CrossRef]

S. Hughes, G. Spruce, B. S. Wherrett, K. R. Welford, and A. D. Lloyd, “The saturation limit to picosecond, induced absorption in dyes,” Opt. Commun. 100, 113 (1993).
[CrossRef]

B. S. Wherrett, A. L. Smirl, and T. F. Boggess, “Theory of degenerate four-wave mixing in picosecond excitation-probe experiments,” IEEE J. Quantum Electron. 19, 680 (1983).
[CrossRef]

S. Hughes, B. S. Wherrett, and G. Spruce, “Theory and analysis of excitation-probe measurements for induced absorptive three-level molecular systems,” J. Opt. Soc. Am. B (to be published).

Wilhelmi, B.

B. Wilhelmi and J. Hermann, “Coherent interaction effects in probe pulse experiments,” Sov. J. Quantum Electron. 10, 1082 (1980).
[CrossRef]

Appl. Phys. (1)

A. V. Jena and H. E. Lessing, “Coherent coupling in picosecond absorption experiments,” Appl. Phys. 19, 131 (1979).
[CrossRef]

Appl. Phys. B (2)

J. M. Burzler, S. Hughes, and B. S. Wherrett, “Split-step Fourier methods applied to model nonlinear refractive effects in optically thick media,” Appl. Phys. B 62, 389 (1996).
[CrossRef]

T. Wei, D. J. Hagan, M. J. Sence, E. W. Van Stryland, J. W. Perry, and D. R. Coulter, “Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines,” Appl. Phys. B 46–51, 46 (1992).
[CrossRef]

Appl. Phys. Lett. (1)

M. P. Joshi, S. R. Mishra, H. S. Rawat, S. C. Mehendale, and K. C. Rustagi, “Investigation of optical limiting in C 60 solution,” Appl. Phys. Lett. 62, 1763 (1993).
[CrossRef]

IEEE J. Quantum Electron. (1)

B. S. Wherrett, A. L. Smirl, and T. F. Boggess, “Theory of degenerate four-wave mixing in picosecond excitation-probe experiments,” IEEE J. Quantum Electron. 19, 680 (1983).
[CrossRef]

J. Appl. Phys. (1)

D. J. Harter, M. L. Shand, and Y. B. Band, “Power/energy limiter using reverse saturable absorption,” J. Appl. Phys. 56, 865 (1984).
[CrossRef]

J. Opt. Soc. Am. B (1)

J. Phys. Chem. (1)

G. R. Allan, D. R. Labergerie, S. J. Rychnovsky, T. F. Boggess, A. L. Smirl, and L. Tutt, “Picosecond reverse saturable absorption in King’s complex (C5H5Fe(CO))4,” J. Phys. Chem. 96, 631 (1992).
[CrossRef]

Opt. Commun. (4)

W. Blau, H. Byrne, W. M. Dennis, and J. Kelly, “Reverse saturable absorption in tetraphenyporphyrins,” Opt. Commun. 56, 1985 (1993).

S. Hughes, “A novel computational technique for propagating picosecond, intense laser pulses through a multi-level system,” Opt. Commun. 132, 236 (1996).
[CrossRef]

S. Hughes, G. Spruce, B. S. Wherrett, K. R. Welford, and A. D. Lloyd, “The saturation limit to picosecond, induced absorption in dyes,” Opt. Commun. 100, 113 (1993).
[CrossRef]

Z. Vardeny and J. Tauc, “Picosecond coherence coupling in the pump and probe technique,” Opt. Commun. 39, 396 (1981).
[CrossRef]

Phys. Rev. A (3)

S. Hughes and B. S. Wherrett, “Multi-level rate-equation analysis to explain the recent observations to optical limiting dyes,” Phys. Rev. A 54, 3546 (1996).
[CrossRef] [PubMed]

J. P. Lavoine, A. Boeglin, S. H. Lin, and A. A. Villaeys, “Coherence–population interdependence in nonlinear optics,” Phys. Rev. A 38, 2896 (1988).
[CrossRef] [PubMed]

R. Bavli and Y. B. Band, “Optical properties of a homogeneously broadened two-level system,” Phys. Rev. A 36, 5200 (1987).
[CrossRef] [PubMed]

Sov. J. Quantum Electron. (1)

B. Wilhelmi and J. Hermann, “Coherent interaction effects in probe pulse experiments,” Sov. J. Quantum Electron. 10, 1082 (1980).
[CrossRef]

Other (5)

S. Hughes, B. S. Wherrett, and G. Spruce, “Theory and analysis of excitation-probe measurements for induced absorptive three-level molecular systems,” J. Opt. Soc. Am. B (to be published).

A. A. Said, T. H. Wei, R. Desalvo, Z. Wang, M. Sheik-Bahae, D. J. Hagan, and E. W. Van Stryland, “Self-protecting optical limiters using cascading geometries,” in Nonlinear and Electro-Optic Materials for Optical Switching, M. Soileau, ed., Proc. SPIE1692, 37 (1992).
[CrossRef]

D. R. Coulter, V. M. Miskowski, J. W. Perry, T. Wei, E. W. Van Stryland, and D. J. Hagan, “Optical limiting in solutions of metallo-phthalocyanines and naphthalocyanines,” in Materials for Optical Switches, Isolators, and Limiters, M. J. Soileau, ed., Proc. SPIE1105, 42 (1989).
[CrossRef]

J. W. Perry, L. R. Khundkar, D. R. Coulter, J. D. Alverez, S. R. Marder, T. Wei, M. Sence, E. W. Van Stryland, and D. Hagan, “Excited state absorption and optical limiting in solutions of metallophthalocyanines,” in Organic Molecules for Nonlinear Optics and PhotonicsJ. Messier, F. Kajzar, and P. Prasad, eds. (Kluwer, Dordrecht, The Netherlands, 1991), p. 369.

Y. B. Band, “Optical properties and applications of reverse saturable absorbers,” in Proceedings of Fritz Harz International Symposium (Plenum, New York, 1985), p. 23.

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Figures (3)

Fig. 1
Fig. 1

Picosecond single-pulse transmittance measurement for a 5 mm CAP solution, demonstrating RSA for increasing input fluences. Also shown is the theoretical simulation (see text).

Fig. 2
Fig. 2

Time-resolved excitation–probe measurements for pulses polarized parallel to each other, with an excitation input fluence of 0.48 J cm-2. Also shown is the theoretical simulation. The measurements are plotted as differential transmittance, where Tp represents the transmittance of the probe beam without any excitation pulse. As an indication of the experimental errors involved on the data points, the differential transmittance may be ±0.015 and the time delay may be ±3 ps.

Fig. 3
Fig. 3

As in Fig. 2 but for a probe beam polarized crossed with respect to the excitation beam. The purely orientational grating does not contribute because the molecules possess a fast reorientational time.

Equations (15)

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N˙0=-N0σ10Iω+N1τ01,
N˙1=NT-N0,
dIdy=-I(N0σ10+N1σ21),
I=I0f(t)f(r)=I0 exp[-(t/τ0)2]exp[-(2r/ω0)2],
P(3)(ω, t, r)
=-NT3(ω-ω21)-iΓ21[(ω-ω21)2+Γ212]Γ10[(ω-ω10)2+Γ102]×|μ12|2|μ01|2 ijkl exp[i(kj-kk+kl)·r]׈iEj(ω, t) -t Ek*(ω, t)×El(ω, t)Aijkl(3)(t-t)dt,
Aijkl(3)(t)=Yij(1)Ykl(1)1-exp-tτor+Yijkl(3) exp-tτorexp-t1τ01+1τkl,
dEp(y)dy=-α02Ep(y)+ik20Pp(3)(ω, t, y),
ΔT=ΔTT=(Tnl-Tlin)Tlin,
ΔTback(3)=-K1 -|Ee(t-τd)|2 -t|Ee(t)|2Appee(3)×(t-t)dtdt+c.c.,
ΔTspike(3)=-K1 - Ee*(t-τd)Ee(t) -t Ee(t-τd)×Ee*(t)Apeep(3)(t-t)dtdt+c.c.,
K1=NTk320α0Γ21[(ω-ω21)2+Γ212]Γ10[(ω-ω10)2+Γ102]|μ12|2|μ01|2×0 exp[-(2r2/wp2+2r2/we2)]2πrdr0 exp[-(2r2/wp2)]2πrdr - Ep*(ω, t, 0)Ep(ω, t, 0)dt,
Azzzz(3)(t)=191-exp-tτor+15exp-tτor×exp-tτ01,
Axxzz3t=191-exp-tτor+115exp-tτor×exp-tτ01,
Axzxz3t=115exp-tτorexp-tτ01,

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