Abstract

Degenerate four-wave mixing experiments (along with saturated absorption experiments) were carried out in and below the excitonic-state resonance in polydiacetylenes. A self-consistent analysis of the data was obtained with a two (electronic) level molecularlike model. The excitonic-state lifetime was determined to be 1.8 psec, and an initial excited-state process with a 100-fsec time constant was resolved. The time constant of the nonresonant third-order nonlinear-optical susceptibility was determined to be less than the resolution of the four-wave mixing experiment, -300 fsec, which was limited by the optical pulse duration.

© 1987 Optical Society of America

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    [Crossref]
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    [Crossref]
  3. M. Pope and C. E. Swenberg, Electronic Processes in Organic Crystals (Oxford U. Press, New York, 1982), pp. 677–696.
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    [Crossref]
  5. M. R. Philpott, Chem. Phys. Lett. 50, 18 (1977).
    [Crossref]
  6. Z. G. Soos, S. Mazumdar, and S. Kuwajima, in Solid State Polymerization: The Structure and Properties of Polymers Produced by Lattice Controlled Processes, D. J. Sandman, ed. (American Chemical Society, Washington, D.C., to be published).
  7. S. Mazumdar, National Chemical Laboratories, Pune, India (personal communication).
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    [Crossref]
  9. J. V. Hryniewicz, G. M. Carter, and Y. J. Chen, Opt. Commun. 54, 230 (1985).
    [Crossref]
  10. B. Nikolaus and D. Grischkowsky, Appl. Phys. Lett. 43, 228 (1983).
    [Crossref]
  11. A. M. Johnson, R. H. Stolen, and W. M. Simpson, Appl. Phys. Lett. 44, 729 (1984).
    [Crossref]
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    [Crossref]
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    [Crossref]
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1987 (1)

1986 (3)

G. M. Carter, J. V. Hryniewicz, M. K. Thakur, Y. J. Chen, and S. E. Meyler, Appl. Phys. Lett. 49, 998 (1986).
[Crossref]

D. N. Rao, P. Chopra, S. K. Ghoshal, J. Swiatkiewicz, and P. N. Prasad, J. Chem. Phys. 84, 7049 (1986).
[Crossref]

D. Cotter, Electron. Lett. 22, 093 (1986).
[Crossref]

1985 (3)

D. S. Chemla and D. A. B. Miller, J. Opt. Soc. Am. B 2, 1155 (1985).
[Crossref]

G. M. Carter, M. K. Thakur, Y. J. Chen, and J. V. Hryniewicz, Appl. Phys. Lett. 47, 457 (1985).
[Crossref]

J. V. Hryniewicz, G. M. Carter, and Y. J. Chen, Opt. Commun. 54, 230 (1985).
[Crossref]

1984 (1)

A. M. Johnson, R. H. Stolen, and W. M. Simpson, Appl. Phys. Lett. 44, 729 (1984).
[Crossref]

1983 (3)

B. Nikolaus and D. Grischkowsky, Appl. Phys. Lett. 43, 228 (1983).
[Crossref]

A. Lattes, H. A. Haus, F. J. Leonberger, and E. P. Ippen, IEEE J. Quantum Electron. QE-19, 1718 (1983).
[Crossref]

R. L. Fork, C. V. Shank, R. Yen, and C. A. Hirlimann, IEEE J. Quantum Electron. QE-19, 500 (1983).
[Crossref]

1981 (1)

L. Sebastian and G. Weiser, Chem. Phys. 62, 447 (1981).
[Crossref]

1980 (1)

1978 (3)

G. P. Agrawal, C. Cojan, and C. Flytzanis, Phys. Rev. B 17, 776 (1978).
[Crossref]

C. A. Hoffman, K. Jarasiunas, H. J. Gerritsen, and A. V. Nurmikko, Appl. Phys. Lett. 33, 536 (1978).
[Crossref]

C. V. Shank, E. P. Ippen, O. Teschke, and R. L. Fork, Chem. Phys. Lett. 57, 433 (1978).
[Crossref]

1977 (1)

M. R. Philpott, Chem. Phys. Lett. 50, 18 (1977).
[Crossref]

1976 (1)

C. Sauteret, J. P. Hermann, R. Frey, F. Pradere, J. Ducuing, R. H. Baughman, and R. R. Chance, Phys. Rev. Lett. 36, 956 (1976).
[Crossref]

Agrawal, G. P.

G. P. Agrawal, C. Cojan, and C. Flytzanis, Phys. Rev. B 17, 776 (1978).
[Crossref]

Alfano, R. R.

Baughman, R. H.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradere, J. Ducuing, R. H. Baughman, and R. R. Chance, Phys. Rev. Lett. 36, 956 (1976).
[Crossref]

Carter, G. M.

G. M. Carter, J. V. Hryniewicz, M. K. Thakur, Y. J. Chen, and S. E. Meyler, Appl. Phys. Lett. 49, 998 (1986).
[Crossref]

G. M. Carter, M. K. Thakur, Y. J. Chen, and J. V. Hryniewicz, Appl. Phys. Lett. 47, 457 (1985).
[Crossref]

J. V. Hryniewicz, G. M. Carter, and Y. J. Chen, Opt. Commun. 54, 230 (1985).
[Crossref]

G. M. Carter, Y. J. Chen, M. F. Rubner, D. J. Sandman, M. K. Thakur, and S. K. Tripathy, in Nonlinear Optical Properties of Organic Molecules and Crystals, D. S. Chemla and J. Zyss, eds. (Academic, New York, to be published), Vol. 2.

J. M. Huxley, J. G. Fujimoto, E. P. Ippen, G. M. Carter, and P. Mataloni, in Digest of the Conference on Lasers and Electro-Optics (Optical Society of America, Washington, D.C., 1987).

Chance, R. R.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradere, J. Ducuing, R. H. Baughman, and R. R. Chance, Phys. Rev. Lett. 36, 956 (1976).
[Crossref]

Chemla, D. S.

Chen, Y. J.

G. M. Carter, J. V. Hryniewicz, M. K. Thakur, Y. J. Chen, and S. E. Meyler, Appl. Phys. Lett. 49, 998 (1986).
[Crossref]

G. M. Carter, M. K. Thakur, Y. J. Chen, and J. V. Hryniewicz, Appl. Phys. Lett. 47, 457 (1985).
[Crossref]

J. V. Hryniewicz, G. M. Carter, and Y. J. Chen, Opt. Commun. 54, 230 (1985).
[Crossref]

G. M. Carter, Y. J. Chen, M. F. Rubner, D. J. Sandman, M. K. Thakur, and S. K. Tripathy, in Nonlinear Optical Properties of Organic Molecules and Crystals, D. S. Chemla and J. Zyss, eds. (Academic, New York, to be published), Vol. 2.

Chopra, P.

D. N. Rao, P. Chopra, S. K. Ghoshal, J. Swiatkiewicz, and P. N. Prasad, J. Chem. Phys. 84, 7049 (1986).
[Crossref]

Cojan, C.

G. P. Agrawal, C. Cojan, and C. Flytzanis, Phys. Rev. B 17, 776 (1978).
[Crossref]

Cotter, D.

D. Cotter, Electron. Lett. 22, 093 (1986).
[Crossref]

D. C. Hanna, M. A. Yuratich, and D. Cotter, Nonlinear Optics of Free Atoms and Molecules (Springer-Verlag, Berlin, 1979), Chap. 2.
[Crossref]

Ducuing, J.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradere, J. Ducuing, R. H. Baughman, and R. R. Chance, Phys. Rev. Lett. 36, 956 (1976).
[Crossref]

Eckbreth, A. C.

Flytzanis, C.

G. P. Agrawal, C. Cojan, and C. Flytzanis, Phys. Rev. B 17, 776 (1978).
[Crossref]

C. Flytzanis, in Nonlinear Optical Properties of Organic and Polymeric Materials, American Chemical Society Symposium Series 233, D. J. Williams, ed. (American Chemical Society, Washington, D.C., 1983), Chap. 8.

Fork, R. L.

R. L. Fork, C. V. Shank, R. Yen, and C. A. Hirlimann, IEEE J. Quantum Electron. QE-19, 500 (1983).
[Crossref]

C. V. Shank, E. P. Ippen, O. Teschke, and R. L. Fork, Chem. Phys. Lett. 57, 433 (1978).
[Crossref]

Frey, R.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradere, J. Ducuing, R. H. Baughman, and R. R. Chance, Phys. Rev. Lett. 36, 956 (1976).
[Crossref]

Fujimoto, J. G.

J. M. Huxley, J. G. Fujimoto, E. P. Ippen, G. M. Carter, and P. Mataloni, in Digest of the Conference on Lasers and Electro-Optics (Optical Society of America, Washington, D.C., 1987).

Gerritsen, H. J.

C. A. Hoffman, K. Jarasiunas, H. J. Gerritsen, and A. V. Nurmikko, Appl. Phys. Lett. 33, 536 (1978).
[Crossref]

Ghoshal, S. K.

D. N. Rao, P. Chopra, S. K. Ghoshal, J. Swiatkiewicz, and P. N. Prasad, J. Chem. Phys. 84, 7049 (1986).
[Crossref]

Grischkowsky, D.

B. Nikolaus and D. Grischkowsky, Appl. Phys. Lett. 43, 228 (1983).
[Crossref]

Hall, R. J.

Hanna, D. C.

D. C. Hanna, M. A. Yuratich, and D. Cotter, Nonlinear Optics of Free Atoms and Molecules (Springer-Verlag, Berlin, 1979), Chap. 2.
[Crossref]

Haus, H. A.

A. Lattes, H. A. Haus, F. J. Leonberger, and E. P. Ippen, IEEE J. Quantum Electron. QE-19, 1718 (1983).
[Crossref]

Hermann, J. P.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradere, J. Ducuing, R. H. Baughman, and R. R. Chance, Phys. Rev. Lett. 36, 956 (1976).
[Crossref]

Hirlimann, C. A.

R. L. Fork, C. V. Shank, R. Yen, and C. A. Hirlimann, IEEE J. Quantum Electron. QE-19, 500 (1983).
[Crossref]

Ho, P. P.

Hoffman, C. A.

C. A. Hoffman, K. Jarasiunas, H. J. Gerritsen, and A. V. Nurmikko, Appl. Phys. Lett. 33, 536 (1978).
[Crossref]

Hryniewicz, J. V.

G. M. Carter, J. V. Hryniewicz, M. K. Thakur, Y. J. Chen, and S. E. Meyler, Appl. Phys. Lett. 49, 998 (1986).
[Crossref]

G. M. Carter, M. K. Thakur, Y. J. Chen, and J. V. Hryniewicz, Appl. Phys. Lett. 47, 457 (1985).
[Crossref]

J. V. Hryniewicz, G. M. Carter, and Y. J. Chen, Opt. Commun. 54, 230 (1985).
[Crossref]

Huxley, J. M.

J. M. Huxley, J. G. Fujimoto, E. P. Ippen, G. M. Carter, and P. Mataloni, in Digest of the Conference on Lasers and Electro-Optics (Optical Society of America, Washington, D.C., 1987).

Ippen, E. P.

A. Lattes, H. A. Haus, F. J. Leonberger, and E. P. Ippen, IEEE J. Quantum Electron. QE-19, 1718 (1983).
[Crossref]

C. V. Shank, E. P. Ippen, O. Teschke, and R. L. Fork, Chem. Phys. Lett. 57, 433 (1978).
[Crossref]

J. M. Huxley, J. G. Fujimoto, E. P. Ippen, G. M. Carter, and P. Mataloni, in Digest of the Conference on Lasers and Electro-Optics (Optical Society of America, Washington, D.C., 1987).

Jarasiunas, K.

C. A. Hoffman, K. Jarasiunas, H. J. Gerritsen, and A. V. Nurmikko, Appl. Phys. Lett. 33, 536 (1978).
[Crossref]

Jimbo, T.

Johnson, A. M.

A. M. Johnson, R. H. Stolen, and W. M. Simpson, Appl. Phys. Lett. 44, 729 (1984).
[Crossref]

Kuwajima, S.

Z. G. Soos, S. Mazumdar, and S. Kuwajima, in Solid State Polymerization: The Structure and Properties of Polymers Produced by Lattice Controlled Processes, D. J. Sandman, ed. (American Chemical Society, Washington, D.C., to be published).

Lattes, A.

A. Lattes, H. A. Haus, F. J. Leonberger, and E. P. Ippen, IEEE J. Quantum Electron. QE-19, 1718 (1983).
[Crossref]

Laubereau, A.

P. Troeger, C. H. Liu, and A. Laubereau, in Time-Resolved Vibrational Spectroscopy, A. Laubereau and M. Stockburger, eds. (Springer-Verlag, Berlin, 1985), pp. 62–66.
[Crossref]

Leonberger, F. J.

A. Lattes, H. A. Haus, F. J. Leonberger, and E. P. Ippen, IEEE J. Quantum Electron. QE-19, 1718 (1983).
[Crossref]

Liu, C. H.

P. Troeger, C. H. Liu, and A. Laubereau, in Time-Resolved Vibrational Spectroscopy, A. Laubereau and M. Stockburger, eds. (Springer-Verlag, Berlin, 1985), pp. 62–66.
[Crossref]

Mataloni, P.

J. M. Huxley, J. G. Fujimoto, E. P. Ippen, G. M. Carter, and P. Mataloni, in Digest of the Conference on Lasers and Electro-Optics (Optical Society of America, Washington, D.C., 1987).

Mazumdar, S.

S. Mazumdar, National Chemical Laboratories, Pune, India (personal communication).

Z. G. Soos, S. Mazumdar, and S. Kuwajima, in Solid State Polymerization: The Structure and Properties of Polymers Produced by Lattice Controlled Processes, D. J. Sandman, ed. (American Chemical Society, Washington, D.C., to be published).

Meyler, S. E.

G. M. Carter, J. V. Hryniewicz, M. K. Thakur, Y. J. Chen, and S. E. Meyler, Appl. Phys. Lett. 49, 998 (1986).
[Crossref]

Miller, D. A. B.

Nikolaus, B.

B. Nikolaus and D. Grischkowsky, Appl. Phys. Lett. 43, 228 (1983).
[Crossref]

Nurmikko, A. V.

C. A. Hoffman, K. Jarasiunas, H. J. Gerritsen, and A. V. Nurmikko, Appl. Phys. Lett. 33, 536 (1978).
[Crossref]

Philpott, M. R.

M. R. Philpott, Chem. Phys. Lett. 50, 18 (1977).
[Crossref]

Pope, M.

M. Pope and C. E. Swenberg, Electronic Processes in Organic Crystals (Oxford U. Press, New York, 1982), pp. 677–696.

Pradere, F.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradere, J. Ducuing, R. H. Baughman, and R. R. Chance, Phys. Rev. Lett. 36, 956 (1976).
[Crossref]

Prasad, P. N.

D. N. Rao, P. Chopra, S. K. Ghoshal, J. Swiatkiewicz, and P. N. Prasad, J. Chem. Phys. 84, 7049 (1986).
[Crossref]

Rao, D. N.

D. N. Rao, P. Chopra, S. K. Ghoshal, J. Swiatkiewicz, and P. N. Prasad, J. Chem. Phys. 84, 7049 (1986).
[Crossref]

Rubner, M. F.

G. M. Carter, Y. J. Chen, M. F. Rubner, D. J. Sandman, M. K. Thakur, and S. K. Tripathy, in Nonlinear Optical Properties of Organic Molecules and Crystals, D. S. Chemla and J. Zyss, eds. (Academic, New York, to be published), Vol. 2.

Sandman, D. J.

G. M. Carter, Y. J. Chen, M. F. Rubner, D. J. Sandman, M. K. Thakur, and S. K. Tripathy, in Nonlinear Optical Properties of Organic Molecules and Crystals, D. S. Chemla and J. Zyss, eds. (Academic, New York, to be published), Vol. 2.

Sauteret, C.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradere, J. Ducuing, R. H. Baughman, and R. R. Chance, Phys. Rev. Lett. 36, 956 (1976).
[Crossref]

Sebastian, L.

L. Sebastian and G. Weiser, Chem. Phys. 62, 447 (1981).
[Crossref]

Shank, C. V.

R. L. Fork, C. V. Shank, R. Yen, and C. A. Hirlimann, IEEE J. Quantum Electron. QE-19, 500 (1983).
[Crossref]

C. V. Shank, E. P. Ippen, O. Teschke, and R. L. Fork, Chem. Phys. Lett. 57, 433 (1978).
[Crossref]

Shen, Y. R.

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), pp. 249–251.

Shirley, J. A.

Simpson, W. M.

A. M. Johnson, R. H. Stolen, and W. M. Simpson, Appl. Phys. Lett. 44, 729 (1984).
[Crossref]

Soos, Z. G.

Z. G. Soos, S. Mazumdar, and S. Kuwajima, in Solid State Polymerization: The Structure and Properties of Polymers Produced by Lattice Controlled Processes, D. J. Sandman, ed. (American Chemical Society, Washington, D.C., to be published).

Stolen, R. H.

A. M. Johnson, R. H. Stolen, and W. M. Simpson, Appl. Phys. Lett. 44, 729 (1984).
[Crossref]

Swenberg, C. E.

M. Pope and C. E. Swenberg, Electronic Processes in Organic Crystals (Oxford U. Press, New York, 1982), pp. 677–696.

Swiatkiewicz, J.

D. N. Rao, P. Chopra, S. K. Ghoshal, J. Swiatkiewicz, and P. N. Prasad, J. Chem. Phys. 84, 7049 (1986).
[Crossref]

Teschke, O.

C. V. Shank, E. P. Ippen, O. Teschke, and R. L. Fork, Chem. Phys. Lett. 57, 433 (1978).
[Crossref]

Thakur, M. K.

G. M. Carter, J. V. Hryniewicz, M. K. Thakur, Y. J. Chen, and S. E. Meyler, Appl. Phys. Lett. 49, 998 (1986).
[Crossref]

G. M. Carter, M. K. Thakur, Y. J. Chen, and J. V. Hryniewicz, Appl. Phys. Lett. 47, 457 (1985).
[Crossref]

G. M. Carter, Y. J. Chen, M. F. Rubner, D. J. Sandman, M. K. Thakur, and S. K. Tripathy, in Nonlinear Optical Properties of Organic Molecules and Crystals, D. S. Chemla and J. Zyss, eds. (Academic, New York, to be published), Vol. 2.

Tripathy, S. K.

G. M. Carter, Y. J. Chen, M. F. Rubner, D. J. Sandman, M. K. Thakur, and S. K. Tripathy, in Nonlinear Optical Properties of Organic Molecules and Crystals, D. S. Chemla and J. Zyss, eds. (Academic, New York, to be published), Vol. 2.

Troeger, P.

P. Troeger, C. H. Liu, and A. Laubereau, in Time-Resolved Vibrational Spectroscopy, A. Laubereau and M. Stockburger, eds. (Springer-Verlag, Berlin, 1985), pp. 62–66.
[Crossref]

Wang, Q. Z.

Weiser, G.

L. Sebastian and G. Weiser, Chem. Phys. 62, 447 (1981).
[Crossref]

Yang, N. L.

Yariv, A.

A. Yariv, Quantum Electronics, 2nd ed. (Wiley, New York, 1975), Chap. 8.

Yen, R.

R. L. Fork, C. V. Shank, R. Yen, and C. A. Hirlimann, IEEE J. Quantum Electron. QE-19, 500 (1983).
[Crossref]

Yuratich, M. A.

D. C. Hanna, M. A. Yuratich, and D. Cotter, Nonlinear Optics of Free Atoms and Molecules (Springer-Verlag, Berlin, 1979), Chap. 2.
[Crossref]

Appl. Phys. Lett. (5)

B. Nikolaus and D. Grischkowsky, Appl. Phys. Lett. 43, 228 (1983).
[Crossref]

A. M. Johnson, R. H. Stolen, and W. M. Simpson, Appl. Phys. Lett. 44, 729 (1984).
[Crossref]

G. M. Carter, M. K. Thakur, Y. J. Chen, and J. V. Hryniewicz, Appl. Phys. Lett. 47, 457 (1985).
[Crossref]

G. M. Carter, J. V. Hryniewicz, M. K. Thakur, Y. J. Chen, and S. E. Meyler, Appl. Phys. Lett. 49, 998 (1986).
[Crossref]

C. A. Hoffman, K. Jarasiunas, H. J. Gerritsen, and A. V. Nurmikko, Appl. Phys. Lett. 33, 536 (1978).
[Crossref]

Chem. Phys. (1)

L. Sebastian and G. Weiser, Chem. Phys. 62, 447 (1981).
[Crossref]

Chem. Phys. Lett. (2)

M. R. Philpott, Chem. Phys. Lett. 50, 18 (1977).
[Crossref]

C. V. Shank, E. P. Ippen, O. Teschke, and R. L. Fork, Chem. Phys. Lett. 57, 433 (1978).
[Crossref]

Electron. Lett. (1)

D. Cotter, Electron. Lett. 22, 093 (1986).
[Crossref]

IEEE J. Quantum Electron. (2)

R. L. Fork, C. V. Shank, R. Yen, and C. A. Hirlimann, IEEE J. Quantum Electron. QE-19, 500 (1983).
[Crossref]

A. Lattes, H. A. Haus, F. J. Leonberger, and E. P. Ippen, IEEE J. Quantum Electron. QE-19, 1718 (1983).
[Crossref]

J. Chem. Phys. (1)

D. N. Rao, P. Chopra, S. K. Ghoshal, J. Swiatkiewicz, and P. N. Prasad, J. Chem. Phys. 84, 7049 (1986).
[Crossref]

J. Opt. Soc. Am. B (2)

Opt. Commun. (1)

J. V. Hryniewicz, G. M. Carter, and Y. J. Chen, Opt. Commun. 54, 230 (1985).
[Crossref]

Opt. Lett. (1)

Phys. Rev. B (1)

G. P. Agrawal, C. Cojan, and C. Flytzanis, Phys. Rev. B 17, 776 (1978).
[Crossref]

Phys. Rev. Lett. (1)

C. Sauteret, J. P. Hermann, R. Frey, F. Pradere, J. Ducuing, R. H. Baughman, and R. R. Chance, Phys. Rev. Lett. 36, 956 (1976).
[Crossref]

Other (10)

G. M. Carter, Y. J. Chen, M. F. Rubner, D. J. Sandman, M. K. Thakur, and S. K. Tripathy, in Nonlinear Optical Properties of Organic Molecules and Crystals, D. S. Chemla and J. Zyss, eds. (Academic, New York, to be published), Vol. 2.

A. Yariv, Quantum Electronics, 2nd ed. (Wiley, New York, 1975), Chap. 8.

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), pp. 249–251.

M. Pope and C. E. Swenberg, Electronic Processes in Organic Crystals (Oxford U. Press, New York, 1982), pp. 677–696.

Z. G. Soos, S. Mazumdar, and S. Kuwajima, in Solid State Polymerization: The Structure and Properties of Polymers Produced by Lattice Controlled Processes, D. J. Sandman, ed. (American Chemical Society, Washington, D.C., to be published).

S. Mazumdar, National Chemical Laboratories, Pune, India (personal communication).

C. Flytzanis, in Nonlinear Optical Properties of Organic and Polymeric Materials, American Chemical Society Symposium Series 233, D. J. Williams, ed. (American Chemical Society, Washington, D.C., 1983), Chap. 8.

D. C. Hanna, M. A. Yuratich, and D. Cotter, Nonlinear Optics of Free Atoms and Molecules (Springer-Verlag, Berlin, 1979), Chap. 2.
[Crossref]

P. Troeger, C. H. Liu, and A. Laubereau, in Time-Resolved Vibrational Spectroscopy, A. Laubereau and M. Stockburger, eds. (Springer-Verlag, Berlin, 1985), pp. 62–66.
[Crossref]

J. M. Huxley, J. G. Fujimoto, E. P. Ippen, G. M. Carter, and P. Mataloni, in Digest of the Conference on Lasers and Electro-Optics (Optical Society of America, Washington, D.C., 1987).

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Figures (4)

Fig. 1
Fig. 1

Schematic of the optical beam geometry in the plane of the material for the degenerate four-wave mixing process. The arrival time of the incident beam 2 is offset from incident beams 1 and 3 by Td. The polymer chain axis is shown by the arrow. The dashed and solid lines represent the two population gratings produced in the resonant four-wave mixing experiments. The direction a is the direction of the polymer chain axis. Note that, even though the four beams are actually spatially overlapping in the sample, for clarity the four beams are shown spatially separated as they would be after leaving the sample.

Fig. 2
Fig. 2

The four-wave mixing signal S4 as a function of time delay of one of the incident laser beams. The open circles represent results for incident laser pulses 6 psec in duration, and the filled circles represent results for 300-fsec pulses. For both sets of data the laser wavelength was 6500 Å in resonance with the excitonic state in PDA.

Fig. 3
Fig. 3

The filled circles represent the measured nonresonant four-wave mixing signal S4 as a function of time delay of one of the incident pulses. The other curves are theoretical simulations of a four-wave mixing process with various response times, using the optical pulse parameters from the experiment. The incident laser wavelength was 7200 Å.

Fig. 4
Fig. 4

Theoretical simulation of a four-wave mixing signal S12 as a function of time delay of one the incident beams. A beam geometry in which two of the incident beams were counterpropagating in the nonlinear material and in which the third beam was time delayed was assumed. The three curves shown are for three assumed relaxation times of the nonlinear process and an optical pulse duration of 300 fsec.

Equations (5)

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ξ j = E j ( ρ , t ) exp ( i k j · r - ω t ) ,
E j ( ρ , t ) = A j exp ( - ρ 2 / ρ 0 2 ) sech ( a t ) .
exp ( i k 4 · r ) d E 4 d z = C { χ i 123 ( 3 ) E 1 E 2 E 3 * exp [ i ( k 1 + k 2 - k 3 ) · r ] + χ j 123 ( 3 ) E 1 E 2 * E 3 exp [ i ( k 1 - k 2 + k 3 ) · r ] + } ,
d p d t = - p T 1 + R ( ω ) [ E 2 ( t + T d ) E 1 ( t ) + E 3 ( t ) E 1 ( t ) ] ,
E 4 ( t ) = K [ E 3 ( t ) - t d t E 2 ( t + T d ) E 1 ( t ) f ( t , t ) + E 2 ( t + T d ) - t d t E 3 ( t ) E 1 ( t ) f ( t , t ) ] ,

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