Abstract

Accurate second-harmonic generation (SHG) measurements in birefringent single crystals of the asymmetrically substituted diacetylene NP/4-MPU were performed with a 10-ns pulsed laser system with small bandwidth. The measurements show typical oscillations, which overlie the well-known Maker fringe pattern. These oscillations can be explained by interference between the incident fundamental wave and its reflections at the front and back sides of the crystal. The interference is described by a ray-tracer algorithm, which takes into account the beam profile. Furthermore, because the investigated material is biaxially birefringent at its principal axes, the theory for SHG proposed by Okamoto et al. [J. Opt. Soc. Am. B 9, 2083 (1992)] was extended for this case and is written in a compact 4×4 matrix formulation. By using the additional information of the interference of the fundamental wave, we evaluated and fitted the measurements with greater accuracy.

© 1997 Optical Society of America

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  1. C. Sauteret, J. P. Hermann, R. Frey, F. Pradère, J. Ducuing, R. H. Baughman, and R. R. Chance, “Optical nonlinearities in one-dimensional-conjugated polymer crystals,” Phys. Rev. Lett. 36, 956 (1976).
    [CrossRef]
  2. Th. Fehn, Th. Vogtmann, J. Hübner, and M. Schwoerer, “Anisotropy of the nonlinear optical susceptibility χ(3) in polydiacetylene single crystals,” Appl. Phys. B 59, 203 (1994).
    [CrossRef]
  3. P. A. Gass, I. Abram, R. Raj, and M. Schott, “The nonlinear optical spectrum of polydiacetylene in the near infrared,” J. Chem. Phys. 100, 88 (1994).
    [CrossRef]
  4. J. M. Huxley, P. Mataloni, R. W. Schoenlein, J. G. Fujimoto, E. P. Ippen, and G. M. Carter, “Femtosecond excited-state dynamics of polydiacetylene,” Appl. Phys. Lett. 56, 1600 (1990).
    [CrossRef]
  5. T. Kobayashi, “Ultrafast nonlinear optical processes in conjugated polymers,” Optoelectron. Dev. Technol. 8, 309 (1993).
  6. B. L. Lawrence, M. Cha, W. E. Torruellas, G. I. Stegeman, S. Etemad, and G. Baker, “Z-scan measurement of third and fifth order nonlinearities in single crystal PTS at 1064 nm,” Nonlin. Opt. 10, 193 (1995).
  7. G. Wegner, “Topochemical reactions of monomers with conjugated triple bonds. I. Polymerization of derivatives of 2,4-hexadiyn-1,6-diols in the crystalline state,” Z. Naturforsch. B 24, 824 (1969).
  8. P. S. Kalyanaraman, A. F. Garito, A. R. McGhie, and K. N. Desai, “Synthesis of nitrophenoxymethyl substituted diacetylene monomers,” Makromol. Chem. 180, 1393 (1979).
    [CrossRef]
  9. P. Strohriegl, H. Schultes, D. Heindl, P. Gruner-Bauer, V. Enkelmann, and E. Dormann, “Preparation, crystal structure and dielectric properties of the new unsymmetrically substituted diacetylenes NP/R2,” Ber. Bunsenges. Phys. Chem. 91, 918 (1987).
    [CrossRef]
  10. P. Strohriegl, J. Gmeiner, I. Müller, P. Gruner-Bauer, E. Dormann, and V. Enkelmann, “The asymmetrical diacetylene derivatives FBS/TFMBS and DNP/MNP: synthesis and solid state properties,” Ber. Bunsenges. Phys. Chem. 95, 491 (1991).
    [CrossRef]
  11. A. F. Garito, C. C. Teng, K. Y. Wong, and O. Zammani-Khamiri, “Molecular optics: nonlinear optical processes in organic and polymer crystals,” Mol. Cryst. Liq. Cryst. 106, 219 (1984).
    [CrossRef]
  12. T. Yoshimura, “Enhancing second-order nonlinear optical properties by controlling the wave function in one-dimensional conjugated molecules,” Phys. Rev. B 40, 6292 (1989).
    [CrossRef]
  13. Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984).
  14. N. Okamoto, Y. Hirano, and O. Sugihara, “Precise estimation of nonlinear-optical coefficients for anisotropic nonlinear films with C∞V symmetry,” J. Opt. Soc. Am. B 9, 2083 (1992).
    [CrossRef]
  15. R. Morita, T. Kondo, Y. Kaneda, A. Sugihashi, N. Ogasawara, S. Umegaki, and R. Ito, “Multiple-reflection effects in optical second-harmonic generation,” Jpn. J. Appl. Phys. 27, 1134 (1988).
    [CrossRef]
  16. L. Kador, R. Fischer, R. Kasemann, S. Brück, and H. Dürr, “Fine structure in the χ(2) signals of inorganic-organic nanocomposites,” J. Appl. Phys. 75, 2709 (1994).
    [CrossRef]
  17. W. N. Herman and L. M. Hayden, “Maker fringes revisited: second-harmonic generation from birefringent or absorbing materials,” J. Opt. Soc. Am. B 12, 416 (1995).
    [CrossRef]
  18. Th. Fehn and F. Bauer, Physikalisches Institut, Universität Bayreuth, D-95440 Bayreuth, Germany (personal communication, 1996).
  19. W. Milius, Chemisches Institut, Universität Bayreuth, D-95440 Bayreuth, Germany (personal communication, 1995).
  20. P. N. Butcher and D. Cotter, The Elements of Nonlinear Optics, Vol. 9 of Cambridge Studies in Modern Optics (Cambridge U. Press, Cambridge, 1990).
  21. P. Yeh, Optical Waves in Layered Media (Wiley, New York, 1988).
  22. V. G. Dimitriev, G. G. Gurzadyan, and D. N. Nikogosyan, Handbook of Nonlinear Optical Crystals, Vol. 64 of Springer Series in Optical Science (Springer-Verlag, Heidelberg, 1991).

1995 (2)

B. L. Lawrence, M. Cha, W. E. Torruellas, G. I. Stegeman, S. Etemad, and G. Baker, “Z-scan measurement of third and fifth order nonlinearities in single crystal PTS at 1064 nm,” Nonlin. Opt. 10, 193 (1995).

W. N. Herman and L. M. Hayden, “Maker fringes revisited: second-harmonic generation from birefringent or absorbing materials,” J. Opt. Soc. Am. B 12, 416 (1995).
[CrossRef]

1994 (3)

L. Kador, R. Fischer, R. Kasemann, S. Brück, and H. Dürr, “Fine structure in the χ(2) signals of inorganic-organic nanocomposites,” J. Appl. Phys. 75, 2709 (1994).
[CrossRef]

Th. Fehn, Th. Vogtmann, J. Hübner, and M. Schwoerer, “Anisotropy of the nonlinear optical susceptibility χ(3) in polydiacetylene single crystals,” Appl. Phys. B 59, 203 (1994).
[CrossRef]

P. A. Gass, I. Abram, R. Raj, and M. Schott, “The nonlinear optical spectrum of polydiacetylene in the near infrared,” J. Chem. Phys. 100, 88 (1994).
[CrossRef]

1993 (1)

T. Kobayashi, “Ultrafast nonlinear optical processes in conjugated polymers,” Optoelectron. Dev. Technol. 8, 309 (1993).

1992 (1)

1991 (1)

P. Strohriegl, J. Gmeiner, I. Müller, P. Gruner-Bauer, E. Dormann, and V. Enkelmann, “The asymmetrical diacetylene derivatives FBS/TFMBS and DNP/MNP: synthesis and solid state properties,” Ber. Bunsenges. Phys. Chem. 95, 491 (1991).
[CrossRef]

1990 (1)

J. M. Huxley, P. Mataloni, R. W. Schoenlein, J. G. Fujimoto, E. P. Ippen, and G. M. Carter, “Femtosecond excited-state dynamics of polydiacetylene,” Appl. Phys. Lett. 56, 1600 (1990).
[CrossRef]

1989 (1)

T. Yoshimura, “Enhancing second-order nonlinear optical properties by controlling the wave function in one-dimensional conjugated molecules,” Phys. Rev. B 40, 6292 (1989).
[CrossRef]

1988 (1)

R. Morita, T. Kondo, Y. Kaneda, A. Sugihashi, N. Ogasawara, S. Umegaki, and R. Ito, “Multiple-reflection effects in optical second-harmonic generation,” Jpn. J. Appl. Phys. 27, 1134 (1988).
[CrossRef]

1987 (1)

P. Strohriegl, H. Schultes, D. Heindl, P. Gruner-Bauer, V. Enkelmann, and E. Dormann, “Preparation, crystal structure and dielectric properties of the new unsymmetrically substituted diacetylenes NP/R2,” Ber. Bunsenges. Phys. Chem. 91, 918 (1987).
[CrossRef]

1984 (1)

A. F. Garito, C. C. Teng, K. Y. Wong, and O. Zammani-Khamiri, “Molecular optics: nonlinear optical processes in organic and polymer crystals,” Mol. Cryst. Liq. Cryst. 106, 219 (1984).
[CrossRef]

1979 (1)

P. S. Kalyanaraman, A. F. Garito, A. R. McGhie, and K. N. Desai, “Synthesis of nitrophenoxymethyl substituted diacetylene monomers,” Makromol. Chem. 180, 1393 (1979).
[CrossRef]

1976 (1)

C. Sauteret, J. P. Hermann, R. Frey, F. Pradère, J. Ducuing, R. H. Baughman, and R. R. Chance, “Optical nonlinearities in one-dimensional-conjugated polymer crystals,” Phys. Rev. Lett. 36, 956 (1976).
[CrossRef]

1969 (1)

G. Wegner, “Topochemical reactions of monomers with conjugated triple bonds. I. Polymerization of derivatives of 2,4-hexadiyn-1,6-diols in the crystalline state,” Z. Naturforsch. B 24, 824 (1969).

Abram, I.

P. A. Gass, I. Abram, R. Raj, and M. Schott, “The nonlinear optical spectrum of polydiacetylene in the near infrared,” J. Chem. Phys. 100, 88 (1994).
[CrossRef]

Baker, G.

B. L. Lawrence, M. Cha, W. E. Torruellas, G. I. Stegeman, S. Etemad, and G. Baker, “Z-scan measurement of third and fifth order nonlinearities in single crystal PTS at 1064 nm,” Nonlin. Opt. 10, 193 (1995).

Bauer, F.

Th. Fehn and F. Bauer, Physikalisches Institut, Universität Bayreuth, D-95440 Bayreuth, Germany (personal communication, 1996).

Baughman, R. H.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradère, J. Ducuing, R. H. Baughman, and R. R. Chance, “Optical nonlinearities in one-dimensional-conjugated polymer crystals,” Phys. Rev. Lett. 36, 956 (1976).
[CrossRef]

Brück, S.

L. Kador, R. Fischer, R. Kasemann, S. Brück, and H. Dürr, “Fine structure in the χ(2) signals of inorganic-organic nanocomposites,” J. Appl. Phys. 75, 2709 (1994).
[CrossRef]

Butcher, P. N.

P. N. Butcher and D. Cotter, The Elements of Nonlinear Optics, Vol. 9 of Cambridge Studies in Modern Optics (Cambridge U. Press, Cambridge, 1990).

Carter, G. M.

J. M. Huxley, P. Mataloni, R. W. Schoenlein, J. G. Fujimoto, E. P. Ippen, and G. M. Carter, “Femtosecond excited-state dynamics of polydiacetylene,” Appl. Phys. Lett. 56, 1600 (1990).
[CrossRef]

Cha, M.

B. L. Lawrence, M. Cha, W. E. Torruellas, G. I. Stegeman, S. Etemad, and G. Baker, “Z-scan measurement of third and fifth order nonlinearities in single crystal PTS at 1064 nm,” Nonlin. Opt. 10, 193 (1995).

Chance, R. R.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradère, J. Ducuing, R. H. Baughman, and R. R. Chance, “Optical nonlinearities in one-dimensional-conjugated polymer crystals,” Phys. Rev. Lett. 36, 956 (1976).
[CrossRef]

Cotter, D.

P. N. Butcher and D. Cotter, The Elements of Nonlinear Optics, Vol. 9 of Cambridge Studies in Modern Optics (Cambridge U. Press, Cambridge, 1990).

Desai, K. N.

P. S. Kalyanaraman, A. F. Garito, A. R. McGhie, and K. N. Desai, “Synthesis of nitrophenoxymethyl substituted diacetylene monomers,” Makromol. Chem. 180, 1393 (1979).
[CrossRef]

Dimitriev, V. G.

V. G. Dimitriev, G. G. Gurzadyan, and D. N. Nikogosyan, Handbook of Nonlinear Optical Crystals, Vol. 64 of Springer Series in Optical Science (Springer-Verlag, Heidelberg, 1991).

Dormann, E.

P. Strohriegl, J. Gmeiner, I. Müller, P. Gruner-Bauer, E. Dormann, and V. Enkelmann, “The asymmetrical diacetylene derivatives FBS/TFMBS and DNP/MNP: synthesis and solid state properties,” Ber. Bunsenges. Phys. Chem. 95, 491 (1991).
[CrossRef]

P. Strohriegl, H. Schultes, D. Heindl, P. Gruner-Bauer, V. Enkelmann, and E. Dormann, “Preparation, crystal structure and dielectric properties of the new unsymmetrically substituted diacetylenes NP/R2,” Ber. Bunsenges. Phys. Chem. 91, 918 (1987).
[CrossRef]

Ducuing, J.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradère, J. Ducuing, R. H. Baughman, and R. R. Chance, “Optical nonlinearities in one-dimensional-conjugated polymer crystals,” Phys. Rev. Lett. 36, 956 (1976).
[CrossRef]

Dürr, H.

L. Kador, R. Fischer, R. Kasemann, S. Brück, and H. Dürr, “Fine structure in the χ(2) signals of inorganic-organic nanocomposites,” J. Appl. Phys. 75, 2709 (1994).
[CrossRef]

Enkelmann, V.

P. Strohriegl, J. Gmeiner, I. Müller, P. Gruner-Bauer, E. Dormann, and V. Enkelmann, “The asymmetrical diacetylene derivatives FBS/TFMBS and DNP/MNP: synthesis and solid state properties,” Ber. Bunsenges. Phys. Chem. 95, 491 (1991).
[CrossRef]

P. Strohriegl, H. Schultes, D. Heindl, P. Gruner-Bauer, V. Enkelmann, and E. Dormann, “Preparation, crystal structure and dielectric properties of the new unsymmetrically substituted diacetylenes NP/R2,” Ber. Bunsenges. Phys. Chem. 91, 918 (1987).
[CrossRef]

Etemad, S.

B. L. Lawrence, M. Cha, W. E. Torruellas, G. I. Stegeman, S. Etemad, and G. Baker, “Z-scan measurement of third and fifth order nonlinearities in single crystal PTS at 1064 nm,” Nonlin. Opt. 10, 193 (1995).

Fehn, Th.

Th. Fehn, Th. Vogtmann, J. Hübner, and M. Schwoerer, “Anisotropy of the nonlinear optical susceptibility χ(3) in polydiacetylene single crystals,” Appl. Phys. B 59, 203 (1994).
[CrossRef]

Th. Fehn and F. Bauer, Physikalisches Institut, Universität Bayreuth, D-95440 Bayreuth, Germany (personal communication, 1996).

Fischer, R.

L. Kador, R. Fischer, R. Kasemann, S. Brück, and H. Dürr, “Fine structure in the χ(2) signals of inorganic-organic nanocomposites,” J. Appl. Phys. 75, 2709 (1994).
[CrossRef]

Frey, R.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradère, J. Ducuing, R. H. Baughman, and R. R. Chance, “Optical nonlinearities in one-dimensional-conjugated polymer crystals,” Phys. Rev. Lett. 36, 956 (1976).
[CrossRef]

Fujimoto, J. G.

J. M. Huxley, P. Mataloni, R. W. Schoenlein, J. G. Fujimoto, E. P. Ippen, and G. M. Carter, “Femtosecond excited-state dynamics of polydiacetylene,” Appl. Phys. Lett. 56, 1600 (1990).
[CrossRef]

Garito, A. F.

A. F. Garito, C. C. Teng, K. Y. Wong, and O. Zammani-Khamiri, “Molecular optics: nonlinear optical processes in organic and polymer crystals,” Mol. Cryst. Liq. Cryst. 106, 219 (1984).
[CrossRef]

P. S. Kalyanaraman, A. F. Garito, A. R. McGhie, and K. N. Desai, “Synthesis of nitrophenoxymethyl substituted diacetylene monomers,” Makromol. Chem. 180, 1393 (1979).
[CrossRef]

Gass, P. A.

P. A. Gass, I. Abram, R. Raj, and M. Schott, “The nonlinear optical spectrum of polydiacetylene in the near infrared,” J. Chem. Phys. 100, 88 (1994).
[CrossRef]

Gmeiner, J.

P. Strohriegl, J. Gmeiner, I. Müller, P. Gruner-Bauer, E. Dormann, and V. Enkelmann, “The asymmetrical diacetylene derivatives FBS/TFMBS and DNP/MNP: synthesis and solid state properties,” Ber. Bunsenges. Phys. Chem. 95, 491 (1991).
[CrossRef]

Gruner-Bauer, P.

P. Strohriegl, J. Gmeiner, I. Müller, P. Gruner-Bauer, E. Dormann, and V. Enkelmann, “The asymmetrical diacetylene derivatives FBS/TFMBS and DNP/MNP: synthesis and solid state properties,” Ber. Bunsenges. Phys. Chem. 95, 491 (1991).
[CrossRef]

P. Strohriegl, H. Schultes, D. Heindl, P. Gruner-Bauer, V. Enkelmann, and E. Dormann, “Preparation, crystal structure and dielectric properties of the new unsymmetrically substituted diacetylenes NP/R2,” Ber. Bunsenges. Phys. Chem. 91, 918 (1987).
[CrossRef]

Gurzadyan, G. G.

V. G. Dimitriev, G. G. Gurzadyan, and D. N. Nikogosyan, Handbook of Nonlinear Optical Crystals, Vol. 64 of Springer Series in Optical Science (Springer-Verlag, Heidelberg, 1991).

Hayden, L. M.

Heindl, D.

P. Strohriegl, H. Schultes, D. Heindl, P. Gruner-Bauer, V. Enkelmann, and E. Dormann, “Preparation, crystal structure and dielectric properties of the new unsymmetrically substituted diacetylenes NP/R2,” Ber. Bunsenges. Phys. Chem. 91, 918 (1987).
[CrossRef]

Herman, W. N.

Hermann, J. P.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradère, J. Ducuing, R. H. Baughman, and R. R. Chance, “Optical nonlinearities in one-dimensional-conjugated polymer crystals,” Phys. Rev. Lett. 36, 956 (1976).
[CrossRef]

Hirano, Y.

Hübner, J.

Th. Fehn, Th. Vogtmann, J. Hübner, and M. Schwoerer, “Anisotropy of the nonlinear optical susceptibility χ(3) in polydiacetylene single crystals,” Appl. Phys. B 59, 203 (1994).
[CrossRef]

Huxley, J. M.

J. M. Huxley, P. Mataloni, R. W. Schoenlein, J. G. Fujimoto, E. P. Ippen, and G. M. Carter, “Femtosecond excited-state dynamics of polydiacetylene,” Appl. Phys. Lett. 56, 1600 (1990).
[CrossRef]

Ippen, E. P.

J. M. Huxley, P. Mataloni, R. W. Schoenlein, J. G. Fujimoto, E. P. Ippen, and G. M. Carter, “Femtosecond excited-state dynamics of polydiacetylene,” Appl. Phys. Lett. 56, 1600 (1990).
[CrossRef]

Ito, R.

R. Morita, T. Kondo, Y. Kaneda, A. Sugihashi, N. Ogasawara, S. Umegaki, and R. Ito, “Multiple-reflection effects in optical second-harmonic generation,” Jpn. J. Appl. Phys. 27, 1134 (1988).
[CrossRef]

Kador, L.

L. Kador, R. Fischer, R. Kasemann, S. Brück, and H. Dürr, “Fine structure in the χ(2) signals of inorganic-organic nanocomposites,” J. Appl. Phys. 75, 2709 (1994).
[CrossRef]

Kalyanaraman, P. S.

P. S. Kalyanaraman, A. F. Garito, A. R. McGhie, and K. N. Desai, “Synthesis of nitrophenoxymethyl substituted diacetylene monomers,” Makromol. Chem. 180, 1393 (1979).
[CrossRef]

Kaneda, Y.

R. Morita, T. Kondo, Y. Kaneda, A. Sugihashi, N. Ogasawara, S. Umegaki, and R. Ito, “Multiple-reflection effects in optical second-harmonic generation,” Jpn. J. Appl. Phys. 27, 1134 (1988).
[CrossRef]

Kasemann, R.

L. Kador, R. Fischer, R. Kasemann, S. Brück, and H. Dürr, “Fine structure in the χ(2) signals of inorganic-organic nanocomposites,” J. Appl. Phys. 75, 2709 (1994).
[CrossRef]

Kobayashi, T.

T. Kobayashi, “Ultrafast nonlinear optical processes in conjugated polymers,” Optoelectron. Dev. Technol. 8, 309 (1993).

Kondo, T.

R. Morita, T. Kondo, Y. Kaneda, A. Sugihashi, N. Ogasawara, S. Umegaki, and R. Ito, “Multiple-reflection effects in optical second-harmonic generation,” Jpn. J. Appl. Phys. 27, 1134 (1988).
[CrossRef]

Lawrence, B. L.

B. L. Lawrence, M. Cha, W. E. Torruellas, G. I. Stegeman, S. Etemad, and G. Baker, “Z-scan measurement of third and fifth order nonlinearities in single crystal PTS at 1064 nm,” Nonlin. Opt. 10, 193 (1995).

Mataloni, P.

J. M. Huxley, P. Mataloni, R. W. Schoenlein, J. G. Fujimoto, E. P. Ippen, and G. M. Carter, “Femtosecond excited-state dynamics of polydiacetylene,” Appl. Phys. Lett. 56, 1600 (1990).
[CrossRef]

McGhie, A. R.

P. S. Kalyanaraman, A. F. Garito, A. R. McGhie, and K. N. Desai, “Synthesis of nitrophenoxymethyl substituted diacetylene monomers,” Makromol. Chem. 180, 1393 (1979).
[CrossRef]

Milius, W.

W. Milius, Chemisches Institut, Universität Bayreuth, D-95440 Bayreuth, Germany (personal communication, 1995).

Morita, R.

R. Morita, T. Kondo, Y. Kaneda, A. Sugihashi, N. Ogasawara, S. Umegaki, and R. Ito, “Multiple-reflection effects in optical second-harmonic generation,” Jpn. J. Appl. Phys. 27, 1134 (1988).
[CrossRef]

Müller, I.

P. Strohriegl, J. Gmeiner, I. Müller, P. Gruner-Bauer, E. Dormann, and V. Enkelmann, “The asymmetrical diacetylene derivatives FBS/TFMBS and DNP/MNP: synthesis and solid state properties,” Ber. Bunsenges. Phys. Chem. 95, 491 (1991).
[CrossRef]

Nikogosyan, D. N.

V. G. Dimitriev, G. G. Gurzadyan, and D. N. Nikogosyan, Handbook of Nonlinear Optical Crystals, Vol. 64 of Springer Series in Optical Science (Springer-Verlag, Heidelberg, 1991).

Ogasawara, N.

R. Morita, T. Kondo, Y. Kaneda, A. Sugihashi, N. Ogasawara, S. Umegaki, and R. Ito, “Multiple-reflection effects in optical second-harmonic generation,” Jpn. J. Appl. Phys. 27, 1134 (1988).
[CrossRef]

Okamoto, N.

Pradère, F.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradère, J. Ducuing, R. H. Baughman, and R. R. Chance, “Optical nonlinearities in one-dimensional-conjugated polymer crystals,” Phys. Rev. Lett. 36, 956 (1976).
[CrossRef]

Raj, R.

P. A. Gass, I. Abram, R. Raj, and M. Schott, “The nonlinear optical spectrum of polydiacetylene in the near infrared,” J. Chem. Phys. 100, 88 (1994).
[CrossRef]

Sauteret, C.

C. Sauteret, J. P. Hermann, R. Frey, F. Pradère, J. Ducuing, R. H. Baughman, and R. R. Chance, “Optical nonlinearities in one-dimensional-conjugated polymer crystals,” Phys. Rev. Lett. 36, 956 (1976).
[CrossRef]

Schoenlein, R. W.

J. M. Huxley, P. Mataloni, R. W. Schoenlein, J. G. Fujimoto, E. P. Ippen, and G. M. Carter, “Femtosecond excited-state dynamics of polydiacetylene,” Appl. Phys. Lett. 56, 1600 (1990).
[CrossRef]

Schott, M.

P. A. Gass, I. Abram, R. Raj, and M. Schott, “The nonlinear optical spectrum of polydiacetylene in the near infrared,” J. Chem. Phys. 100, 88 (1994).
[CrossRef]

Schultes, H.

P. Strohriegl, H. Schultes, D. Heindl, P. Gruner-Bauer, V. Enkelmann, and E. Dormann, “Preparation, crystal structure and dielectric properties of the new unsymmetrically substituted diacetylenes NP/R2,” Ber. Bunsenges. Phys. Chem. 91, 918 (1987).
[CrossRef]

Schwoerer, M.

Th. Fehn, Th. Vogtmann, J. Hübner, and M. Schwoerer, “Anisotropy of the nonlinear optical susceptibility χ(3) in polydiacetylene single crystals,” Appl. Phys. B 59, 203 (1994).
[CrossRef]

Shen, Y. R.

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

Stegeman, G. I.

B. L. Lawrence, M. Cha, W. E. Torruellas, G. I. Stegeman, S. Etemad, and G. Baker, “Z-scan measurement of third and fifth order nonlinearities in single crystal PTS at 1064 nm,” Nonlin. Opt. 10, 193 (1995).

Strohriegl, P.

P. Strohriegl, J. Gmeiner, I. Müller, P. Gruner-Bauer, E. Dormann, and V. Enkelmann, “The asymmetrical diacetylene derivatives FBS/TFMBS and DNP/MNP: synthesis and solid state properties,” Ber. Bunsenges. Phys. Chem. 95, 491 (1991).
[CrossRef]

P. Strohriegl, H. Schultes, D. Heindl, P. Gruner-Bauer, V. Enkelmann, and E. Dormann, “Preparation, crystal structure and dielectric properties of the new unsymmetrically substituted diacetylenes NP/R2,” Ber. Bunsenges. Phys. Chem. 91, 918 (1987).
[CrossRef]

Sugihara, O.

Sugihashi, A.

R. Morita, T. Kondo, Y. Kaneda, A. Sugihashi, N. Ogasawara, S. Umegaki, and R. Ito, “Multiple-reflection effects in optical second-harmonic generation,” Jpn. J. Appl. Phys. 27, 1134 (1988).
[CrossRef]

Teng, C. C.

A. F. Garito, C. C. Teng, K. Y. Wong, and O. Zammani-Khamiri, “Molecular optics: nonlinear optical processes in organic and polymer crystals,” Mol. Cryst. Liq. Cryst. 106, 219 (1984).
[CrossRef]

Torruellas, W. E.

B. L. Lawrence, M. Cha, W. E. Torruellas, G. I. Stegeman, S. Etemad, and G. Baker, “Z-scan measurement of third and fifth order nonlinearities in single crystal PTS at 1064 nm,” Nonlin. Opt. 10, 193 (1995).

Umegaki, S.

R. Morita, T. Kondo, Y. Kaneda, A. Sugihashi, N. Ogasawara, S. Umegaki, and R. Ito, “Multiple-reflection effects in optical second-harmonic generation,” Jpn. J. Appl. Phys. 27, 1134 (1988).
[CrossRef]

Vogtmann, Th.

Th. Fehn, Th. Vogtmann, J. Hübner, and M. Schwoerer, “Anisotropy of the nonlinear optical susceptibility χ(3) in polydiacetylene single crystals,” Appl. Phys. B 59, 203 (1994).
[CrossRef]

Wegner, G.

G. Wegner, “Topochemical reactions of monomers with conjugated triple bonds. I. Polymerization of derivatives of 2,4-hexadiyn-1,6-diols in the crystalline state,” Z. Naturforsch. B 24, 824 (1969).

Wong, K. Y.

A. F. Garito, C. C. Teng, K. Y. Wong, and O. Zammani-Khamiri, “Molecular optics: nonlinear optical processes in organic and polymer crystals,” Mol. Cryst. Liq. Cryst. 106, 219 (1984).
[CrossRef]

Yeh, P.

P. Yeh, Optical Waves in Layered Media (Wiley, New York, 1988).

Yoshimura, T.

T. Yoshimura, “Enhancing second-order nonlinear optical properties by controlling the wave function in one-dimensional conjugated molecules,” Phys. Rev. B 40, 6292 (1989).
[CrossRef]

Zammani-Khamiri, O.

A. F. Garito, C. C. Teng, K. Y. Wong, and O. Zammani-Khamiri, “Molecular optics: nonlinear optical processes in organic and polymer crystals,” Mol. Cryst. Liq. Cryst. 106, 219 (1984).
[CrossRef]

Appl. Phys. B (1)

Th. Fehn, Th. Vogtmann, J. Hübner, and M. Schwoerer, “Anisotropy of the nonlinear optical susceptibility χ(3) in polydiacetylene single crystals,” Appl. Phys. B 59, 203 (1994).
[CrossRef]

Appl. Phys. Lett. (1)

J. M. Huxley, P. Mataloni, R. W. Schoenlein, J. G. Fujimoto, E. P. Ippen, and G. M. Carter, “Femtosecond excited-state dynamics of polydiacetylene,” Appl. Phys. Lett. 56, 1600 (1990).
[CrossRef]

Ber. Bunsenges. Phys. Chem. (2)

P. Strohriegl, H. Schultes, D. Heindl, P. Gruner-Bauer, V. Enkelmann, and E. Dormann, “Preparation, crystal structure and dielectric properties of the new unsymmetrically substituted diacetylenes NP/R2,” Ber. Bunsenges. Phys. Chem. 91, 918 (1987).
[CrossRef]

P. Strohriegl, J. Gmeiner, I. Müller, P. Gruner-Bauer, E. Dormann, and V. Enkelmann, “The asymmetrical diacetylene derivatives FBS/TFMBS and DNP/MNP: synthesis and solid state properties,” Ber. Bunsenges. Phys. Chem. 95, 491 (1991).
[CrossRef]

J. Appl. Phys. (1)

L. Kador, R. Fischer, R. Kasemann, S. Brück, and H. Dürr, “Fine structure in the χ(2) signals of inorganic-organic nanocomposites,” J. Appl. Phys. 75, 2709 (1994).
[CrossRef]

J. Chem. Phys. (1)

P. A. Gass, I. Abram, R. Raj, and M. Schott, “The nonlinear optical spectrum of polydiacetylene in the near infrared,” J. Chem. Phys. 100, 88 (1994).
[CrossRef]

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

Jpn. J. Appl. Phys. (1)

R. Morita, T. Kondo, Y. Kaneda, A. Sugihashi, N. Ogasawara, S. Umegaki, and R. Ito, “Multiple-reflection effects in optical second-harmonic generation,” Jpn. J. Appl. Phys. 27, 1134 (1988).
[CrossRef]

Makromol. Chem. (1)

P. S. Kalyanaraman, A. F. Garito, A. R. McGhie, and K. N. Desai, “Synthesis of nitrophenoxymethyl substituted diacetylene monomers,” Makromol. Chem. 180, 1393 (1979).
[CrossRef]

Mol. Cryst. Liq. Cryst. (1)

A. F. Garito, C. C. Teng, K. Y. Wong, and O. Zammani-Khamiri, “Molecular optics: nonlinear optical processes in organic and polymer crystals,” Mol. Cryst. Liq. Cryst. 106, 219 (1984).
[CrossRef]

Nonlin. Opt. (1)

B. L. Lawrence, M. Cha, W. E. Torruellas, G. I. Stegeman, S. Etemad, and G. Baker, “Z-scan measurement of third and fifth order nonlinearities in single crystal PTS at 1064 nm,” Nonlin. Opt. 10, 193 (1995).

Optoelectron. Dev. Technol. (1)

T. Kobayashi, “Ultrafast nonlinear optical processes in conjugated polymers,” Optoelectron. Dev. Technol. 8, 309 (1993).

Phys. Rev. B (1)

T. Yoshimura, “Enhancing second-order nonlinear optical properties by controlling the wave function in one-dimensional conjugated molecules,” Phys. Rev. B 40, 6292 (1989).
[CrossRef]

Phys. Rev. Lett. (1)

C. Sauteret, J. P. Hermann, R. Frey, F. Pradère, J. Ducuing, R. H. Baughman, and R. R. Chance, “Optical nonlinearities in one-dimensional-conjugated polymer crystals,” Phys. Rev. Lett. 36, 956 (1976).
[CrossRef]

Z. Naturforsch. B (1)

G. Wegner, “Topochemical reactions of monomers with conjugated triple bonds. I. Polymerization of derivatives of 2,4-hexadiyn-1,6-diols in the crystalline state,” Z. Naturforsch. B 24, 824 (1969).

Other (6)

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

Th. Fehn and F. Bauer, Physikalisches Institut, Universität Bayreuth, D-95440 Bayreuth, Germany (personal communication, 1996).

W. Milius, Chemisches Institut, Universität Bayreuth, D-95440 Bayreuth, Germany (personal communication, 1995).

P. N. Butcher and D. Cotter, The Elements of Nonlinear Optics, Vol. 9 of Cambridge Studies in Modern Optics (Cambridge U. Press, Cambridge, 1990).

P. Yeh, Optical Waves in Layered Media (Wiley, New York, 1988).

V. G. Dimitriev, G. G. Gurzadyan, and D. N. Nikogosyan, Handbook of Nonlinear Optical Crystals, Vol. 64 of Springer Series in Optical Science (Springer-Verlag, Heidelberg, 1991).

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Figures (6)

Fig. 1
Fig. 1

Schematic of topochemical solid-state polymerization in DA’s: monomer single crystal (left) and polymer single crystal (right).

Fig. 2
Fig. 2

Origin of the Maker fringes. Paths of rays with the wave vectors of the bound and the free waves in the crystal. The interference, depending on the angle of incidence ϕ, between the bound (kb) and the free (kf) waves generates the well-known Maker fringe oscillation pattern.

Fig. 3
Fig. 3

Reflected intensity depending on the angle of incidence: NP/4-MPU single crystal, 632.8 nm (p polarized), all theoretical curves (fits) made with the same parameters (na=1.66, nb=1.77, d=86.2 µm, B=24 µm). a, measurement; b, fit by the ray-tracer algorithm; c, fit by Fresnel’s formula, Eqs. (22); d, fit by the self-consistent field method, Eq. (23).

Fig. 4
Fig. 4

Partial beams in the ray-tracer algorithm: The incident beam is separated into partial beams of width b(ϕ), so the reflection of each partial beam can completely interfere with that of the neighboring partial beam. The intensity profile is considered.

Fig. 5
Fig. 5

SHG Maker fringes: measurement and theoretical curves. a, Measurement, NP/4-MPU single crystal, plane of incidence aˆbˆ, fundamental wavelength λ=987.1 nm, s-polarized; b, fit 1: theoretical curve calculated by Eqs. (21) and Fresnel’s formulas for the fundamental wave; c, fit 2: theoretical curve calculated by Eqs. (21) and the ray-tracer for the fundamental wave; d, the measured curve (a) and the theoretical curve (c) plotted in one diagram.

Fig. 6
Fig. 6

Detail of SHG Maker fringe: measurement and theoretical curve. NP/4-MPU single crystal, plane of incidence aˆbˆ, fundamental wavelength λ=987.1 nm, p polarized.

Tables (2)

Tables Icon

Table 1 Refractive Indices of NP/4-MPU Single Crystals for Several Wavelengths λ Determined by Interferometry, Reflectrometry, and SHG Maker Fringe Measurements

Tables Icon

Table 2 Values (pm V-1) of Modules of the Contracted Matrix d of NP/4-MPU Single Crystals Determined by SHG Maker Fringe Measurementsa

Equations (52)

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R1-CC-CC-R2,
R1=-CH2-O-phenyl-NO2;
R2=-CH2-O-CO-NH-phenyl-CH3.
P(2)=0000da,ac0000db,bc00dc,aadc,bbdc,cc000Ew,a2Ew,b2Ew,c22Ew,bEw,c2Ew,cEw,a2Ew,aEw,b,
××E2ω(1)-(2ω)2μεd¯¯2ωE2ω(1)=(2ω)2μP2ω(2).
××Eω(1)-ω2μεd¯¯ωEω(1)=0,
εd¯¯ω=εω,x000εω,y000εω,z.
E:=pˆQ exp{i[kω(1)r-ωt]},kω(1)=:(αω, 0, γ).
αω=kω,x(1)=kω,x(0)=(ω/c) sin ϕ.
mx(ω):=ω2μεω,x,my(ω):=ω2μεω,y,
mz(ω):=ω2μεω,z,
γ12=±[my(ω)-αω2]1/2(To/Ro),
γ3/4=±{[mx(ω)/mz(ω)][mz(ω)-αω2]}1/2(Te/Re).
pˆ1/2=(0, 1, 0)(To/Ro),
pˆ3/4=W-1[mz(ω)-αω2, 0, -αωγ3/4](Te/Re),
W:={[mz(ω)-αω2]2+(αωγ3)2}1/2.
Hi=cωμki×Ei=:hi̲|Ei|,
hi=cωμki×pˆi.
Eω(n)(r, t)=j=14pˆj(n)Qj(n)exp{i[kω,j(n)r-ωt]},
Hω(n)(r, t)=j=14hj(n)Qj(n)exp{i[kω,j(n)r-ωt]}.
xˆ·Eω(n-1)=xˆ·Eω(n),
yˆ·Hω(n-1)=yˆ·Hω(n),
yˆ·Eω(n-1)=yˆ·Eω(n)
xˆ·Hω(n-1)=xˆ·Hω(n).
Q(n-1)=D¯¯-1(n-1)D¯¯(n)P¯¯(n)Q(n),
Q(n):=[Q1(n), Q2(n), Q3(n), Q4(n)],
Pjk(n):=δjk exp[iγj(n)d(n)],
D1k(n):=xˆ·pˆk(n),D2k(n):=yˆ·hk(n),
D3k(n):=yˆ·pˆk(n),D4k(n):=xˆ·hk(n),
Ef(n)(r, t)=j=14pˆf,j(n)Qf,j(n)exp{i[kf,j(n)r-2ωt]},
Hf(n)(r, t)=j=14hf,j(n)Qf,j(n)exp{i[kf,j(n)r-2ωt]}.
Eb,j:=pˆb,jQb,j exp[i(kb,jr-2ωt)],
kb,j=(α2ω, 0, γb,j):=2kω,t/r(1),
M¯¯b,j(2ω)pˆb,jQb,j=(2ω)2μP2ω.
pˆb,jQb,j=(2ω)2μM¯¯b,j-1(2ω)P2ω.
pˆb,jQb,j=(2ω)2μ[α2ω2+γb,j2-my(2ω)]-1×(0, P2ω,y, 0)(To/Ro),
pˆb,jQb,j=(2ω)2μC-1([α2ω2-mz(2ω)]P2ω,x+α2ωγb,jP2ω,z,0, α2ωγb,jP2ω,x+[γb,j2-mx(2ω)]P2ω,z),(Te/Re),
C=[γb,j2-mx(2ω)][α2ω2-mz(2ω)]-(α2ωγb,j)2.
E(n)(r, t)=j=14pˆb,j(n)Qb,j(n)exp{i[kb,j(n)r-2ωt]}+j=14pˆf,j(n)Qf,j(n)×exp{i[kf,j(n)r-2ωt]},
H(n)(r, t)=j=14hb,j(n)Qb,j(n)exp{i[kb,j(n)r-2ωt]}+j=14hf,j(n)Qf,j(n)×exp{i[kf,j(n)r-2ωt]}.
Q(0)=D¯¯-1(0)D¯¯fP¯¯fQf+D¯¯-1(0)D¯¯bP¯¯bQb,
Q(2)=D¯¯-1(2)D¯¯fQf+D¯¯-1(2)D¯¯bQb.
Ireflected=Iincidentr01+k=120t01r102kt10.
Q(0)=D¯¯-1(0)D¯¯(1)P¯¯(1)D¯¯-1(1)D¯¯(2)P¯¯(2)Q(2).
b(φ)=(2α/γ)d cos φ,
IisRisIipRip=D¯¯-1(0)D¯¯(1)P¯¯(1)TioTRi-1oTieTRi-1e.
TioTRioTieTRie=D¯¯-1(1)D¯¯(2)TTis0TTip0.
Eω(1)(Traytrace/t12)1/2.
D¯¯(0)=D¯¯(2)=00cωδcωδ001μ-1μ1100-cωμδcωμδ00,D¯¯-1(0)=D¯¯-1(2)=0012-ωμ2cδ0012ωμ2cδω2cδμ200ω2cδ-μ200,
D¯¯(1)=00W-1[mz(ω)-αω2]W-1[mz(ω)-αω2]00cωμW-1mz(ω)γ3cωμW-1mz(ω)γ41100-cωμγ1-cωμγ200,
D¯¯f=00W2ω-1[mz(2ω)-α2ω2]W2ω-1(mz(2ω)-α2ω2)00c2ωμW2ω-1mz(2ω)γf,3c2ωμW2ω-1mz(2ω)γf,41100-c2ωμγf,1-c2ωμγf,200,
D¯¯b=00B-1{[α2ω2-mz(2ω)]P2ω,x+γb,3α2ωP2ω,z}000c2ωμB-1[mx(2ω)α2ωP2ω,z-γb,3mz(2ω)P2ω,x]01000-c2ωμγb,1000,

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