OSA's Digital Library

Journal of the Optical Society of America B

Journal of the Optical Society of America B

| OPTICAL PHYSICS

  • Vol. 15, Iss. 1 — Jan. 1, 1998
  • pp: 369–378

Study of domain formation and relaxation in thin polymeric films by femtosecond hyper-Rayleigh scattering

Geert Olbrechts, Erik J. H. Put, David Van Steenwinckel, Koen Clays, André Persoons, Celest Samyn, and Naoki Matsuda  »View Author Affiliations


JOSA B, Vol. 15, Issue 1, pp. 369-378 (1998)
http://dx.doi.org/10.1364/JOSAB.15.000369


View Full Text Article

Acrobat PDF (256 KB)





Browse Journals / Lookup Meetings

Browse by Journal and Year


   


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools

Share
Citations

Abstract

Femtosecond hyper-Rayleigh scattering has been used to probe the spatial orientational fluctuations between nonlinear optical chromophores as dopants in spin-coated polymer films. The fluctuation in the second-order incoherently scattered light intensity on microtranslation of the solid sample is indicative of the degree of spatial correlation between the individual chromophores. The decay of the autocorrelation function of this fluctuating signal is characterized by a spatial correlation length. Electric-field poling of dipolar chromophores is shown to increase this correlation length. The temporal characteristics of the correlation length have been studied and compared with thermal relaxation times obtained with coherent second-harmonic generation. The correlation length decays much faster than the second-harmonic intensity. Possible implications of this fast relaxation are addressed.

© 1998 Optical Society of America

OCIS Codes
(190.0190) Nonlinear optics : Nonlinear optics
(190.4710) Nonlinear optics : Optical nonlinearities in organic materials
(290.5870) Scattering : Scattering, Rayleigh
(320.2250) Ultrafast optics : Femtosecond phenomena

Citation
Geert Olbrechts, Erik J. H. Put, David Van Steenwinckel, Koen Clays, André Persoons, Celest Samyn, and Naoki Matsuda, "Study of domain formation and relaxation in thin polymeric films by femtosecond hyper-Rayleigh scattering," J. Opt. Soc. Am. B 15, 369-378 (1998)
http://www.opticsinfobase.org/josab/abstract.cfm?URI=josab-15-1-369


Sort:  Author  |  Year  |  Journal  |  Reset

References

  1. D. J. Williams, Introduction to Nonlinear Optical Effects in Molecules and Polymers (Wiley, New York, 1991).
  2. B. F. Levine and C. G. Bethea, “Second and third order hyperpolarizabilities of organic molecules,” J. Chem. Phys. 63, 2666–2682 (1975).
  3. K. D. Singer and A. F. Garito, “Measurements of molecular second order optical susceptibilities using dc induced second harmonic generation,” J. Chem. Phys. 75, 3572–3580 (1981).
  4. G. R. Meredith, “Small computer-based system for determination of second- and third-order optical nonlinearities,” Rev. Sci. Instrum. 53, 48–53 (1982).
  5. K. Clays and A. Persoons, “Hyper-Rayleigh scattering in solution,” Phys. Rev. Lett. 66, 2980–2983 (1991).
  6. K. Clays and A. Persoons, “Hyper-Rayleigh scattering in solution,” Rev. Sci. Instrum. 63, 3285–3289 (1992).
  7. K. Clays, A. Persoons, and L. De Maeyer, “Hyper-Rayleigh scattering in solution,” in Modern Nonlinear Optics, Part 3, M. Evans and S. Kielich, eds. (Wiley, New York, 1994), pp. 455–498.
  8. T. Verbiest, K. Clays, A. Persoons, F. Meyers, and J.-L. Brédas, “Determination of the hyperpolarizability of an octopolar molecular ion by hyper-Rayleigh scattering,” Opt. Lett. 18, 525–527 (1993).
  9. T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, and A. Persoons, “Investigations of the hyperpolarizability in organic molecules from dipolar to octopolar systems,” J. Am. Chem. Soc. 116, 9320–9323 (1994).
  10. C. Dhenaut, I. Ledoux, I. D. W. Samuel, J. Zyss, M. Bourgault, and H. L. Bozec, “Chiral metal complexes with large octupolar optical nonlinearities,” Nature 374, 339–342 (1995).
  11. W. M. Laidlaw, R. G. Denning, T. Verbiest, E. Chauchard, and A. Persoons, “Large second-order optical polarizabilities in mixed-valence metal complexes,” Nature 363, 58–59 (1993).
  12. K. Clays, E. Hendrickx, M. Triest, T. Verbiest, A. Persoons, C. Dehu, and J.-L. Brédas, “Nonlinear optical properties of proteins measured by hyper-Rayleigh scattering in solution,” Science 262, 1419–1422 (1993).
  13. K. Clays and A. Persoons, “Hyper-Rayleigh scattering in solution with tunable femtosecond continuous-wave laser source,” Rev. Sci. Instrum. 65, 2190–2194 (1994).
  14. O. F. J. Noordman and N. F. v. Hulst, “Time-resolved hyper-Rayleigh scattering: measuring first hyperpolarizabilities b of fluorescent molecules,” Chem. Phys. Lett. 253, 145–150 (1996).
  15. K. Clays, J. S. Schildkraut, and D. J. Williams, “Phase-matched second-harmonic generation in a four-layered polymeric waveguide,” J. Opt. Soc. Am. B 11, 655–664 (1994).
  16. O. K. Song, C. H. Wang, B. R. Cho, and J. T. Je, “Measurement of first-order hyperpolarizability of several barbituric acid derivatives in solution by hyper-Rayleigh scattering,” J. Phys. Chem. 99, 6808–6811 (1995).
  17. M. A. Pauley, H.-W. Guan, C. H. Wang, and A. K.-Y. Jen, “Determination of first hyperpolarizability of nonlinear optical chromophores by second-harmonic scattering using an external reference,” J. Chem. Phys. 104, 7821–7829 (1996).
  18. A. E. Siegman, Lasers (Oxford U. Press, Oxford, 1986).
  19. R. Bersohn, Y.-H. Pao, and H. L. Frisch, “Double-quantum light scattering by molecules,” J. Chem. Phys. 45, 3184–3507 (1966).
  20. T. Verbiest, E. Hendrickx, A. Persoons, and K. Clays, “Measurements of molecular hyperpolarizabilities using hyper-Rayleigh scattering,” in Nonlinear Optical Properties of Organic Materials V, D. J. Williams, ed., Proc. SPIE 1775, 206–212 (1992).
  21. G. J. T. Heesink, A. G. T. Ruiter, N. F. vanHulst, and B. Bölger, “Determination of hyperpolarizability tensor components by depolarized hyper-Rayleigh scattering,” Phys. Rev. Lett. 71, 999–1002 (1993).
  22. M. Kauranen and A. Persoons, “Theory of polarization measurements of second-order nonlinear light scattering,” J. Chem. Phys. 104, 3445–3456 (1996).
  23. I. D. Morrison, R. G. Denning, W. M. Laidlaw, and M. A. Stammers, “Measurement of first hyperpolarizabilities by hyper-Rayleigh scattering,” Rev. Sci. Instrum. 67, 1445–1453 (1996).
  24. M. Flörsheimer, M. Küpfer, C. Bosshard, H. Looser, and P. Günter, “Phase-matched optical second-harmonic generation in Langmuir–Blodgett film waveguides by mode conversion,” Adv. Mater. 4, 795–798 (1992).
  25. K. Clays, M. Wu, and A. Persoons, “Femtosecond hyper-Rayleigh scattering study of spatial orientational correlations between chromophores,” J. Nonlinear Opt. Phys. Mater. 5, 59–71 (1996).
  26. C. A. Bosshard, “Optical and nonlinear optical properties of 2-cylcooctylamino-5-nitropyridine and 2-docosylamino-5-nitropyridine molecules, crystals and Langmuir–Blodgett films,” Ph.D. dissertation (Swiss Federal Institute of Technology, Lausanne, Switzerland, 1991).
  27. G. Olbrechts, E. Put, K. Clays, A. Persoons, and N. Matsuda, “Probing of spatial orientational correlations between chromophores in polymer films by femtosecond hyper-Rayleigh scattering,” Chem. Phys. Lett. 253, 135–140 (1996).
  28. G. Khanarian, R. A. Norwood, D. Haas, B. Feuer, and D. Karim, “Phase-matched second-harmonic generation in a polymer waveguide,” Appl. Phys. Lett. 57, 977–979 (1990).
  29. T. L. Penner, H. R. Motschmann, N. J. Armstrong, M. C. Ezenyilimba, and D. J. Williams, “Efficient phase-matched second-harmonic generation of blue light in an organic waveguide,” Nature 367, 49–51 (1994).
  30. N. Matsuda, G. Olbrechts, E. J. H. Put, K. Clays, and A. Persoons, “Comparison between optical nonlinearity relaxation times from coherent second-harmonic generation and from incoherent hyper-Rayleigh scattering,” Appl. Phys. Lett. 69, 4145–4147 (1996).
  31. D. M. Burland, R. D. Miller, and C. A. Walsh, “Second-order nonlinearity in poled-polymer systems,” Chem. Rev. 94, 31–75 (1994).
  32. T. Verbiest, D. M. Burland, M. C. Jurich, V. Y. Lee, R. D. Miller, and W. Volksen, “Exceptionally thermally stable polyimides for second-order nonlinear optical applications,” Science 268, 1604–1606 (1995).
  33. T. Verbiest and D. M. Burland, “The use of the Wagner function to describe poled-order relaxation processes in electrooptic polymers,” Chem. Phys. Lett. 236, 253–258 (1995).
  34. B. J. Berne and R. Pecora, Dynamic Light Scattering (Wiley Interscience, New York, 1975).

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