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Journal of the Optical Society of America B

Journal of the Optical Society of America B


  • Vol. 15, Iss. 1 — Jan. 1, 1998
  • pp: 466–470

Improved second-harmonic generation from homomolecular Langmuir–Blodgett films of a transparent dye

Geoffrey J. Ashwell, Tokuhiko Handa, and Rakesh Ranjan  »View Author Affiliations

JOSA B, Vol. 15, Issue 1, pp. 466-470 (1998)

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The optically nonlinear dye [E-N-dodecyl-4-(2-(4-docosyloxyphenyl)ethenyl)quinolinium]+-(octadecylsulfate-)x(bromide-)1-x forms noncentrosymmetric Langmuir–Blodgett films. The second-harmonic intensity increases quadratically with the number of layers in the range investigated, i.e., as I2ω(N)=I2ω(1)N2 for 2N100, and shows long-term stability. Films of the dye are almost transparent, with an absorbance of 3×10-4 layer-1 at the second-harmonic wavelength, but, nonetheless, the equivalent monolayer intensity, I2ω(N)/N2, is 30% of the resonantly enhanced signal from monolayer films of the colored hemicyanine dye reported by Girling [J. Opt. Soc. Am. B 4, 950 (1987)]. The second-order susceptibility, film thickness, and chromophore tilt angle relative to the normal to the substrate are χzzz(2)=26 pm V-1 at 1.064 μm, l=5.0 nm layer-1, and ϕ=30°, respectively, for x=0.5.

© 1998 Optical Society of America

OCIS Codes
(310.3840) Thin films : Materials and process characterization

Geoffrey J. Ashwell, Tokuhiko Handa, and Rakesh Ranjan, "Improved second-harmonic generation from homomolecular Langmuir Blodgett films of a transparent dye," J. Opt. Soc. Am. B 15, 466-470 (1998)

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  1. I. R. Girling, N. A. Cade, P. V. Kolinsky, R. J. Jones, I. R. Peterson, M. M. Ahmad, D. B. Neal, M. C. Petty, G. G. Roberts, and W. J. Feast, “Second-harmonic generation in mixed hemicyanine-fatty acid Langmuir–Blodgett multilayers,” J. Opt. Soc. Am. B 4, 950–955 (1987). [CrossRef]
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  5. G. J. Ashwell, E. J. C. Dawnay, A. P. Kuczynski, and P. J. Martin, “The highest observed second-harmonic intensity from a multilayered Langmuir–Blodgett film structure,” in Physical Concepts of Materials for Novel Optoelectronic Device Applications. I. Materials Growth and Characterization, M. Razeghi, ed., Proc. SPIE 1361, 589–598 (1991). [CrossRef]
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  7. G. J. Ashwell, P. D. Jackson, D. Lochun, W. A. Crossland, P. A. Thompson, G. S. Bahra, C. R. Brown, and C. Jasper, “Second-harmonic generation from alternate-layer LB films: quadratic enhancement with film thickness,” Proc. R. Soc. London Ser. A 445, 385–398 (1994). [CrossRef]
  8. G. J. Ashwell, T. W. Walker, I. R. Gentle, G. J. Foran, G. S. Bahra, and C. R. Brown, “Molecular zips: evidence of the interdigitation of layers in Langmuir–Blodgett films of an optically nonlinear dye and a compatible spacer,” J. Mater. Chem. 6, 969–974 (1996). [CrossRef]
  9. O. A. Aktsipetrov, N. N. Akhmediev, I. M. Baranova, E. D. Mishina, and V. R. Novak, “Multilayer Langmuir films for optoelectronics,” Soviet Tech. Phys. Lett. 11, 249–250 (1985).
  10. T. Richardson, G. G. Roberts, M. E. C. Polywka, and S. G. Davies, “Preparation and characterization of organotransition metal Langmuir–Blodgett films,” Thin Solid Films 160, 231–239 (1988). [CrossRef]
  11. S. H. Ou, J. A. Mann, J. B. Lando, L. Zhou, and K. D. Singer, “Nonlinear optical studies of polar polymeric Langmuir–Schaefer films,” Appl. Phys. Lett. 61, 2284–2286 (1992). [CrossRef]
  12. M. A. Rutkis, E. Wistus, S. E. Lindquist, E. Mukhtar, G. Liberts, V. A. Zauls, A. B. Klimkans, and E. A. Silinsh, “Langmuir–Blodgett films of indandione-1, 3-pyridinium betaine. III. Linear dichroism and nonlinear optical properties,” Adv. Mater. Opt. Electron. 6, 39–50 (1996). [CrossRef]
  13. G. J. Ashwell, G. Jefferies, E. J. C. Dawnay, A. P. Kuczynski, D. E. Lynch, G. Yu, and D. G. Bucknall, “Linear and nonlinear optical properties of the different Langmuir–Blodgett phases of CnH2n+1–Q3CNQ,” J. Mater. Chem. 5, 975–980 (1995). [CrossRef]
  14. G. J. Ashwell, P. D. Jackson, and W. A. Crossland, “Non-centrosymmetry and second-harmonic generation in Z-type Langmuir–Blodgett films,” Nature (London) 368438–440 (1994). [CrossRef]
  15. G. J. Ashwell, G. Jefferies, C. D. George, R. Ranjan, R. B. Charters, and R. P. Tatam, “Z-type Langmuir–Blodgett film structures: surface plasmon resonance, second-harmonic generation and fibre optic devices,” J. Mater. Chem. 6, 131–136 (1996). [CrossRef]
  16. G. J. Ashwell, P. D. Jackson, G. Jefferies, I. R. Gentle, and C. H. L. Kennard, “Controlling the structure of transparent Langmuir–Blodgett films for nonlinear optical applications,” J. Mater. Chem. 6, 137–141 (1996). [CrossRef]
  17. G. J. Ashwell, D. Lochun, G. S. Bahra, C. R. Brown, I. R. Gentle, and C. H. L. Kennard, “Non-centrosymmetric alignment of optically nonlinear dyes,” Supramolec. Sci. 2, 131–134 (1995).
  18. G. Decher, B. Tieke, C. Bosshard, and P. Günter, “Optical second-harmonic generation in Langmuir–Blodgett films of 2-docosylamino-5-nitropyridine,” J. Chem. Soc. Chem. Commun. 933–934 (1988). [CrossRef]
  19. G. Decher, B. Tieke, C. Bosshard, and P. Günter, “Optical second-harmonic generation in Langmuir–Blodgett films of novel donor-acceptor substituted pyridine and benzene derivatives,” Ferroelectrics 91, 193–207 (1989). [CrossRef]
  20. G. J. Ashwell, T. Handa, G. Jefferies, and D. G. Hamilton, “Linear and nonlinear optical properties of Z-type Langmuir–Blodgett films of a benzothiazolium dye,” Colloids Surf. A 102, 133–136 (1995). [CrossRef]
  21. G. J. Ashwell, T. Handa, G. Jefferies, T. W. Walker, M. R. Bryce, and A. M. Grainger, “Langmuir–Blodgett deposition and nonlinear optical properties of a two-legged dye,” Supramolec. Sci. 4, 219–222 (1997).
  22. H. M. Wang, “Reflection-transmission measurements of anisotropic films with one of the principal axes in the direction of columnar growth,” J. Mod. Opt. 42, 497–505 (1995). [CrossRef]
  23. K. Kajikawa, K. Kigata, H. Takezoe, and A. Fukuda, “Second-harmonic generation from Langmuir–Blodgett films in various optical geometries,” Mol. Cryst. Liq. Cryst. 182, 91–101 (1990).

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