Abstract

Phase-matched χ(2) polarization in a polymeric waveguide induced by an all-optical poling technique was investigated. We fabricated the polymeric waveguide on a quartz substrate by casting from a chloroform solution of poly(methyl methacrylate) with 1,4-bis(2-{4-[N,N-di(p-tolyl)amino]phenyl}vinyl) benzene (BTAPVB). The waveguide film was found to have no absorption at either the fundamental (1064 nm) or the second-harmonic (532 nm) wavelengths. We observed that the induced second-harmonic intensity has a quadratic dependence on the propagation length. This quadratic dependence suggests that the phase-matched χ(2) polarization was formed along the direction of the beam propagation. The analysis of χ(2) tensor components supports the fact that BTAPVB possesses an octupolar component in addition to a dipolar one.

© 2003 Optical Society of America

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References

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  1. C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, “Photoinduced non centrosymmetry in azo-dye polymers,” Nonlinear Opt. 9, 339–347 (1995).
  2. C. Fiorini, F. Charra, J.-M. Nunzi, I. D. W. Samuel, and J. Zyss, “Light-induced second-harmonic generation in an octupolar dye,” Opt. Lett. 20, 2469–2471 (1995).
    [CrossRef] [PubMed]
  3. N. Tsutsumi, Y. Ikeyama, and W. Sakai, “Self-organized phase-matched second harmonic generation from the all optically induced χ(2) polar structures,” Nonlinear Opt. 22, 63–66 (1999).
  4. N. Tsutsumi, J. Yamamoto, and W. Sakai, “Diffraction measurement for grating formed in optically polymeric materials,” Jpn. J. Appl. Phys., 40, 2264–2268 (2001).
    [CrossRef]
  5. N. Tsutsumi, M. Imamura, W. Sakai, Y. Nagase, N. Nemoto, Y. Tian, and J. Abe, “All optically induced χ(2) structures and their optical anisotropy in betaine dispersed in polymer matrix,” Jpn. J. Appl. Phys. 41, 5247–5253 (2002).
    [CrossRef]
  6. W. Chalupczak, C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Efficient all-optical poling of an azo-dye copolymer using a low power laser,” Opt. Commun. 126, 103–107 (1996).
    [CrossRef]
  7. C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Quasi-permanent all-optical encoding of noncentrosymmetry in azo-dye polymers,” J. Opt. Soc. Am. B 14, 1984–2003 (1997).
    [CrossRef]
  8. S. Brasselet and J. Zyss, “Relation between quantum geometric dimensionalities in molecular nonlinear optics: beyond the two-level model for anisotropic systems,” J. Nonlinear Opt. Phys. Mater. 5, 671–693 (1996).
    [CrossRef]
  9. S. Brasselet and J. Zyss, “Control of the polarization dependence of optically poled nonlinear polymer films,” Opt. Lett. 22, 1464–1466 (1997).
    [CrossRef]
  10. A.-C. Etilé, C. Fiorini, F. Charra, and J. M. Nunzi, “Phase-coherent control of the molecular polar order in polymers using dual-frequency interferences between circularly polarized beams,” Phys. Rev. A 56, 3888–3896 (1997).
    [CrossRef]
  11. J. Si, J. Qiu, K. Kitaoka, and K. Hirao, “Photoinduced phase-matched second-harmonic generation in azodye-doped polymer films,” J. Appl. Phys. 89, 2029–2032 (2001).
    [CrossRef]
  12. J. Si, J. Qiu, and K. Hirao, “Control of the noncentrosymmetry of thick polymer films by nonresonant all-optical poling,” J. Appl. Phys. 90, 4895–4899 (2001).
    [CrossRef]
  13. C. Fiorini, F. Charra, P. Raimond, A. Lorin, and J.-M. Nunzi, “All-optical induction of noncentrosymmetry in a transparent nonlinear polymer rod,” Opt. Lett. 22, 1846–1848 (1997).
    [CrossRef]
  14. V. M. Churikov and C.-C. Hsu, “Dynamics of photoinduced second order nonlinearity in dimethylamino-nitrostilbene polymer thin films,” Opt. Commun. 190, 367–371 (2001).
    [CrossRef]
  15. P. N. Parasad and D. J. Williams, Introduction to Nonlinear Optical Effects in Molecules and Polymers (Wiley-Interscience, New York, 1991), Chap. 11.

2002 (1)

N. Tsutsumi, M. Imamura, W. Sakai, Y. Nagase, N. Nemoto, Y. Tian, and J. Abe, “All optically induced χ(2) structures and their optical anisotropy in betaine dispersed in polymer matrix,” Jpn. J. Appl. Phys. 41, 5247–5253 (2002).
[CrossRef]

2001 (4)

N. Tsutsumi, J. Yamamoto, and W. Sakai, “Diffraction measurement for grating formed in optically polymeric materials,” Jpn. J. Appl. Phys., 40, 2264–2268 (2001).
[CrossRef]

J. Si, J. Qiu, K. Kitaoka, and K. Hirao, “Photoinduced phase-matched second-harmonic generation in azodye-doped polymer films,” J. Appl. Phys. 89, 2029–2032 (2001).
[CrossRef]

J. Si, J. Qiu, and K. Hirao, “Control of the noncentrosymmetry of thick polymer films by nonresonant all-optical poling,” J. Appl. Phys. 90, 4895–4899 (2001).
[CrossRef]

V. M. Churikov and C.-C. Hsu, “Dynamics of photoinduced second order nonlinearity in dimethylamino-nitrostilbene polymer thin films,” Opt. Commun. 190, 367–371 (2001).
[CrossRef]

1999 (1)

N. Tsutsumi, Y. Ikeyama, and W. Sakai, “Self-organized phase-matched second harmonic generation from the all optically induced χ(2) polar structures,” Nonlinear Opt. 22, 63–66 (1999).

1997 (4)

1996 (2)

S. Brasselet and J. Zyss, “Relation between quantum geometric dimensionalities in molecular nonlinear optics: beyond the two-level model for anisotropic systems,” J. Nonlinear Opt. Phys. Mater. 5, 671–693 (1996).
[CrossRef]

W. Chalupczak, C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Efficient all-optical poling of an azo-dye copolymer using a low power laser,” Opt. Commun. 126, 103–107 (1996).
[CrossRef]

1995 (2)

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, “Photoinduced non centrosymmetry in azo-dye polymers,” Nonlinear Opt. 9, 339–347 (1995).

C. Fiorini, F. Charra, J.-M. Nunzi, I. D. W. Samuel, and J. Zyss, “Light-induced second-harmonic generation in an octupolar dye,” Opt. Lett. 20, 2469–2471 (1995).
[CrossRef] [PubMed]

Abe, J.

N. Tsutsumi, M. Imamura, W. Sakai, Y. Nagase, N. Nemoto, Y. Tian, and J. Abe, “All optically induced χ(2) structures and their optical anisotropy in betaine dispersed in polymer matrix,” Jpn. J. Appl. Phys. 41, 5247–5253 (2002).
[CrossRef]

Brasselet, S.

S. Brasselet and J. Zyss, “Control of the polarization dependence of optically poled nonlinear polymer films,” Opt. Lett. 22, 1464–1466 (1997).
[CrossRef]

S. Brasselet and J. Zyss, “Relation between quantum geometric dimensionalities in molecular nonlinear optics: beyond the two-level model for anisotropic systems,” J. Nonlinear Opt. Phys. Mater. 5, 671–693 (1996).
[CrossRef]

Chalupczak, W.

W. Chalupczak, C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Efficient all-optical poling of an azo-dye copolymer using a low power laser,” Opt. Commun. 126, 103–107 (1996).
[CrossRef]

Charra, F.

A.-C. Etilé, C. Fiorini, F. Charra, and J. M. Nunzi, “Phase-coherent control of the molecular polar order in polymers using dual-frequency interferences between circularly polarized beams,” Phys. Rev. A 56, 3888–3896 (1997).
[CrossRef]

C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Quasi-permanent all-optical encoding of noncentrosymmetry in azo-dye polymers,” J. Opt. Soc. Am. B 14, 1984–2003 (1997).
[CrossRef]

C. Fiorini, F. Charra, P. Raimond, A. Lorin, and J.-M. Nunzi, “All-optical induction of noncentrosymmetry in a transparent nonlinear polymer rod,” Opt. Lett. 22, 1846–1848 (1997).
[CrossRef]

W. Chalupczak, C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Efficient all-optical poling of an azo-dye copolymer using a low power laser,” Opt. Commun. 126, 103–107 (1996).
[CrossRef]

C. Fiorini, F. Charra, J.-M. Nunzi, I. D. W. Samuel, and J. Zyss, “Light-induced second-harmonic generation in an octupolar dye,” Opt. Lett. 20, 2469–2471 (1995).
[CrossRef] [PubMed]

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, “Photoinduced non centrosymmetry in azo-dye polymers,” Nonlinear Opt. 9, 339–347 (1995).

Churikov, V. M.

V. M. Churikov and C.-C. Hsu, “Dynamics of photoinduced second order nonlinearity in dimethylamino-nitrostilbene polymer thin films,” Opt. Commun. 190, 367–371 (2001).
[CrossRef]

Etilé, A.-C.

A.-C. Etilé, C. Fiorini, F. Charra, and J. M. Nunzi, “Phase-coherent control of the molecular polar order in polymers using dual-frequency interferences between circularly polarized beams,” Phys. Rev. A 56, 3888–3896 (1997).
[CrossRef]

Fiorini, C.

A.-C. Etilé, C. Fiorini, F. Charra, and J. M. Nunzi, “Phase-coherent control of the molecular polar order in polymers using dual-frequency interferences between circularly polarized beams,” Phys. Rev. A 56, 3888–3896 (1997).
[CrossRef]

C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Quasi-permanent all-optical encoding of noncentrosymmetry in azo-dye polymers,” J. Opt. Soc. Am. B 14, 1984–2003 (1997).
[CrossRef]

C. Fiorini, F. Charra, P. Raimond, A. Lorin, and J.-M. Nunzi, “All-optical induction of noncentrosymmetry in a transparent nonlinear polymer rod,” Opt. Lett. 22, 1846–1848 (1997).
[CrossRef]

W. Chalupczak, C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Efficient all-optical poling of an azo-dye copolymer using a low power laser,” Opt. Commun. 126, 103–107 (1996).
[CrossRef]

C. Fiorini, F. Charra, J.-M. Nunzi, I. D. W. Samuel, and J. Zyss, “Light-induced second-harmonic generation in an octupolar dye,” Opt. Lett. 20, 2469–2471 (1995).
[CrossRef] [PubMed]

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, “Photoinduced non centrosymmetry in azo-dye polymers,” Nonlinear Opt. 9, 339–347 (1995).

Hirao, K.

J. Si, J. Qiu, K. Kitaoka, and K. Hirao, “Photoinduced phase-matched second-harmonic generation in azodye-doped polymer films,” J. Appl. Phys. 89, 2029–2032 (2001).
[CrossRef]

J. Si, J. Qiu, and K. Hirao, “Control of the noncentrosymmetry of thick polymer films by nonresonant all-optical poling,” J. Appl. Phys. 90, 4895–4899 (2001).
[CrossRef]

Hsu, C.-C.

V. M. Churikov and C.-C. Hsu, “Dynamics of photoinduced second order nonlinearity in dimethylamino-nitrostilbene polymer thin films,” Opt. Commun. 190, 367–371 (2001).
[CrossRef]

Ikeyama, Y.

N. Tsutsumi, Y. Ikeyama, and W. Sakai, “Self-organized phase-matched second harmonic generation from the all optically induced χ(2) polar structures,” Nonlinear Opt. 22, 63–66 (1999).

Imamura, M.

N. Tsutsumi, M. Imamura, W. Sakai, Y. Nagase, N. Nemoto, Y. Tian, and J. Abe, “All optically induced χ(2) structures and their optical anisotropy in betaine dispersed in polymer matrix,” Jpn. J. Appl. Phys. 41, 5247–5253 (2002).
[CrossRef]

Kitaoka, K.

J. Si, J. Qiu, K. Kitaoka, and K. Hirao, “Photoinduced phase-matched second-harmonic generation in azodye-doped polymer films,” J. Appl. Phys. 89, 2029–2032 (2001).
[CrossRef]

Lorin, A.

Nagase, Y.

N. Tsutsumi, M. Imamura, W. Sakai, Y. Nagase, N. Nemoto, Y. Tian, and J. Abe, “All optically induced χ(2) structures and their optical anisotropy in betaine dispersed in polymer matrix,” Jpn. J. Appl. Phys. 41, 5247–5253 (2002).
[CrossRef]

Nemoto, N.

N. Tsutsumi, M. Imamura, W. Sakai, Y. Nagase, N. Nemoto, Y. Tian, and J. Abe, “All optically induced χ(2) structures and their optical anisotropy in betaine dispersed in polymer matrix,” Jpn. J. Appl. Phys. 41, 5247–5253 (2002).
[CrossRef]

Nunzi, J. M.

A.-C. Etilé, C. Fiorini, F. Charra, and J. M. Nunzi, “Phase-coherent control of the molecular polar order in polymers using dual-frequency interferences between circularly polarized beams,” Phys. Rev. A 56, 3888–3896 (1997).
[CrossRef]

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, “Photoinduced non centrosymmetry in azo-dye polymers,” Nonlinear Opt. 9, 339–347 (1995).

Nunzi, J.-M.

Qiu, J.

J. Si, J. Qiu, K. Kitaoka, and K. Hirao, “Photoinduced phase-matched second-harmonic generation in azodye-doped polymer films,” J. Appl. Phys. 89, 2029–2032 (2001).
[CrossRef]

J. Si, J. Qiu, and K. Hirao, “Control of the noncentrosymmetry of thick polymer films by nonresonant all-optical poling,” J. Appl. Phys. 90, 4895–4899 (2001).
[CrossRef]

Raimond, P.

C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Quasi-permanent all-optical encoding of noncentrosymmetry in azo-dye polymers,” J. Opt. Soc. Am. B 14, 1984–2003 (1997).
[CrossRef]

C. Fiorini, F. Charra, P. Raimond, A. Lorin, and J.-M. Nunzi, “All-optical induction of noncentrosymmetry in a transparent nonlinear polymer rod,” Opt. Lett. 22, 1846–1848 (1997).
[CrossRef]

W. Chalupczak, C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Efficient all-optical poling of an azo-dye copolymer using a low power laser,” Opt. Commun. 126, 103–107 (1996).
[CrossRef]

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, “Photoinduced non centrosymmetry in azo-dye polymers,” Nonlinear Opt. 9, 339–347 (1995).

Sakai, W.

N. Tsutsumi, M. Imamura, W. Sakai, Y. Nagase, N. Nemoto, Y. Tian, and J. Abe, “All optically induced χ(2) structures and their optical anisotropy in betaine dispersed in polymer matrix,” Jpn. J. Appl. Phys. 41, 5247–5253 (2002).
[CrossRef]

N. Tsutsumi, J. Yamamoto, and W. Sakai, “Diffraction measurement for grating formed in optically polymeric materials,” Jpn. J. Appl. Phys., 40, 2264–2268 (2001).
[CrossRef]

N. Tsutsumi, Y. Ikeyama, and W. Sakai, “Self-organized phase-matched second harmonic generation from the all optically induced χ(2) polar structures,” Nonlinear Opt. 22, 63–66 (1999).

Samuel, I. D. W.

Si, J.

J. Si, J. Qiu, K. Kitaoka, and K. Hirao, “Photoinduced phase-matched second-harmonic generation in azodye-doped polymer films,” J. Appl. Phys. 89, 2029–2032 (2001).
[CrossRef]

J. Si, J. Qiu, and K. Hirao, “Control of the noncentrosymmetry of thick polymer films by nonresonant all-optical poling,” J. Appl. Phys. 90, 4895–4899 (2001).
[CrossRef]

Tian, Y.

N. Tsutsumi, M. Imamura, W. Sakai, Y. Nagase, N. Nemoto, Y. Tian, and J. Abe, “All optically induced χ(2) structures and their optical anisotropy in betaine dispersed in polymer matrix,” Jpn. J. Appl. Phys. 41, 5247–5253 (2002).
[CrossRef]

Tsutsumi, N.

N. Tsutsumi, M. Imamura, W. Sakai, Y. Nagase, N. Nemoto, Y. Tian, and J. Abe, “All optically induced χ(2) structures and their optical anisotropy in betaine dispersed in polymer matrix,” Jpn. J. Appl. Phys. 41, 5247–5253 (2002).
[CrossRef]

N. Tsutsumi, J. Yamamoto, and W. Sakai, “Diffraction measurement for grating formed in optically polymeric materials,” Jpn. J. Appl. Phys., 40, 2264–2268 (2001).
[CrossRef]

N. Tsutsumi, Y. Ikeyama, and W. Sakai, “Self-organized phase-matched second harmonic generation from the all optically induced χ(2) polar structures,” Nonlinear Opt. 22, 63–66 (1999).

Yamamoto, J.

N. Tsutsumi, J. Yamamoto, and W. Sakai, “Diffraction measurement for grating formed in optically polymeric materials,” Jpn. J. Appl. Phys., 40, 2264–2268 (2001).
[CrossRef]

Zyss, J.

J. Appl. Phys. (2)

J. Si, J. Qiu, K. Kitaoka, and K. Hirao, “Photoinduced phase-matched second-harmonic generation in azodye-doped polymer films,” J. Appl. Phys. 89, 2029–2032 (2001).
[CrossRef]

J. Si, J. Qiu, and K. Hirao, “Control of the noncentrosymmetry of thick polymer films by nonresonant all-optical poling,” J. Appl. Phys. 90, 4895–4899 (2001).
[CrossRef]

J. Nonlinear Opt. Phys. Mater. (1)

S. Brasselet and J. Zyss, “Relation between quantum geometric dimensionalities in molecular nonlinear optics: beyond the two-level model for anisotropic systems,” J. Nonlinear Opt. Phys. Mater. 5, 671–693 (1996).
[CrossRef]

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

Jpn. J. Appl. Phys. (2)

N. Tsutsumi, J. Yamamoto, and W. Sakai, “Diffraction measurement for grating formed in optically polymeric materials,” Jpn. J. Appl. Phys., 40, 2264–2268 (2001).
[CrossRef]

N. Tsutsumi, M. Imamura, W. Sakai, Y. Nagase, N. Nemoto, Y. Tian, and J. Abe, “All optically induced χ(2) structures and their optical anisotropy in betaine dispersed in polymer matrix,” Jpn. J. Appl. Phys. 41, 5247–5253 (2002).
[CrossRef]

Nonlinear Opt. (2)

N. Tsutsumi, Y. Ikeyama, and W. Sakai, “Self-organized phase-matched second harmonic generation from the all optically induced χ(2) polar structures,” Nonlinear Opt. 22, 63–66 (1999).

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, “Photoinduced non centrosymmetry in azo-dye polymers,” Nonlinear Opt. 9, 339–347 (1995).

Opt. Commun. (2)

W. Chalupczak, C. Fiorini, F. Charra, J.-M. Nunzi, and P. Raimond, “Efficient all-optical poling of an azo-dye copolymer using a low power laser,” Opt. Commun. 126, 103–107 (1996).
[CrossRef]

V. M. Churikov and C.-C. Hsu, “Dynamics of photoinduced second order nonlinearity in dimethylamino-nitrostilbene polymer thin films,” Opt. Commun. 190, 367–371 (2001).
[CrossRef]

Opt. Lett. (3)

Phys. Rev. A (1)

A.-C. Etilé, C. Fiorini, F. Charra, and J. M. Nunzi, “Phase-coherent control of the molecular polar order in polymers using dual-frequency interferences between circularly polarized beams,” Phys. Rev. A 56, 3888–3896 (1997).
[CrossRef]

Other (1)

P. N. Parasad and D. J. Williams, Introduction to Nonlinear Optical Effects in Molecules and Polymers (Wiley-Interscience, New York, 1991), Chap. 11.

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Figures (9)

Fig. 1
Fig. 1

(a) Chemical structure of BTAPVB. (b) Geometrically optimized molecular structure of BTAPVB.

Fig. 2
Fig. 2

Absorption spectrum in the UV and visible wavelength regions of BTAPVB in PMMA polymer film.

Fig. 3
Fig. 3

Optimization of fundamental and SH energies for optical poling: (a) dependence of χ(2) value (relative) on E2ω/Eω2; (b) plots of the initial growth rate of the relative χ(2) value dχ(2)/dt versus Eω4E2ω; (c) increase of I2ωSHG/Iω2 on poling time for various fundamental energies.

Fig. 4
Fig. 4

Schematic of the waveguide mode optical poling. The values of np, nf, and na are the refractive indices of prism, thin film, and air, respectively. θp is an angle of incidence with respect to the sample normal, θ is an angle of incidence from air to prism, and θ is the corresponding angle of refraction in the prism. α is 45° in this case.

Fig. 5
Fig. 5

(a) Increase of I2ωSHG/Iω2 as a function of time for various waveguide thicknesses. The propagation path is fixed at 5 mm. (b) Logarithmic plots of I2ωSHG/Iω2 and the initial SH growth rate [d(I2ωSHG/Iω2)/dt] as a function of waveguide thickness.

Fig. 6
Fig. 6

(a) Increase of I2ωSHG/Iω2 as a function of time for various propagation lengths in waveguide mode optical poling. (b) Logarithmic plots of I2ωSHG/Iω2 and the initial SH growth rate [d(I2ωSHG/Iω2)/dt] as a function of propagation length.

Fig. 7
Fig. 7

(a) Increase of I2ωSHG/Iω2 as a function of time for various propagation lengths (film thickness) for a normal mode optical poling. (b) Logarithmic plots of I2ωSHG/Iω2 and the initial SH growth rate [d(I2ωSHG/Iω2)/dt] as a function of propagation length (film thickness).

Fig. 8
Fig. 8

Configuration of sample rotation. Angle δ is a simultaneous rotation angle of the polarizer and the analyzer.

Fig. 9
Fig. 9

Plots of the square root of I2ωSHG/Iω2 as a function of rotation angle δ. The solid curve represents a theoretical fit that was obtained with Eq. (5).

Tables (1)

Tables Icon

Table 1 Summary of Refractive Indices and Angles of the Waveguide Mode for Sample Films When BTAPVB Concentration Varies

Equations (5)

Equations on this page are rendered with MathJax. Learn more.

npk sin θp=v(m)=nfk
npsin θ=nasin θ,
θ=θp-α,
I2ωSHG=ω2deff24n2c210OD Iω2l2,
χΔΔΔ(2)=Nβiii0A3cos3 δ+35 (A1-A3)cos δ,

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