Abstract

What is believed to be the first evidence of an all-optical orientation of a highly transparent polymer is presented. The samples are bulk rods of poly(methyl methacrylate) grafted with paranitroaniline (PNA) obtained by use of copolymerization of methyl methacrylate (MMA) monomers mixed with grafted MMA–PNA monomers. Bulk samples were obtained after molding and polishing of the copolymer with standard techniques. Experiments show that the photoinduced second-order1 susceptibility χ2 may occur through molecular reorientation following selective polar excitation of the nonlinear chromophores by simultaneous two- and three-photon absorption on the same electronic level.

© 1997 Optical Society of America

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References

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  1. Ch. Bosshard, K. Sutter, Ph. Prêtre, J. Hullinger, M. Flörsheimez, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon and Breach, Amsterdam, The Netherlands, 1995), Vol.  1.
  2. S. Bauer, J. Appl. Phys. 80, 5531 (1996).
    [Crossref]
  3. C. Fiorini, J.-M. Nunzi, F. Charra, and P. Raimond, Opt. Photon. News 7(12) 12 (1996); A.-C. Etilé, C. Fiorini, F. Charra, and J.-M. Nunzi, Phys. Rev. A 56, 3888 (1997).
    [Crossref]
  4. R. H. Stolen and H. W. K. Tom, Opt. Lett. 12, 585 (1987).
    [Crossref] [PubMed]
  5. C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, J. Opt. Am. B 14, 1984 (1997).
    [Crossref]
  6. W. Chalupczak, C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, Opt. Commun. 126, 103 (1996).
    [Crossref]
  7. C. Fiorini, J. M. Nunzi, F. Charra, F. Kajzar, M. Lequan, R. M. Lequan, and K. Chane-Ching, Chem. Phys. Lett. 271, 335 (1997).
    [Crossref]
  8. J. L. Oudar and D. S. Chemla, J. Chem. Phys. 66, 2264 (1976).
  9. W. Liptay, Chem. Int. Ed. Engl. 8, 177 (1969).
    [Crossref]
  10. J.-M. Nunzi, C. Fiorini, and A.-C. Etilé, “All-optical poling in polymers: dynamical aspects and perspectives,” Proc. SPIE3147 (to be published).
  11. M. Dumont, G. Froc, and S. Hosotte, Nonlin. Opt. 9, 327 (1995).
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    [Crossref]

1997 (2)

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, J. Opt. Am. B 14, 1984 (1997).
[Crossref]

C. Fiorini, J. M. Nunzi, F. Charra, F. Kajzar, M. Lequan, R. M. Lequan, and K. Chane-Ching, Chem. Phys. Lett. 271, 335 (1997).
[Crossref]

1996 (3)

W. Chalupczak, C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, Opt. Commun. 126, 103 (1996).
[Crossref]

S. Bauer, J. Appl. Phys. 80, 5531 (1996).
[Crossref]

C. Fiorini, J.-M. Nunzi, F. Charra, and P. Raimond, Opt. Photon. News 7(12) 12 (1996); A.-C. Etilé, C. Fiorini, F. Charra, and J.-M. Nunzi, Phys. Rev. A 56, 3888 (1997).
[Crossref]

1995 (1)

M. Dumont, G. Froc, and S. Hosotte, Nonlin. Opt. 9, 327 (1995).

1992 (1)

P. Rochon, J. Gosselin, A. Nathansohn, and S. Xie, Appl. Phys. Lett. 60, 4 (1992).
[Crossref]

1987 (1)

1976 (1)

J. L. Oudar and D. S. Chemla, J. Chem. Phys. 66, 2264 (1976).

1969 (1)

W. Liptay, Chem. Int. Ed. Engl. 8, 177 (1969).
[Crossref]

Bauer, S.

S. Bauer, J. Appl. Phys. 80, 5531 (1996).
[Crossref]

Bosshard, Ch.

Ch. Bosshard, K. Sutter, Ph. Prêtre, J. Hullinger, M. Flörsheimez, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon and Breach, Amsterdam, The Netherlands, 1995), Vol.  1.

Chalupczak, W.

W. Chalupczak, C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, Opt. Commun. 126, 103 (1996).
[Crossref]

Chane-Ching, K.

C. Fiorini, J. M. Nunzi, F. Charra, F. Kajzar, M. Lequan, R. M. Lequan, and K. Chane-Ching, Chem. Phys. Lett. 271, 335 (1997).
[Crossref]

Charra, F.

C. Fiorini, J. M. Nunzi, F. Charra, F. Kajzar, M. Lequan, R. M. Lequan, and K. Chane-Ching, Chem. Phys. Lett. 271, 335 (1997).
[Crossref]

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, J. Opt. Am. B 14, 1984 (1997).
[Crossref]

W. Chalupczak, C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, Opt. Commun. 126, 103 (1996).
[Crossref]

C. Fiorini, J.-M. Nunzi, F. Charra, and P. Raimond, Opt. Photon. News 7(12) 12 (1996); A.-C. Etilé, C. Fiorini, F. Charra, and J.-M. Nunzi, Phys. Rev. A 56, 3888 (1997).
[Crossref]

Chemla, D. S.

J. L. Oudar and D. S. Chemla, J. Chem. Phys. 66, 2264 (1976).

Dumont, M.

M. Dumont, G. Froc, and S. Hosotte, Nonlin. Opt. 9, 327 (1995).

Etilé, A.-C.

J.-M. Nunzi, C. Fiorini, and A.-C. Etilé, “All-optical poling in polymers: dynamical aspects and perspectives,” Proc. SPIE3147 (to be published).

Fiorini, C.

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, J. Opt. Am. B 14, 1984 (1997).
[Crossref]

C. Fiorini, J. M. Nunzi, F. Charra, F. Kajzar, M. Lequan, R. M. Lequan, and K. Chane-Ching, Chem. Phys. Lett. 271, 335 (1997).
[Crossref]

W. Chalupczak, C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, Opt. Commun. 126, 103 (1996).
[Crossref]

C. Fiorini, J.-M. Nunzi, F. Charra, and P. Raimond, Opt. Photon. News 7(12) 12 (1996); A.-C. Etilé, C. Fiorini, F. Charra, and J.-M. Nunzi, Phys. Rev. A 56, 3888 (1997).
[Crossref]

J.-M. Nunzi, C. Fiorini, and A.-C. Etilé, “All-optical poling in polymers: dynamical aspects and perspectives,” Proc. SPIE3147 (to be published).

Flörsheimez, M.

Ch. Bosshard, K. Sutter, Ph. Prêtre, J. Hullinger, M. Flörsheimez, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon and Breach, Amsterdam, The Netherlands, 1995), Vol.  1.

Froc, G.

M. Dumont, G. Froc, and S. Hosotte, Nonlin. Opt. 9, 327 (1995).

Gosselin, J.

P. Rochon, J. Gosselin, A. Nathansohn, and S. Xie, Appl. Phys. Lett. 60, 4 (1992).
[Crossref]

Günter, P.

Ch. Bosshard, K. Sutter, Ph. Prêtre, J. Hullinger, M. Flörsheimez, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon and Breach, Amsterdam, The Netherlands, 1995), Vol.  1.

Hosotte, S.

M. Dumont, G. Froc, and S. Hosotte, Nonlin. Opt. 9, 327 (1995).

Hullinger, J.

Ch. Bosshard, K. Sutter, Ph. Prêtre, J. Hullinger, M. Flörsheimez, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon and Breach, Amsterdam, The Netherlands, 1995), Vol.  1.

Kaatz, P.

Ch. Bosshard, K. Sutter, Ph. Prêtre, J. Hullinger, M. Flörsheimez, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon and Breach, Amsterdam, The Netherlands, 1995), Vol.  1.

Kajzar, F.

C. Fiorini, J. M. Nunzi, F. Charra, F. Kajzar, M. Lequan, R. M. Lequan, and K. Chane-Ching, Chem. Phys. Lett. 271, 335 (1997).
[Crossref]

Lequan, M.

C. Fiorini, J. M. Nunzi, F. Charra, F. Kajzar, M. Lequan, R. M. Lequan, and K. Chane-Ching, Chem. Phys. Lett. 271, 335 (1997).
[Crossref]

Lequan, R. M.

C. Fiorini, J. M. Nunzi, F. Charra, F. Kajzar, M. Lequan, R. M. Lequan, and K. Chane-Ching, Chem. Phys. Lett. 271, 335 (1997).
[Crossref]

Liptay, W.

W. Liptay, Chem. Int. Ed. Engl. 8, 177 (1969).
[Crossref]

Nathansohn, A.

P. Rochon, J. Gosselin, A. Nathansohn, and S. Xie, Appl. Phys. Lett. 60, 4 (1992).
[Crossref]

Nunzi, J. M.

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, J. Opt. Am. B 14, 1984 (1997).
[Crossref]

C. Fiorini, J. M. Nunzi, F. Charra, F. Kajzar, M. Lequan, R. M. Lequan, and K. Chane-Ching, Chem. Phys. Lett. 271, 335 (1997).
[Crossref]

W. Chalupczak, C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, Opt. Commun. 126, 103 (1996).
[Crossref]

Nunzi, J.-M.

C. Fiorini, J.-M. Nunzi, F. Charra, and P. Raimond, Opt. Photon. News 7(12) 12 (1996); A.-C. Etilé, C. Fiorini, F. Charra, and J.-M. Nunzi, Phys. Rev. A 56, 3888 (1997).
[Crossref]

J.-M. Nunzi, C. Fiorini, and A.-C. Etilé, “All-optical poling in polymers: dynamical aspects and perspectives,” Proc. SPIE3147 (to be published).

Oudar, J. L.

J. L. Oudar and D. S. Chemla, J. Chem. Phys. 66, 2264 (1976).

Prêtre, Ph.

Ch. Bosshard, K. Sutter, Ph. Prêtre, J. Hullinger, M. Flörsheimez, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon and Breach, Amsterdam, The Netherlands, 1995), Vol.  1.

Raimond, P.

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, J. Opt. Am. B 14, 1984 (1997).
[Crossref]

W. Chalupczak, C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, Opt. Commun. 126, 103 (1996).
[Crossref]

C. Fiorini, J.-M. Nunzi, F. Charra, and P. Raimond, Opt. Photon. News 7(12) 12 (1996); A.-C. Etilé, C. Fiorini, F. Charra, and J.-M. Nunzi, Phys. Rev. A 56, 3888 (1997).
[Crossref]

Rochon, P.

P. Rochon, J. Gosselin, A. Nathansohn, and S. Xie, Appl. Phys. Lett. 60, 4 (1992).
[Crossref]

Stolen, R. H.

Sutter, K.

Ch. Bosshard, K. Sutter, Ph. Prêtre, J. Hullinger, M. Flörsheimez, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon and Breach, Amsterdam, The Netherlands, 1995), Vol.  1.

Tom, H. W. K.

Xie, S.

P. Rochon, J. Gosselin, A. Nathansohn, and S. Xie, Appl. Phys. Lett. 60, 4 (1992).
[Crossref]

Appl. Phys. Lett. (1)

P. Rochon, J. Gosselin, A. Nathansohn, and S. Xie, Appl. Phys. Lett. 60, 4 (1992).
[Crossref]

Chem. Int. Ed. Engl. (1)

W. Liptay, Chem. Int. Ed. Engl. 8, 177 (1969).
[Crossref]

Chem. Phys. Lett. (1)

C. Fiorini, J. M. Nunzi, F. Charra, F. Kajzar, M. Lequan, R. M. Lequan, and K. Chane-Ching, Chem. Phys. Lett. 271, 335 (1997).
[Crossref]

J. Appl. Phys. (1)

S. Bauer, J. Appl. Phys. 80, 5531 (1996).
[Crossref]

J. Chem. Phys. (1)

J. L. Oudar and D. S. Chemla, J. Chem. Phys. 66, 2264 (1976).

J. Opt. Am. B (1)

C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, J. Opt. Am. B 14, 1984 (1997).
[Crossref]

Nonlin. Opt. (1)

M. Dumont, G. Froc, and S. Hosotte, Nonlin. Opt. 9, 327 (1995).

Opt. Commun. (1)

W. Chalupczak, C. Fiorini, F. Charra, J. M. Nunzi, and P. Raimond, Opt. Commun. 126, 103 (1996).
[Crossref]

Opt. Lett. (1)

Opt. Photon. News (1)

C. Fiorini, J.-M. Nunzi, F. Charra, and P. Raimond, Opt. Photon. News 7(12) 12 (1996); A.-C. Etilé, C. Fiorini, F. Charra, and J.-M. Nunzi, Phys. Rev. A 56, 3888 (1997).
[Crossref]

Other (2)

Ch. Bosshard, K. Sutter, Ph. Prêtre, J. Hullinger, M. Flörsheimez, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon and Breach, Amsterdam, The Netherlands, 1995), Vol.  1.

J.-M. Nunzi, C. Fiorini, and A.-C. Etilé, “All-optical poling in polymers: dynamical aspects and perspectives,” Proc. SPIE3147 (to be published).

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Figures (3)

Fig. 1
Fig. 1

Typical growth of the photoinduced second-order susceptibility χ2 recorded in an 8-mm-thick PMMA–PNA copolymer rod. The writing-beam fluences at the fundamental and the second-harmonic frequencies are 3 GW/cm2, respectively. The curve is a fit to the usual poling dynamics.10 We interrupted data acquisition with the growth period to avoid overflow. Inset, chemical representation of the PMMA–PNA copolymer n=2.

Fig. 2
Fig. 2

Dependence of the initial photoinduced χ2 growth on the product of the ω- and the 2ω-frequency writing-beam intensities, Iω2I2ω. Inset, expected polar excitation scheme with simultaneous two- and three-photon absorption on the same electronic level.

Fig. 3
Fig. 3

Dependence of the SH susceptibility χ2,sat extrapolated at saturation with the intensity ratio between the writing beams at frequencies ω and 2ω. The curve is a fit to a χ2,satX/γ2+X2 dependence, with X=E2ω/Eω2.6,10

Equations (2)

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

P019μ01E2ω 2ΔμEω2+μ01Eω 2ΔμEω44ω2+3μ01E2ωΔμEωμ01Eω*ΔμEω*2+3μ01E2ω*ΔμEω*μ01EωΔμEω22ω,
E2ωEω2=Δμ32ωcos θ21/2=Δμ332ω.

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