Abstract

Optical second-harmonic generation (SHG) is used as a noninvasive probe of two-dimensional (2D) ferroelectricity in Langmuir–Blodgett (LB) films of the copolymer vinylidene fluoride with trifluoroethylene. The surface 2D ferroelectric–paraelectric phase transition in the topmost layer of the LB films and a thickness-independent (almost 2D) transition in the bulk of these films are observed in temperature studies of SHG.

© 2000 Optical Society of America

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  1. N. D. Mermin and H. Wagner, Phys. Rev. Lett. 17, 1133 (1966).
    [CrossRef]
  2. D. Weller, S. F. Alvarado, W. Gudat, K. Schroder, and M. Campagna, Phys. Rev. Lett. 54, 1555 (1985).
    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
  11. J. F. Legrand, Ferroelectrics 91, 303 (1989).
    [CrossRef]

1999 (2)

G. Lüpke, Surf. Sci. Rep. 35, 75 (1999); J. F. McGilp, Phys. Status Solidi A 175, 153 (1999).
[CrossRef]

E. D. Mishina, T. V. Misuryaev, A. A. Nikulin, Th. Rasing, and O. A. Aktsipetrov, J. Opt. Soc. Am. B 16, 1692 (1999).
[CrossRef]

1998 (2)

S. Ducharme, A. V. Bune, L. M. Blinov, V. M. Fridkin, S. P. Palto, A. V. Sorokin, and S. G. Yudin, Phys. Rev. B 57, 25 (1998).
[CrossRef]

A. V. Bune, V. M. Fridkin, S. Durcharme, L. M. Blinov, S. P. Palto, A. V. Sorokin, S. G. Yudin, and A. Zlatkin, Nature 391, 874 (1998).
[CrossRef]

1994 (1)

G. J. Ashwell, P. D. Jackson, and W. A. Crossland, Nature 368, 438 (1994).
[CrossRef]

1989 (2)

G. G. Roberts, Ferroelectrics 91, 21 (1989).
[CrossRef]

J. F. Legrand, Ferroelectrics 91, 303 (1989).
[CrossRef]

1985 (1)

D. Weller, S. F. Alvarado, W. Gudat, K. Schroder, and M. Campagna, Phys. Rev. Lett. 54, 1555 (1985).
[CrossRef] [PubMed]

1984 (1)

O. A. Aktsipetrov and E. D. Mishina, Sov. Phys. Dokl. 29, 37 (1984).

1976 (1)

M. Pomerantz and A. Aviram, Solid State Commun. 20, 9 (1976).
[CrossRef]

1966 (1)

N. D. Mermin and H. Wagner, Phys. Rev. Lett. 17, 1133 (1966).
[CrossRef]

Aktsipetrov, O. A.

Alvarado, S. F.

D. Weller, S. F. Alvarado, W. Gudat, K. Schroder, and M. Campagna, Phys. Rev. Lett. 54, 1555 (1985).
[CrossRef] [PubMed]

Ashwell, G. J.

G. J. Ashwell, P. D. Jackson, and W. A. Crossland, Nature 368, 438 (1994).
[CrossRef]

Aviram, A.

M. Pomerantz and A. Aviram, Solid State Commun. 20, 9 (1976).
[CrossRef]

Blinov, L. M.

S. Ducharme, A. V. Bune, L. M. Blinov, V. M. Fridkin, S. P. Palto, A. V. Sorokin, and S. G. Yudin, Phys. Rev. B 57, 25 (1998).
[CrossRef]

A. V. Bune, V. M. Fridkin, S. Durcharme, L. M. Blinov, S. P. Palto, A. V. Sorokin, S. G. Yudin, and A. Zlatkin, Nature 391, 874 (1998).
[CrossRef]

Bune, A. V.

A. V. Bune, V. M. Fridkin, S. Durcharme, L. M. Blinov, S. P. Palto, A. V. Sorokin, S. G. Yudin, and A. Zlatkin, Nature 391, 874 (1998).
[CrossRef]

S. Ducharme, A. V. Bune, L. M. Blinov, V. M. Fridkin, S. P. Palto, A. V. Sorokin, and S. G. Yudin, Phys. Rev. B 57, 25 (1998).
[CrossRef]

Campagna, M.

D. Weller, S. F. Alvarado, W. Gudat, K. Schroder, and M. Campagna, Phys. Rev. Lett. 54, 1555 (1985).
[CrossRef] [PubMed]

Crossland, W. A.

G. J. Ashwell, P. D. Jackson, and W. A. Crossland, Nature 368, 438 (1994).
[CrossRef]

Ducharme, S.

S. Ducharme, A. V. Bune, L. M. Blinov, V. M. Fridkin, S. P. Palto, A. V. Sorokin, and S. G. Yudin, Phys. Rev. B 57, 25 (1998).
[CrossRef]

Durcharme, S.

A. V. Bune, V. M. Fridkin, S. Durcharme, L. M. Blinov, S. P. Palto, A. V. Sorokin, S. G. Yudin, and A. Zlatkin, Nature 391, 874 (1998).
[CrossRef]

Fridkin, V. M.

A. V. Bune, V. M. Fridkin, S. Durcharme, L. M. Blinov, S. P. Palto, A. V. Sorokin, S. G. Yudin, and A. Zlatkin, Nature 391, 874 (1998).
[CrossRef]

S. Ducharme, A. V. Bune, L. M. Blinov, V. M. Fridkin, S. P. Palto, A. V. Sorokin, and S. G. Yudin, Phys. Rev. B 57, 25 (1998).
[CrossRef]

Gudat, W.

D. Weller, S. F. Alvarado, W. Gudat, K. Schroder, and M. Campagna, Phys. Rev. Lett. 54, 1555 (1985).
[CrossRef] [PubMed]

Jackson, P. D.

G. J. Ashwell, P. D. Jackson, and W. A. Crossland, Nature 368, 438 (1994).
[CrossRef]

Legrand, J. F.

J. F. Legrand, Ferroelectrics 91, 303 (1989).
[CrossRef]

Lüpke, G.

G. Lüpke, Surf. Sci. Rep. 35, 75 (1999); J. F. McGilp, Phys. Status Solidi A 175, 153 (1999).
[CrossRef]

Mermin, N. D.

N. D. Mermin and H. Wagner, Phys. Rev. Lett. 17, 1133 (1966).
[CrossRef]

Mishina, E. D.

Misuryaev, T. V.

Nikulin, A. A.

Palto, S. P.

A. V. Bune, V. M. Fridkin, S. Durcharme, L. M. Blinov, S. P. Palto, A. V. Sorokin, S. G. Yudin, and A. Zlatkin, Nature 391, 874 (1998).
[CrossRef]

S. Ducharme, A. V. Bune, L. M. Blinov, V. M. Fridkin, S. P. Palto, A. V. Sorokin, and S. G. Yudin, Phys. Rev. B 57, 25 (1998).
[CrossRef]

Pomerantz, M.

M. Pomerantz and A. Aviram, Solid State Commun. 20, 9 (1976).
[CrossRef]

Rasing, Th.

Roberts, G. G.

G. G. Roberts, Ferroelectrics 91, 21 (1989).
[CrossRef]

Schroder, K.

D. Weller, S. F. Alvarado, W. Gudat, K. Schroder, and M. Campagna, Phys. Rev. Lett. 54, 1555 (1985).
[CrossRef] [PubMed]

Sorokin, A. V.

A. V. Bune, V. M. Fridkin, S. Durcharme, L. M. Blinov, S. P. Palto, A. V. Sorokin, S. G. Yudin, and A. Zlatkin, Nature 391, 874 (1998).
[CrossRef]

S. Ducharme, A. V. Bune, L. M. Blinov, V. M. Fridkin, S. P. Palto, A. V. Sorokin, and S. G. Yudin, Phys. Rev. B 57, 25 (1998).
[CrossRef]

Wagner, H.

N. D. Mermin and H. Wagner, Phys. Rev. Lett. 17, 1133 (1966).
[CrossRef]

Weller, D.

D. Weller, S. F. Alvarado, W. Gudat, K. Schroder, and M. Campagna, Phys. Rev. Lett. 54, 1555 (1985).
[CrossRef] [PubMed]

Yudin, S. G.

S. Ducharme, A. V. Bune, L. M. Blinov, V. M. Fridkin, S. P. Palto, A. V. Sorokin, and S. G. Yudin, Phys. Rev. B 57, 25 (1998).
[CrossRef]

A. V. Bune, V. M. Fridkin, S. Durcharme, L. M. Blinov, S. P. Palto, A. V. Sorokin, S. G. Yudin, and A. Zlatkin, Nature 391, 874 (1998).
[CrossRef]

Zlatkin, A.

A. V. Bune, V. M. Fridkin, S. Durcharme, L. M. Blinov, S. P. Palto, A. V. Sorokin, S. G. Yudin, and A. Zlatkin, Nature 391, 874 (1998).
[CrossRef]

Ferroelectrics (2)

G. G. Roberts, Ferroelectrics 91, 21 (1989).
[CrossRef]

J. F. Legrand, Ferroelectrics 91, 303 (1989).
[CrossRef]

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

Nature (2)

G. J. Ashwell, P. D. Jackson, and W. A. Crossland, Nature 368, 438 (1994).
[CrossRef]

A. V. Bune, V. M. Fridkin, S. Durcharme, L. M. Blinov, S. P. Palto, A. V. Sorokin, S. G. Yudin, and A. Zlatkin, Nature 391, 874 (1998).
[CrossRef]

Phys. Rev. B (1)

S. Ducharme, A. V. Bune, L. M. Blinov, V. M. Fridkin, S. P. Palto, A. V. Sorokin, and S. G. Yudin, Phys. Rev. B 57, 25 (1998).
[CrossRef]

Phys. Rev. Lett. (2)

N. D. Mermin and H. Wagner, Phys. Rev. Lett. 17, 1133 (1966).
[CrossRef]

D. Weller, S. F. Alvarado, W. Gudat, K. Schroder, and M. Campagna, Phys. Rev. Lett. 54, 1555 (1985).
[CrossRef] [PubMed]

Solid State Commun. (1)

M. Pomerantz and A. Aviram, Solid State Commun. 20, 9 (1976).
[CrossRef]

Sov. Phys. Dokl. (1)

O. A. Aktsipetrov and E. D. Mishina, Sov. Phys. Dokl. 29, 37 (1984).

Surf. Sci. Rep. (1)

G. Lüpke, Surf. Sci. Rep. 35, 75 (1999); J. F. McGilp, Phys. Status Solidi A 175, 153 (1999).
[CrossRef]

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Figures (2)

Fig. 1
Fig. 1

(a) Temperature dependence of the SHG intensity for a 60-monolayer-thick LB film. The arrows show the direction of the temperature variations. Filled and open symbols are for the heating and the cooling branches of the hysteresis loop, respectively. (b) Azimuthal angular dependence of the SHG intensity from a 15-monolayer-thick LB film. (c) Temperature dependence of the static dielectric constant (from Ref. 3).

Fig. 2
Fig. 2

(a) Schematic of the nonlinear optical model of ferroelectric LB film, which includes the air–LB film and the LB film–substrate interfaces with dipole quadratic susceptibilities, χ2,S1T and χ2,S2T, Curie temperatures TcS1 and TcS2, and bulk quadruple, χ2,Q, and dipole, χ2,dT, susceptibilities below the Curie temperature, TcB. (b), (c) Schematics of the model temperature dependences of the surface and the bulk susceptibilities and their interfering combinations for the model temperature dependence of the SHG intensity. (d) Experimental temperature dependence of the SHG intensity in the vicinity of the surface phase transition for a 15-monolayer-thick LB film. (e) Same as (d) but for a 60-monolayer-thick LB film.

Equations (1)

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I2ωTP2ωd,S1T+P2ωd,S2T2+P2ωd,bulkT+P2ωQ,bulk2,

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