Abstract

Incoherent optical second harmonic (SH) generation, or hyper-Rayleigh scattering (HRS), is used to study the structure and properties of Gd/C18H36O2 multilayer Langmuir–Blodgett (LB) films. SH reflection spectra (in combination with linear absorption spectra), HRS indicatrices, thickness dependence, and wave polarization diagrams are measured for s-polarized fundamental radiation. The SH radiation is entirely diffuse but predominantly s polarized, with the maximum of the HRS indicatrix shifted by 8° relative to the specular direction, which is interpreted as being due to the contribution of a fluctuating quadrupole to the nonlinear-optical response of the films. The estimated correlation length of spatial fluctuations of the nonlinear-optical polarization in the film is ∼400 nm. These properties are associated with an islandlike structure formed by Gd ions inside LB structural units.

© 2000 Optical Society of America

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  1. C. Boutton, K. Clays, A. Persoons, T. Wada, and H. Sasabe, “Second-order off-diagonal hyperpolarizability tensor components of substituted carbazoles by hyper-Rayleigh scattering depolarization measurements,” Chem. Phys. Lett. 286, 101–106 (1998).
    [CrossRef]
  2. T. W. Chui and K. Y. Wong, “Study of hyper-Rayleigh scat-tering and two-photon absorption induced fluorescence from crystal violet,” J. Chem. Phys. 109, 1391–1396 (1998).
    [CrossRef]
  3. R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurements of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
    [CrossRef]
  4. P. D. Maker, “Spectral broadening of elastic second-harmonic light scattering in liquids,” Phys. Rev. A 1, 923–951 (1970).
    [CrossRef]
  5. S. Kielich, Molecular Nonlinear Optics (Mir, Moscow, 1974; in Russian).
  6. O. A. Aktsipetrov, A. A. Fedyanin, T. V. Murzina, G. P. Borisevich, and A. A. Kononenko, “Electro- and photoinduced effects in optical second-harmonic generation and hyper-Rayleigh scattering from thin films of bacteriorhodopsin,” J. Opt. Soc. Am. B 14, 771–776 (1997).
    [CrossRef]
  7. O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
    [CrossRef]
  8. O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
    [CrossRef]
  9. E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
    [CrossRef]
  10. A. M. Tishin, Yu. A. Koksharov, J. Bohr, and G. B. Khomutov, “Evidence for magnetic ordering in ultrathin gadolinium Langmuir–Blodgett films,” Phys. Rev. B 55, 11064–11067 (1997).
    [CrossRef]
  11. O. A. Aktsipetrov, I. M. Baranova, and Yu. A. Il’inskii, “Surface contribution to the generation of reflected second harmonic for centrosymmetric semiconductors,” Zh. Eksp. Teor. Fiz. 91, 287–296 (1986) [ Sov. Phys. JETP 64, 167–172 (1986)].
  12. N. Bloembergen, R. K. Chang, S. S. Jha, and C. H. Lee, “Optical second harmonic generation in reflection from media with inversion symmetry,” Phys. Rev. 174, 813–822 (1968).
    [CrossRef]
  13. L. D. Landau and E. M. Lifshits, Field Theory (Nauka, Moscow, 1973; in Russian).

1998 (2)

C. Boutton, K. Clays, A. Persoons, T. Wada, and H. Sasabe, “Second-order off-diagonal hyperpolarizability tensor components of substituted carbazoles by hyper-Rayleigh scattering depolarization measurements,” Chem. Phys. Lett. 286, 101–106 (1998).
[CrossRef]

T. W. Chui and K. Y. Wong, “Study of hyper-Rayleigh scat-tering and two-photon absorption induced fluorescence from crystal violet,” J. Chem. Phys. 109, 1391–1396 (1998).
[CrossRef]

1997 (4)

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

A. M. Tishin, Yu. A. Koksharov, J. Bohr, and G. B. Khomutov, “Evidence for magnetic ordering in ultrathin gadolinium Langmuir–Blodgett films,” Phys. Rev. B 55, 11064–11067 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, T. V. Murzina, G. P. Borisevich, and A. A. Kononenko, “Electro- and photoinduced effects in optical second-harmonic generation and hyper-Rayleigh scattering from thin films of bacteriorhodopsin,” J. Opt. Soc. Am. B 14, 771–776 (1997).
[CrossRef]

1996 (1)

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

1986 (1)

O. A. Aktsipetrov, I. M. Baranova, and Yu. A. Il’inskii, “Surface contribution to the generation of reflected second harmonic for centrosymmetric semiconductors,” Zh. Eksp. Teor. Fiz. 91, 287–296 (1986) [ Sov. Phys. JETP 64, 167–172 (1986)].

1970 (1)

P. D. Maker, “Spectral broadening of elastic second-harmonic light scattering in liquids,” Phys. Rev. A 1, 923–951 (1970).
[CrossRef]

1968 (1)

N. Bloembergen, R. K. Chang, S. S. Jha, and C. H. Lee, “Optical second harmonic generation in reflection from media with inversion symmetry,” Phys. Rev. 174, 813–822 (1968).
[CrossRef]

1965 (1)

R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurements of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
[CrossRef]

Aktsipetrov, O. A.

O. A. Aktsipetrov, A. A. Fedyanin, T. V. Murzina, G. P. Borisevich, and A. A. Kononenko, “Electro- and photoinduced effects in optical second-harmonic generation and hyper-Rayleigh scattering from thin films of bacteriorhodopsin,” J. Opt. Soc. Am. B 14, 771–776 (1997).
[CrossRef]

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

O. A. Aktsipetrov, I. M. Baranova, and Yu. A. Il’inskii, “Surface contribution to the generation of reflected second harmonic for centrosymmetric semiconductors,” Zh. Eksp. Teor. Fiz. 91, 287–296 (1986) [ Sov. Phys. JETP 64, 167–172 (1986)].

Baranova, I. M.

O. A. Aktsipetrov, I. M. Baranova, and Yu. A. Il’inskii, “Surface contribution to the generation of reflected second harmonic for centrosymmetric semiconductors,” Zh. Eksp. Teor. Fiz. 91, 287–296 (1986) [ Sov. Phys. JETP 64, 167–172 (1986)].

Bloembergen, N.

N. Bloembergen, R. K. Chang, S. S. Jha, and C. H. Lee, “Optical second harmonic generation in reflection from media with inversion symmetry,” Phys. Rev. 174, 813–822 (1968).
[CrossRef]

Bohr, J.

A. M. Tishin, Yu. A. Koksharov, J. Bohr, and G. B. Khomutov, “Evidence for magnetic ordering in ultrathin gadolinium Langmuir–Blodgett films,” Phys. Rev. B 55, 11064–11067 (1997).
[CrossRef]

Borisevich, G. P.

Boutton, C.

C. Boutton, K. Clays, A. Persoons, T. Wada, and H. Sasabe, “Second-order off-diagonal hyperpolarizability tensor components of substituted carbazoles by hyper-Rayleigh scattering depolarization measurements,” Chem. Phys. Lett. 286, 101–106 (1998).
[CrossRef]

Chang, R. K.

N. Bloembergen, R. K. Chang, S. S. Jha, and C. H. Lee, “Optical second harmonic generation in reflection from media with inversion symmetry,” Phys. Rev. 174, 813–822 (1968).
[CrossRef]

Chui, T. W.

T. W. Chui and K. Y. Wong, “Study of hyper-Rayleigh scat-tering and two-photon absorption induced fluorescence from crystal violet,” J. Chem. Phys. 109, 1391–1396 (1998).
[CrossRef]

Clays, K.

C. Boutton, K. Clays, A. Persoons, T. Wada, and H. Sasabe, “Second-order off-diagonal hyperpolarizability tensor components of substituted carbazoles by hyper-Rayleigh scattering depolarization measurements,” Chem. Phys. Lett. 286, 101–106 (1998).
[CrossRef]

Devillers, M. A. C.

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

Fedyanin, A. A.

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, T. V. Murzina, G. P. Borisevich, and A. A. Kononenko, “Electro- and photoinduced effects in optical second-harmonic generation and hyper-Rayleigh scattering from thin films of bacteriorhodopsin,” J. Opt. Soc. Am. B 14, 771–776 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

Il’inskii, Yu. A.

O. A. Aktsipetrov, I. M. Baranova, and Yu. A. Il’inskii, “Surface contribution to the generation of reflected second harmonic for centrosymmetric semiconductors,” Zh. Eksp. Teor. Fiz. 91, 287–296 (1986) [ Sov. Phys. JETP 64, 167–172 (1986)].

Jha, S. S.

N. Bloembergen, R. K. Chang, S. S. Jha, and C. H. Lee, “Optical second harmonic generation in reflection from media with inversion symmetry,” Phys. Rev. 174, 813–822 (1968).
[CrossRef]

Khomutov, G. B.

A. M. Tishin, Yu. A. Koksharov, J. Bohr, and G. B. Khomutov, “Evidence for magnetic ordering in ultrathin gadolinium Langmuir–Blodgett films,” Phys. Rev. B 55, 11064–11067 (1997).
[CrossRef]

Klimkin, D. A.

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

Koksharov, Yu. A.

A. M. Tishin, Yu. A. Koksharov, J. Bohr, and G. B. Khomutov, “Evidence for magnetic ordering in ultrathin gadolinium Langmuir–Blodgett films,” Phys. Rev. B 55, 11064–11067 (1997).
[CrossRef]

Kononenko, A. A.

Lee, C. H.

N. Bloembergen, R. K. Chang, S. S. Jha, and C. H. Lee, “Optical second harmonic generation in reflection from media with inversion symmetry,” Phys. Rev. 174, 813–822 (1968).
[CrossRef]

Maker, P. D.

P. D. Maker, “Spectral broadening of elastic second-harmonic light scattering in liquids,” Phys. Rev. A 1, 923–951 (1970).
[CrossRef]

R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurements of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
[CrossRef]

Mishina, E. D.

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

Murzina, T. V.

Nikulin, A. A.

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

Novak, V. R.

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

Persoons, A.

C. Boutton, K. Clays, A. Persoons, T. Wada, and H. Sasabe, “Second-order off-diagonal hyperpolarizability tensor components of substituted carbazoles by hyper-Rayleigh scattering depolarization measurements,” Chem. Phys. Lett. 286, 101–106 (1998).
[CrossRef]

Rasing, Th.

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

Sasabe, H.

C. Boutton, K. Clays, A. Persoons, T. Wada, and H. Sasabe, “Second-order off-diagonal hyperpolarizability tensor components of substituted carbazoles by hyper-Rayleigh scattering depolarization measurements,” Chem. Phys. Lett. 286, 101–106 (1998).
[CrossRef]

Savage, C. M.

R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurements of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
[CrossRef]

Sigov, A. S.

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

Terhune, R. W.

R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurements of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
[CrossRef]

Tishin, A. M.

A. M. Tishin, Yu. A. Koksharov, J. Bohr, and G. B. Khomutov, “Evidence for magnetic ordering in ultrathin gadolinium Langmuir–Blodgett films,” Phys. Rev. B 55, 11064–11067 (1997).
[CrossRef]

Vorob’eva, S. L.

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

Vorotilov, K. A.

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

Wada, T.

C. Boutton, K. Clays, A. Persoons, T. Wada, and H. Sasabe, “Second-order off-diagonal hyperpolarizability tensor components of substituted carbazoles by hyper-Rayleigh scattering depolarization measurements,” Chem. Phys. Lett. 286, 101–106 (1998).
[CrossRef]

Wong, K. Y.

T. W. Chui and K. Y. Wong, “Study of hyper-Rayleigh scat-tering and two-photon absorption induced fluorescence from crystal violet,” J. Chem. Phys. 109, 1391–1396 (1998).
[CrossRef]

Chem. Phys. Lett. (1)

C. Boutton, K. Clays, A. Persoons, T. Wada, and H. Sasabe, “Second-order off-diagonal hyperpolarizability tensor components of substituted carbazoles by hyper-Rayleigh scattering depolarization measurements,” Chem. Phys. Lett. 286, 101–106 (1998).
[CrossRef]

Ferroelectrics (2)

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin lead-zirconate-titanate ferroelectrics films,” Ferroelectrics 183, 215–218 (1996).
[CrossRef]

O. A. Aktsipetrov, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, E. D. Mishina, A. S. Sigov, K. A. Vorotilov, M. A. C. Devillers, and Th. Rasing, “Optical second harmonic generation studies of thin ferroelectrics films,” Ferroelectrics 190, 143–148 (1997).
[CrossRef]

J. Chem. Phys. (1)

T. W. Chui and K. Y. Wong, “Study of hyper-Rayleigh scat-tering and two-photon absorption induced fluorescence from crystal violet,” J. Chem. Phys. 109, 1391–1396 (1998).
[CrossRef]

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

Phys. Rev. (1)

N. Bloembergen, R. K. Chang, S. S. Jha, and C. H. Lee, “Optical second harmonic generation in reflection from media with inversion symmetry,” Phys. Rev. 174, 813–822 (1968).
[CrossRef]

Phys. Rev. A (1)

P. D. Maker, “Spectral broadening of elastic second-harmonic light scattering in liquids,” Phys. Rev. A 1, 923–951 (1970).
[CrossRef]

Phys. Rev. B (1)

A. M. Tishin, Yu. A. Koksharov, J. Bohr, and G. B. Khomutov, “Evidence for magnetic ordering in ultrathin gadolinium Langmuir–Blodgett films,” Phys. Rev. B 55, 11064–11067 (1997).
[CrossRef]

Phys. Rev. Lett. (1)

R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurements of nonlinear light scattering,” Phys. Rev. Lett. 14, 681–684 (1965).
[CrossRef]

Sov. Phys. JETP (1)

O. A. Aktsipetrov, I. M. Baranova, and Yu. A. Il’inskii, “Surface contribution to the generation of reflected second harmonic for centrosymmetric semiconductors,” Zh. Eksp. Teor. Fiz. 91, 287–296 (1986) [ Sov. Phys. JETP 64, 167–172 (1986)].

Surf. Sci. (1)

E. D. Mishina, A. A. Fedyanin, D. A. Klimkin, A. A. Nikulin, O. A. Aktsipetrov, S. L. Vorob’eva, V. R. Novak, M. A. C. Devillers, and Th. Rasing, “Second harmonic generation and hyper-Rayleigh scattering in Langmuir–Blodgett films of fullerenes,” Surf. Sci. 382, L696–699 (1997).
[CrossRef]

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S. Kielich, Molecular Nonlinear Optics (Mir, Moscow, 1974; in Russian).

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Figures (4)

Fig. 1
Fig. 1

Two-stage formation of the structural unit of the organometallic superstructure during a, immersion and b, withdrawal of the substrate.

Fig. 2
Fig. 2

SH intensity as a function of the fundamental wavelength. Inset, differential spectrum of the linear-optical absorption in the film with a pure stearic acid multilayer as a reference.

Fig. 3
Fig. 3

Filled circles, HRS indicatrix for s-in, s-out at λω=740 nm and θ0=-22.5° (incidence and scattering angles θ0 and θ are measured from the direction of the normal to the film, with the choice of sign fixed by the condition θ0<0). Solid curve, dependence given by relation (3) and Eq. (4) with β/α=b/a=-0.74, L=0.53λω, 2ω=1.93. Inset, thickness dependence of the HRS signal at θ=22.5° (specular direction). The curves in the inset are theoretical curves according to Eq. (5): 1, n=1, K0=0.11, Ka2=185.73, bQ/a=-0.74, bD/a=0.00, 2ω=1.93; 2, n=2, K0=0.24, Ka2=6.24, bQ/a=-0.73, bD/a=-0.01, 2ω=1.93.

Fig. 4
Fig. 4

Filled circles, HRS wave polarization diagram measured for s-polarized fundamental radiation at λω=740 nm and θ0=-45°. The analyzer rotation angles of 0° (180°) and 90° (270°) correspond to s and p polarization, respectively. Solid curve, dependence given by Eq. (6) at φ0=0° and δ=3.62.

Equations (18)

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P2ω(R)=P2ωD(R)-·Q2ω(R),
A*(R)B(R)=A*(r, z)B(r, z)=C˜(A, B)F(|r-r|, z, z)×exp[2iq(r-r)],
I2ωs,s(θ)|a+b(2ω-sin2 θ)1/2|2f[2ω(sin θ
-sin θ0)/c],
a=1f(0)0ddz0ddz-drta:[P2ωD(0)]*P2ωD(r)1/2=[ta:C(P2ωD, P2ωD)]1/2,
bD=2ωc1f(0)0d dz 0d dz×- drzztb:[P2ωD(0)]*P2ωD(r)1/22ωdc[tb:C(P2ωD, P2ωD)]1/2,
bQ=2ωc1f(0)0d dz 0d dz×-drtb:zˆzˆ:[Q2ω(0)]*Q2ω(r)1/2=2ωc{tb:[zˆzˆ:C˜(Q2ω, Q2ω)]}1/2,
f(k)=C exp[-(kL)2],
I2ω(NGd)=K0+KNGdna+bQ+bD NGdN0×(2ω-sin2 θ0)1/22,
I2ω(φ)=Imax{1+δ+(δ-1)cos[2(φ-φ0)]}/(2δ),
ξ1=(δ-1)sin 2φ0/(δ+1),
ξ3=(δ-1)cos 2φ0/(δ+1),
l=ξ12+ξ32=(δ-1)/(δ+1).
δ=τ2ω(θ0)yy(0)cos2 θ0xx(0)+sin2 θ0zz(0)+2 sin θ0 cos θ0xz(0),
θ0=arcsinsin θ02ω,
τ2ω(θ0)=cos θ0+2ω cos θ02ω cos θ0+cos θ02,
jj(k)=0d dz 0ddz - drP2ω,j*(r, z)P2ω,j(0, z)×exp(-ikr).
ΔQΔDδ(1+cos 2θ0)-2τ2ω(θ0)2δ sin 2θ0,

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