Abstract

We have used a high-intensity tunable picosecond infrared laser source to measure the spectral content of light scattered near the second harmonic for two well-known organic dyes, p-Nitroaniline and Disperse Red 1, at a number of wavelengths in the near infrared. We found that in Disperse red 1 a broad two-photon fluorescence competes with the sharp hyper-Rayleigh peak. Further, dephasing of the virtual excited state leads to elimination of hyper-Rayleigh scattering in favor of fluorescence if the harmonic is in the linear absorption tail. We determined the dispersion of the magnitude of the first hyperpolarizability for both dyes, using a simple referencing technique, and found it to be consistent with that of a two-level dispersion model.

© 1996 Optical Society of America

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References

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  1. K. D. Singer, J. E. Sohn, L. A. King, H. M. Gordon, H. E. Katz, C. W. Dirk, J. Opt. Soc. Am. B 6, 1339 (1989).
    [CrossRef]
  2. R. W. Terhune, P. D. Maker, C. M. Savage, Phys. Rev. Lett. 14, 681 (1965).
    [CrossRef]
  3. K. Clays, A. Persoons, Phys. Rev. Lett. 66, 2980 (1991).
    [CrossRef] [PubMed]
  4. Z. Zyss, Nonlinear Opt. 1, 3 (1991).
  5. T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. Persoons, J. Am. Chem. Soc. 116, 9320 (1994).
    [CrossRef]
  6. W. M. McClain, J. Chem. Phys. 67, 5026 (1972).
  7. M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
    [CrossRef]
  8. J. Zyss, I. Ledoux, Chem. Rev. 94, 473 (1994).
    [CrossRef]
  9. J. D. V. Khaydarov, J. H. Andrews, K. D. Singer, J. Opt. Soc. Sci. Am. B 12, 2199 (1991).
    [CrossRef]
  10. G. J. T. Heesink, A. G. T. Ruiter, N. F. Van Hulst, B. Bölger, Phys. Rev. Lett. 71, 999 (1993).
    [CrossRef] [PubMed]
  11. M. Joffre, D. Yaron, R. Silbey, J. Zyss, J. Chem. Phys. 97, 5607 (1992).
    [CrossRef]
  12. S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford U. Press, Oxford, 1995), Chap. 7–9.
  13. S. Stadler, R. Deitrich, G. Bourhill, Ch. Bräuchle, Opt. Lett. 21, 251 (1995).
    [CrossRef]

1995 (2)

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

S. Stadler, R. Deitrich, G. Bourhill, Ch. Bräuchle, Opt. Lett. 21, 251 (1995).
[CrossRef]

1994 (2)

J. Zyss, I. Ledoux, Chem. Rev. 94, 473 (1994).
[CrossRef]

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. Persoons, J. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

1993 (1)

G. J. T. Heesink, A. G. T. Ruiter, N. F. Van Hulst, B. Bölger, Phys. Rev. Lett. 71, 999 (1993).
[CrossRef] [PubMed]

1992 (1)

M. Joffre, D. Yaron, R. Silbey, J. Zyss, J. Chem. Phys. 97, 5607 (1992).
[CrossRef]

1991 (3)

J. D. V. Khaydarov, J. H. Andrews, K. D. Singer, J. Opt. Soc. Sci. Am. B 12, 2199 (1991).
[CrossRef]

K. Clays, A. Persoons, Phys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

Z. Zyss, Nonlinear Opt. 1, 3 (1991).

1989 (1)

1972 (1)

W. M. McClain, J. Chem. Phys. 67, 5026 (1972).

1965 (1)

R. W. Terhune, P. D. Maker, C. M. Savage, Phys. Rev. Lett. 14, 681 (1965).
[CrossRef]

Andrews, J. H.

J. D. V. Khaydarov, J. H. Andrews, K. D. Singer, J. Opt. Soc. Sci. Am. B 12, 2199 (1991).
[CrossRef]

Bölger, B.

G. J. T. Heesink, A. G. T. Ruiter, N. F. Van Hulst, B. Bölger, Phys. Rev. Lett. 71, 999 (1993).
[CrossRef] [PubMed]

Bourhill, G.

Bräuchle, Ch.

Clays, K.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. Persoons, J. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

K. Clays, A. Persoons, Phys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

de Jonge, R.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Deitrich, R.

Dirk, C. W.

Flipse, M. C.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Gordon, H. M.

Heesink, G. J. T.

G. J. T. Heesink, A. G. T. Ruiter, N. F. Van Hulst, B. Bölger, Phys. Rev. Lett. 71, 999 (1993).
[CrossRef] [PubMed]

Jenneskens, L. W.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Joffre, M.

M. Joffre, D. Yaron, R. Silbey, J. Zyss, J. Chem. Phys. 97, 5607 (1992).
[CrossRef]

Katz, H. E.

Khaydarov, J. D. V.

J. D. V. Khaydarov, J. H. Andrews, K. D. Singer, J. Opt. Soc. Sci. Am. B 12, 2199 (1991).
[CrossRef]

King, L. A.

Ledoux, I.

J. Zyss, I. Ledoux, Chem. Rev. 94, 473 (1994).
[CrossRef]

Maker, P. D.

R. W. Terhune, P. D. Maker, C. M. Savage, Phys. Rev. Lett. 14, 681 (1965).
[CrossRef]

Marsman, A. W.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

McClain, W. M.

W. M. McClain, J. Chem. Phys. 67, 5026 (1972).

Mukamel, S.

S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford U. Press, Oxford, 1995), Chap. 7–9.

Persoons, A.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. Persoons, J. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

K. Clays, A. Persoons, Phys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

Reinhoudt, D.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. Persoons, J. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

Ruiter, A. G. T.

G. J. T. Heesink, A. G. T. Ruiter, N. F. Van Hulst, B. Bölger, Phys. Rev. Lett. 71, 999 (1993).
[CrossRef] [PubMed]

Samyn, C.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. Persoons, J. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

Savage, C. M.

R. W. Terhune, P. D. Maker, C. M. Savage, Phys. Rev. Lett. 14, 681 (1965).
[CrossRef]

Silbey, R.

M. Joffre, D. Yaron, R. Silbey, J. Zyss, J. Chem. Phys. 97, 5607 (1992).
[CrossRef]

Singer, K. D.

J. D. V. Khaydarov, J. H. Andrews, K. D. Singer, J. Opt. Soc. Sci. Am. B 12, 2199 (1991).
[CrossRef]

K. D. Singer, J. E. Sohn, L. A. King, H. M. Gordon, H. E. Katz, C. W. Dirk, J. Opt. Soc. Am. B 6, 1339 (1989).
[CrossRef]

Sohn, J. E.

Stadler, S.

Terhune, R. W.

R. W. Terhune, P. D. Maker, C. M. Savage, Phys. Rev. Lett. 14, 681 (1965).
[CrossRef]

Van Hulst, N. F.

G. J. T. Heesink, A. G. T. Ruiter, N. F. Van Hulst, B. Bölger, Phys. Rev. Lett. 71, 999 (1993).
[CrossRef] [PubMed]

van Walree, C. A.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Verbiest, T.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. Persoons, J. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

Wolff, J.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. Persoons, J. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

Woudenberg, R. H.

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Yaron, D.

M. Joffre, D. Yaron, R. Silbey, J. Zyss, J. Chem. Phys. 97, 5607 (1992).
[CrossRef]

Zyss, J.

J. Zyss, I. Ledoux, Chem. Rev. 94, 473 (1994).
[CrossRef]

M. Joffre, D. Yaron, R. Silbey, J. Zyss, J. Chem. Phys. 97, 5607 (1992).
[CrossRef]

Zyss, Z.

Z. Zyss, Nonlinear Opt. 1, 3 (1991).

Chem. Phys. Lett. (1)

M. C. Flipse, R. de Jonge, R. H. Woudenberg, A. W. Marsman, C. A. van Walree, L. W. Jenneskens, Chem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Chem. Rev. (1)

J. Zyss, I. Ledoux, Chem. Rev. 94, 473 (1994).
[CrossRef]

J. Am. Chem. Soc. (1)

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. Persoons, J. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

J. Chem. Phys. (2)

W. M. McClain, J. Chem. Phys. 67, 5026 (1972).

M. Joffre, D. Yaron, R. Silbey, J. Zyss, J. Chem. Phys. 97, 5607 (1992).
[CrossRef]

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

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

J. D. V. Khaydarov, J. H. Andrews, K. D. Singer, J. Opt. Soc. Sci. Am. B 12, 2199 (1991).
[CrossRef]

Nonlinear Opt. (1)

Z. Zyss, Nonlinear Opt. 1, 3 (1991).

Opt. Lett. (1)

Phys. Rev. Lett. (3)

G. J. T. Heesink, A. G. T. Ruiter, N. F. Van Hulst, B. Bölger, Phys. Rev. Lett. 71, 999 (1993).
[CrossRef] [PubMed]

R. W. Terhune, P. D. Maker, C. M. Savage, Phys. Rev. Lett. 14, 681 (1965).
[CrossRef]

K. Clays, A. Persoons, Phys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

Other (1)

S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford U. Press, Oxford, 1995), Chap. 7–9.

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Figures (3)

Fig. 1
Fig. 1

Hyperpolarizability as a function of wavelength for pNA dissolved in acetone. The filled circles correspond to measured values, and the curve is a fit to a two-level dispersive model. The inset shows the spectra of light scattered near the harmonic for the indicated pump wavelengths.

Fig. 2
Fig. 2

UV–visible absorption spectrum and spectra of radiation emitted near the harmonic from concentrated solutions of DR1 in acetone for pumping at the indicated wavelengths. The solid curve is the UV–visible absorption spectrum. The inset shows UV–visible absorption of a less-concentrated solution over a broad spectral range.

Fig. 3
Fig. 3

Measured and deduced hyperpolarizabilities of DR1 dissolved in acetone. The filled circles are calculated from dilute concentration-dependent measurements, corrected for linear absorption of the harmonic, and include a subtraction of minor two-photon fluorescence (TPF) as background. The hollow points are deduced from spectra produced by concentrated solutions with narrow-band (HRS) or broadband (HRS + TPF) content as indicated. The curve is a prediction based on a two-level model using the maximum of the linear polarizability and an average static hyperpolarizability deduced from concentration-dependent data.

Equations (5)

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I 2 ω = G ( N solvent β solvent 2 + N dye β dye 2 ) 10 ( I ω ) 2 ,
I 2 ω I 2 ω = 3 + 11 u 2 2 u 15 + 27 u 2 + 18 u ,
ρ = 1 3 1 3 u 1 + u .
m R = β dye 2 β reference 2 ,
( m R ) β ref , J 2 = β dye , J 2 ,

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