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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  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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