Abstract

Results of picosecond Raman scattering of the excited state of Rhodamine 560 are reported. Both two-and three-color transient spectroscopy are accomplished with a time resolution of ~10 psec. The method was coherent anti-Stokes Raman probing of the excited states with the Stokes field from a broadband synchronously pumped dye laser. The anti-Stokes signal is detected by using a multichannel spectrometer system.

© 1986 Optical Society of America

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  1. J. Terner, J. D. Strong, T. Spiro, M. Nagumo, M. Nicol, M. A. El-Sayed, Proc. Natl. Acad. Sci. U.S.A. 78, 1313 (1981).
    [CrossRef] [PubMed]
  2. T. L. Gustafson, D. M. Roberts, D. A. Chernoff, J. Chem. Phys. 79, 1559 (1983).
    [CrossRef]
  3. L. S. Goldberg, in Picosecond Phenomena III, K. B. Eisenthal, R. M. Hochstrasser, W. Kaiser, L. Laubereau, eds. (Springer-Verlag, Berlin, 1982), p. 94.
    [CrossRef]
  4. W. Werncke, H.-J. Weigmann, J. Paetzold, A. Lau, K. Lenz, M. Pfeiffer, Chem. Phys. Lett. 61, 105 (1979); H.-J. Weigmann, K. Lenz, A. Lau, M. Pfeiffer, W. Werncke, Chem. Phys. Lett. 73, 175 (1980); T. Kamisuki, I. Moriyama, R. Igarashi, Y. Adachi, S. Maeda, J. Chem. Phys. 73, 3500 (1980); S. Maeda, H. Kataoka, T. Kamisuki, Y. Adachi, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983); A. Lau, H.-J. Weigmann, W. Werncke, K. Lenz, M. Pfeiffer, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983).
    [CrossRef]
  5. G. Dolan, C. R. Goldschmidt, Chem. Phys. Lett. 39, 320 (1976).
    [CrossRef]
  6. S. A. Payne, R. M. Hochstrasser (submitted to J. Phys. Chem.).
  7. E. J. Heilweil, F. E. Doany, R. Moore, R. M. Hochstrasser, J. Chem. Phys. 76, 5632 (1982); F. Doany, E. J. Heilweil, R. J. Moore, R. M. Hochstrasser, J. Chem. Phys. 80, 201 (1984).
    [CrossRef]
  8. M. A. Yuratich, Mol. Phys. 38, 625 (1979).
    [CrossRef]
  9. J. P. Devlin, M. G. Rockley, Chem. Phys. Lett. 56, 608 (1978); R. Konig, A. Lau, H.-J. Weigmann, Chem. Phys. Lett. 69, 87 (1980).
    [CrossRef]

1983

T. L. Gustafson, D. M. Roberts, D. A. Chernoff, J. Chem. Phys. 79, 1559 (1983).
[CrossRef]

1982

E. J. Heilweil, F. E. Doany, R. Moore, R. M. Hochstrasser, J. Chem. Phys. 76, 5632 (1982); F. Doany, E. J. Heilweil, R. J. Moore, R. M. Hochstrasser, J. Chem. Phys. 80, 201 (1984).
[CrossRef]

1981

J. Terner, J. D. Strong, T. Spiro, M. Nagumo, M. Nicol, M. A. El-Sayed, Proc. Natl. Acad. Sci. U.S.A. 78, 1313 (1981).
[CrossRef] [PubMed]

1979

M. A. Yuratich, Mol. Phys. 38, 625 (1979).
[CrossRef]

W. Werncke, H.-J. Weigmann, J. Paetzold, A. Lau, K. Lenz, M. Pfeiffer, Chem. Phys. Lett. 61, 105 (1979); H.-J. Weigmann, K. Lenz, A. Lau, M. Pfeiffer, W. Werncke, Chem. Phys. Lett. 73, 175 (1980); T. Kamisuki, I. Moriyama, R. Igarashi, Y. Adachi, S. Maeda, J. Chem. Phys. 73, 3500 (1980); S. Maeda, H. Kataoka, T. Kamisuki, Y. Adachi, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983); A. Lau, H.-J. Weigmann, W. Werncke, K. Lenz, M. Pfeiffer, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983).
[CrossRef]

1978

J. P. Devlin, M. G. Rockley, Chem. Phys. Lett. 56, 608 (1978); R. Konig, A. Lau, H.-J. Weigmann, Chem. Phys. Lett. 69, 87 (1980).
[CrossRef]

1976

G. Dolan, C. R. Goldschmidt, Chem. Phys. Lett. 39, 320 (1976).
[CrossRef]

Chernoff, D. A.

T. L. Gustafson, D. M. Roberts, D. A. Chernoff, J. Chem. Phys. 79, 1559 (1983).
[CrossRef]

Devlin, J. P.

J. P. Devlin, M. G. Rockley, Chem. Phys. Lett. 56, 608 (1978); R. Konig, A. Lau, H.-J. Weigmann, Chem. Phys. Lett. 69, 87 (1980).
[CrossRef]

Doany, F. E.

E. J. Heilweil, F. E. Doany, R. Moore, R. M. Hochstrasser, J. Chem. Phys. 76, 5632 (1982); F. Doany, E. J. Heilweil, R. J. Moore, R. M. Hochstrasser, J. Chem. Phys. 80, 201 (1984).
[CrossRef]

Dolan, G.

G. Dolan, C. R. Goldschmidt, Chem. Phys. Lett. 39, 320 (1976).
[CrossRef]

El-Sayed, M. A.

J. Terner, J. D. Strong, T. Spiro, M. Nagumo, M. Nicol, M. A. El-Sayed, Proc. Natl. Acad. Sci. U.S.A. 78, 1313 (1981).
[CrossRef] [PubMed]

Goldberg, L. S.

L. S. Goldberg, in Picosecond Phenomena III, K. B. Eisenthal, R. M. Hochstrasser, W. Kaiser, L. Laubereau, eds. (Springer-Verlag, Berlin, 1982), p. 94.
[CrossRef]

Goldschmidt, C. R.

G. Dolan, C. R. Goldschmidt, Chem. Phys. Lett. 39, 320 (1976).
[CrossRef]

Gustafson, T. L.

T. L. Gustafson, D. M. Roberts, D. A. Chernoff, J. Chem. Phys. 79, 1559 (1983).
[CrossRef]

Heilweil, E. J.

E. J. Heilweil, F. E. Doany, R. Moore, R. M. Hochstrasser, J. Chem. Phys. 76, 5632 (1982); F. Doany, E. J. Heilweil, R. J. Moore, R. M. Hochstrasser, J. Chem. Phys. 80, 201 (1984).
[CrossRef]

Hochstrasser, R. M.

E. J. Heilweil, F. E. Doany, R. Moore, R. M. Hochstrasser, J. Chem. Phys. 76, 5632 (1982); F. Doany, E. J. Heilweil, R. J. Moore, R. M. Hochstrasser, J. Chem. Phys. 80, 201 (1984).
[CrossRef]

S. A. Payne, R. M. Hochstrasser (submitted to J. Phys. Chem.).

Lau, A.

W. Werncke, H.-J. Weigmann, J. Paetzold, A. Lau, K. Lenz, M. Pfeiffer, Chem. Phys. Lett. 61, 105 (1979); H.-J. Weigmann, K. Lenz, A. Lau, M. Pfeiffer, W. Werncke, Chem. Phys. Lett. 73, 175 (1980); T. Kamisuki, I. Moriyama, R. Igarashi, Y. Adachi, S. Maeda, J. Chem. Phys. 73, 3500 (1980); S. Maeda, H. Kataoka, T. Kamisuki, Y. Adachi, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983); A. Lau, H.-J. Weigmann, W. Werncke, K. Lenz, M. Pfeiffer, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983).
[CrossRef]

Lenz, K.

W. Werncke, H.-J. Weigmann, J. Paetzold, A. Lau, K. Lenz, M. Pfeiffer, Chem. Phys. Lett. 61, 105 (1979); H.-J. Weigmann, K. Lenz, A. Lau, M. Pfeiffer, W. Werncke, Chem. Phys. Lett. 73, 175 (1980); T. Kamisuki, I. Moriyama, R. Igarashi, Y. Adachi, S. Maeda, J. Chem. Phys. 73, 3500 (1980); S. Maeda, H. Kataoka, T. Kamisuki, Y. Adachi, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983); A. Lau, H.-J. Weigmann, W. Werncke, K. Lenz, M. Pfeiffer, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983).
[CrossRef]

Moore, R.

E. J. Heilweil, F. E. Doany, R. Moore, R. M. Hochstrasser, J. Chem. Phys. 76, 5632 (1982); F. Doany, E. J. Heilweil, R. J. Moore, R. M. Hochstrasser, J. Chem. Phys. 80, 201 (1984).
[CrossRef]

Nagumo, M.

J. Terner, J. D. Strong, T. Spiro, M. Nagumo, M. Nicol, M. A. El-Sayed, Proc. Natl. Acad. Sci. U.S.A. 78, 1313 (1981).
[CrossRef] [PubMed]

Nicol, M.

J. Terner, J. D. Strong, T. Spiro, M. Nagumo, M. Nicol, M. A. El-Sayed, Proc. Natl. Acad. Sci. U.S.A. 78, 1313 (1981).
[CrossRef] [PubMed]

Paetzold, J.

W. Werncke, H.-J. Weigmann, J. Paetzold, A. Lau, K. Lenz, M. Pfeiffer, Chem. Phys. Lett. 61, 105 (1979); H.-J. Weigmann, K. Lenz, A. Lau, M. Pfeiffer, W. Werncke, Chem. Phys. Lett. 73, 175 (1980); T. Kamisuki, I. Moriyama, R. Igarashi, Y. Adachi, S. Maeda, J. Chem. Phys. 73, 3500 (1980); S. Maeda, H. Kataoka, T. Kamisuki, Y. Adachi, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983); A. Lau, H.-J. Weigmann, W. Werncke, K. Lenz, M. Pfeiffer, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983).
[CrossRef]

Payne, S. A.

S. A. Payne, R. M. Hochstrasser (submitted to J. Phys. Chem.).

Pfeiffer, M.

W. Werncke, H.-J. Weigmann, J. Paetzold, A. Lau, K. Lenz, M. Pfeiffer, Chem. Phys. Lett. 61, 105 (1979); H.-J. Weigmann, K. Lenz, A. Lau, M. Pfeiffer, W. Werncke, Chem. Phys. Lett. 73, 175 (1980); T. Kamisuki, I. Moriyama, R. Igarashi, Y. Adachi, S. Maeda, J. Chem. Phys. 73, 3500 (1980); S. Maeda, H. Kataoka, T. Kamisuki, Y. Adachi, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983); A. Lau, H.-J. Weigmann, W. Werncke, K. Lenz, M. Pfeiffer, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983).
[CrossRef]

Roberts, D. M.

T. L. Gustafson, D. M. Roberts, D. A. Chernoff, J. Chem. Phys. 79, 1559 (1983).
[CrossRef]

Rockley, M. G.

J. P. Devlin, M. G. Rockley, Chem. Phys. Lett. 56, 608 (1978); R. Konig, A. Lau, H.-J. Weigmann, Chem. Phys. Lett. 69, 87 (1980).
[CrossRef]

Spiro, T.

J. Terner, J. D. Strong, T. Spiro, M. Nagumo, M. Nicol, M. A. El-Sayed, Proc. Natl. Acad. Sci. U.S.A. 78, 1313 (1981).
[CrossRef] [PubMed]

Strong, J. D.

J. Terner, J. D. Strong, T. Spiro, M. Nagumo, M. Nicol, M. A. El-Sayed, Proc. Natl. Acad. Sci. U.S.A. 78, 1313 (1981).
[CrossRef] [PubMed]

Terner, J.

J. Terner, J. D. Strong, T. Spiro, M. Nagumo, M. Nicol, M. A. El-Sayed, Proc. Natl. Acad. Sci. U.S.A. 78, 1313 (1981).
[CrossRef] [PubMed]

Weigmann, H.-J.

W. Werncke, H.-J. Weigmann, J. Paetzold, A. Lau, K. Lenz, M. Pfeiffer, Chem. Phys. Lett. 61, 105 (1979); H.-J. Weigmann, K. Lenz, A. Lau, M. Pfeiffer, W. Werncke, Chem. Phys. Lett. 73, 175 (1980); T. Kamisuki, I. Moriyama, R. Igarashi, Y. Adachi, S. Maeda, J. Chem. Phys. 73, 3500 (1980); S. Maeda, H. Kataoka, T. Kamisuki, Y. Adachi, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983); A. Lau, H.-J. Weigmann, W. Werncke, K. Lenz, M. Pfeiffer, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983).
[CrossRef]

Werncke, W.

W. Werncke, H.-J. Weigmann, J. Paetzold, A. Lau, K. Lenz, M. Pfeiffer, Chem. Phys. Lett. 61, 105 (1979); H.-J. Weigmann, K. Lenz, A. Lau, M. Pfeiffer, W. Werncke, Chem. Phys. Lett. 73, 175 (1980); T. Kamisuki, I. Moriyama, R. Igarashi, Y. Adachi, S. Maeda, J. Chem. Phys. 73, 3500 (1980); S. Maeda, H. Kataoka, T. Kamisuki, Y. Adachi, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983); A. Lau, H.-J. Weigmann, W. Werncke, K. Lenz, M. Pfeiffer, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983).
[CrossRef]

Yuratich, M. A.

M. A. Yuratich, Mol. Phys. 38, 625 (1979).
[CrossRef]

Chem. Phys. Lett.

W. Werncke, H.-J. Weigmann, J. Paetzold, A. Lau, K. Lenz, M. Pfeiffer, Chem. Phys. Lett. 61, 105 (1979); H.-J. Weigmann, K. Lenz, A. Lau, M. Pfeiffer, W. Werncke, Chem. Phys. Lett. 73, 175 (1980); T. Kamisuki, I. Moriyama, R. Igarashi, Y. Adachi, S. Maeda, J. Chem. Phys. 73, 3500 (1980); S. Maeda, H. Kataoka, T. Kamisuki, Y. Adachi, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983); A. Lau, H.-J. Weigmann, W. Werncke, K. Lenz, M. Pfeiffer, in Time-Resolved Vibrational SpectroscopyG. H. Atkinson, ed. (Academic, New York, 1983).
[CrossRef]

G. Dolan, C. R. Goldschmidt, Chem. Phys. Lett. 39, 320 (1976).
[CrossRef]

J. P. Devlin, M. G. Rockley, Chem. Phys. Lett. 56, 608 (1978); R. Konig, A. Lau, H.-J. Weigmann, Chem. Phys. Lett. 69, 87 (1980).
[CrossRef]

J. Chem. Phys.

E. J. Heilweil, F. E. Doany, R. Moore, R. M. Hochstrasser, J. Chem. Phys. 76, 5632 (1982); F. Doany, E. J. Heilweil, R. J. Moore, R. M. Hochstrasser, J. Chem. Phys. 80, 201 (1984).
[CrossRef]

T. L. Gustafson, D. M. Roberts, D. A. Chernoff, J. Chem. Phys. 79, 1559 (1983).
[CrossRef]

Mol. Phys.

M. A. Yuratich, Mol. Phys. 38, 625 (1979).
[CrossRef]

Proc. Natl. Acad. Sci. U.S.A.

J. Terner, J. D. Strong, T. Spiro, M. Nagumo, M. Nicol, M. A. El-Sayed, Proc. Natl. Acad. Sci. U.S.A. 78, 1313 (1981).
[CrossRef] [PubMed]

Other

L. S. Goldberg, in Picosecond Phenomena III, K. B. Eisenthal, R. M. Hochstrasser, W. Kaiser, L. Laubereau, eds. (Springer-Verlag, Berlin, 1982), p. 94.
[CrossRef]

S. A. Payne, R. M. Hochstrasser (submitted to J. Phys. Chem.).

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Figures (3)

Fig. 1
Fig. 1

Explanation of two- and three-color transient CARS experiments of a condensed-phase molecule.

Fig. 2
Fig. 2

Three-color excited- and ground-state CARS spectra of R560 in ethanol. (Concentration is 0.8 mM; 190-μm solution path length; each spectrum consists of 80 laser shots. The peak of the unpumped spectrum corresponds to 180 counts.)

Fig. 3
Fig. 3

Dependence of two-color CARS spectra on ω1 intensity for R560 in ethanol. [0.10 × (ω1 intensity), the low-intensity spectrum, is due to the ground state only. At full ω1 intensity the spectrum in the lower frame was obtained. The difference spectrum was obtained by subtracting out the ethanol nonresonant background shown. The increase in the 1197-cm−1 line is due to excited-state Raman scattering. Concentration is 4 mM; 190-μm cell path length; each spectrum consists of 80 laser shots. The peak counts of the low- and full-intensity spectra in the upper frame are 330 and 6500.]

Tables (1)

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Table 1 Parameters of Laser Beams

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