Abstract

With the method of self-diffraction of incoherent light, molecular vibrations were observed in real time in various dye molecules pumped near the absorption edge. In Rhodamine 560, 35-fsec oscillations in the signal were measured, which corresponds to a vibrational frequency of 1000 cm−1. Simultaneously, this technique can be used to deduce the ultrafast dephasing times in the molecular vibrational quasi-continuum. Dephasing times of 20 and 150 fsec were observed in Rhodamine 590 and Rhodamine 560, respectively.

© 1990 Optical Society of America

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References

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  1. M. J. Rosker, F. W. Wise, C. L. Tang, Phys. Rev. Lett. 57, 321 (1986).
    [CrossRef] [PubMed]
  2. J. M. Y. Ha, H. J. Maris, W. M. Risen, J. Tauc, Phys. Rev. Lett. 57, 3302 (1986).
    [CrossRef] [PubMed]
  3. C. Hayden, R. Trevino, Lawrence Livermore Laboratory, Livermore, California 94550 (personal communication).
  4. S. Ruhman, A. G. Joly, K. Nelson, IEEE J. Quantum Electron. 24, 460 (1988).
    [CrossRef]
  5. M. A. Dugan, J. S. Melinger, A. C. Albrecht, Chem. Phys. Lett. 147, 411(1988).
    [CrossRef]
  6. P. C. Becker, H. L. Fragnito, J. Y. Bigot, C. H. Brito Cruz, R. L. Fork, C. V. Shank, Phys. Rev. Lett. 63, 505 (1989).
    [CrossRef] [PubMed]
  7. N. Morita, T. Yajima, Phys. Rev. A 30, 2525 (1984).
    [CrossRef]
  8. H. Kalt, R. Renner, C. Klingshirn, IEEE J. Quantum Electron. QE-22, 1312 (1986).
    [CrossRef]
  9. M. Fujiwara, R. Kuroda, H. Nakatsuka, J. Opt. Soc. Am. B 2, 1634 (1985).
    [CrossRef]
  10. D. DeBeer, E. Usadi, S. R. Hartmann, Phys. Rev. Lett. 60, 1262 (1988).
    [CrossRef] [PubMed]
  11. A. M. Weiner, S. DeSilvesti, E. P. Ippen, J. Opt. Soc. Am. B 2, 654 (1985).
    [CrossRef]
  12. Y. J. Xie, Ph.D. dissertation (State University of New York at Buffalo, Amherst, N.Y., 1989).
  13. J. Z. Zhang, E. Heller, D. Huber, D. G. Imre, D. Tannor, J. Chem. Phys. 89, 3602 (1988).
    [CrossRef]
  14. G. Herzberg, Electronic Spectra of Polyatomic Molecules (Van Nostrand Reinhold, New York, 1966).
  15. P. M. Felker, G. V. Hartland, Chem. Phys. Lett. 134, 503 (1987).
    [CrossRef]
  16. M. Dantus, M. J. Rosker, A. H. Zewail, J. Chem. Phys. 89, 6128 (1988).
    [CrossRef]

1989 (1)

P. C. Becker, H. L. Fragnito, J. Y. Bigot, C. H. Brito Cruz, R. L. Fork, C. V. Shank, Phys. Rev. Lett. 63, 505 (1989).
[CrossRef] [PubMed]

1988 (5)

D. DeBeer, E. Usadi, S. R. Hartmann, Phys. Rev. Lett. 60, 1262 (1988).
[CrossRef] [PubMed]

J. Z. Zhang, E. Heller, D. Huber, D. G. Imre, D. Tannor, J. Chem. Phys. 89, 3602 (1988).
[CrossRef]

S. Ruhman, A. G. Joly, K. Nelson, IEEE J. Quantum Electron. 24, 460 (1988).
[CrossRef]

M. A. Dugan, J. S. Melinger, A. C. Albrecht, Chem. Phys. Lett. 147, 411(1988).
[CrossRef]

M. Dantus, M. J. Rosker, A. H. Zewail, J. Chem. Phys. 89, 6128 (1988).
[CrossRef]

1987 (1)

P. M. Felker, G. V. Hartland, Chem. Phys. Lett. 134, 503 (1987).
[CrossRef]

1986 (3)

M. J. Rosker, F. W. Wise, C. L. Tang, Phys. Rev. Lett. 57, 321 (1986).
[CrossRef] [PubMed]

J. M. Y. Ha, H. J. Maris, W. M. Risen, J. Tauc, Phys. Rev. Lett. 57, 3302 (1986).
[CrossRef] [PubMed]

H. Kalt, R. Renner, C. Klingshirn, IEEE J. Quantum Electron. QE-22, 1312 (1986).
[CrossRef]

1985 (2)

1984 (1)

N. Morita, T. Yajima, Phys. Rev. A 30, 2525 (1984).
[CrossRef]

Albrecht, A. C.

M. A. Dugan, J. S. Melinger, A. C. Albrecht, Chem. Phys. Lett. 147, 411(1988).
[CrossRef]

Becker, P. C.

P. C. Becker, H. L. Fragnito, J. Y. Bigot, C. H. Brito Cruz, R. L. Fork, C. V. Shank, Phys. Rev. Lett. 63, 505 (1989).
[CrossRef] [PubMed]

Bigot, J. Y.

P. C. Becker, H. L. Fragnito, J. Y. Bigot, C. H. Brito Cruz, R. L. Fork, C. V. Shank, Phys. Rev. Lett. 63, 505 (1989).
[CrossRef] [PubMed]

Brito Cruz, C. H.

P. C. Becker, H. L. Fragnito, J. Y. Bigot, C. H. Brito Cruz, R. L. Fork, C. V. Shank, Phys. Rev. Lett. 63, 505 (1989).
[CrossRef] [PubMed]

Dantus, M.

M. Dantus, M. J. Rosker, A. H. Zewail, J. Chem. Phys. 89, 6128 (1988).
[CrossRef]

DeBeer, D.

D. DeBeer, E. Usadi, S. R. Hartmann, Phys. Rev. Lett. 60, 1262 (1988).
[CrossRef] [PubMed]

DeSilvesti, S.

Dugan, M. A.

M. A. Dugan, J. S. Melinger, A. C. Albrecht, Chem. Phys. Lett. 147, 411(1988).
[CrossRef]

Felker, P. M.

P. M. Felker, G. V. Hartland, Chem. Phys. Lett. 134, 503 (1987).
[CrossRef]

Fork, R. L.

P. C. Becker, H. L. Fragnito, J. Y. Bigot, C. H. Brito Cruz, R. L. Fork, C. V. Shank, Phys. Rev. Lett. 63, 505 (1989).
[CrossRef] [PubMed]

Fragnito, H. L.

P. C. Becker, H. L. Fragnito, J. Y. Bigot, C. H. Brito Cruz, R. L. Fork, C. V. Shank, Phys. Rev. Lett. 63, 505 (1989).
[CrossRef] [PubMed]

Fujiwara, M.

Ha, J. M. Y.

J. M. Y. Ha, H. J. Maris, W. M. Risen, J. Tauc, Phys. Rev. Lett. 57, 3302 (1986).
[CrossRef] [PubMed]

Hartland, G. V.

P. M. Felker, G. V. Hartland, Chem. Phys. Lett. 134, 503 (1987).
[CrossRef]

Hartmann, S. R.

D. DeBeer, E. Usadi, S. R. Hartmann, Phys. Rev. Lett. 60, 1262 (1988).
[CrossRef] [PubMed]

Hayden, C.

C. Hayden, R. Trevino, Lawrence Livermore Laboratory, Livermore, California 94550 (personal communication).

Heller, E.

J. Z. Zhang, E. Heller, D. Huber, D. G. Imre, D. Tannor, J. Chem. Phys. 89, 3602 (1988).
[CrossRef]

Herzberg, G.

G. Herzberg, Electronic Spectra of Polyatomic Molecules (Van Nostrand Reinhold, New York, 1966).

Huber, D.

J. Z. Zhang, E. Heller, D. Huber, D. G. Imre, D. Tannor, J. Chem. Phys. 89, 3602 (1988).
[CrossRef]

Imre, D. G.

J. Z. Zhang, E. Heller, D. Huber, D. G. Imre, D. Tannor, J. Chem. Phys. 89, 3602 (1988).
[CrossRef]

Ippen, E. P.

Joly, A. G.

S. Ruhman, A. G. Joly, K. Nelson, IEEE J. Quantum Electron. 24, 460 (1988).
[CrossRef]

Kalt, H.

H. Kalt, R. Renner, C. Klingshirn, IEEE J. Quantum Electron. QE-22, 1312 (1986).
[CrossRef]

Klingshirn, C.

H. Kalt, R. Renner, C. Klingshirn, IEEE J. Quantum Electron. QE-22, 1312 (1986).
[CrossRef]

Kuroda, R.

Maris, H. J.

J. M. Y. Ha, H. J. Maris, W. M. Risen, J. Tauc, Phys. Rev. Lett. 57, 3302 (1986).
[CrossRef] [PubMed]

Melinger, J. S.

M. A. Dugan, J. S. Melinger, A. C. Albrecht, Chem. Phys. Lett. 147, 411(1988).
[CrossRef]

Morita, N.

N. Morita, T. Yajima, Phys. Rev. A 30, 2525 (1984).
[CrossRef]

Nakatsuka, H.

Nelson, K.

S. Ruhman, A. G. Joly, K. Nelson, IEEE J. Quantum Electron. 24, 460 (1988).
[CrossRef]

Renner, R.

H. Kalt, R. Renner, C. Klingshirn, IEEE J. Quantum Electron. QE-22, 1312 (1986).
[CrossRef]

Risen, W. M.

J. M. Y. Ha, H. J. Maris, W. M. Risen, J. Tauc, Phys. Rev. Lett. 57, 3302 (1986).
[CrossRef] [PubMed]

Rosker, M. J.

M. Dantus, M. J. Rosker, A. H. Zewail, J. Chem. Phys. 89, 6128 (1988).
[CrossRef]

M. J. Rosker, F. W. Wise, C. L. Tang, Phys. Rev. Lett. 57, 321 (1986).
[CrossRef] [PubMed]

Ruhman, S.

S. Ruhman, A. G. Joly, K. Nelson, IEEE J. Quantum Electron. 24, 460 (1988).
[CrossRef]

Shank, C. V.

P. C. Becker, H. L. Fragnito, J. Y. Bigot, C. H. Brito Cruz, R. L. Fork, C. V. Shank, Phys. Rev. Lett. 63, 505 (1989).
[CrossRef] [PubMed]

Tang, C. L.

M. J. Rosker, F. W. Wise, C. L. Tang, Phys. Rev. Lett. 57, 321 (1986).
[CrossRef] [PubMed]

Tannor, D.

J. Z. Zhang, E. Heller, D. Huber, D. G. Imre, D. Tannor, J. Chem. Phys. 89, 3602 (1988).
[CrossRef]

Tauc, J.

J. M. Y. Ha, H. J. Maris, W. M. Risen, J. Tauc, Phys. Rev. Lett. 57, 3302 (1986).
[CrossRef] [PubMed]

Trevino, R.

C. Hayden, R. Trevino, Lawrence Livermore Laboratory, Livermore, California 94550 (personal communication).

Usadi, E.

D. DeBeer, E. Usadi, S. R. Hartmann, Phys. Rev. Lett. 60, 1262 (1988).
[CrossRef] [PubMed]

Weiner, A. M.

Wise, F. W.

M. J. Rosker, F. W. Wise, C. L. Tang, Phys. Rev. Lett. 57, 321 (1986).
[CrossRef] [PubMed]

Xie, Y. J.

Y. J. Xie, Ph.D. dissertation (State University of New York at Buffalo, Amherst, N.Y., 1989).

Yajima, T.

N. Morita, T. Yajima, Phys. Rev. A 30, 2525 (1984).
[CrossRef]

Zewail, A. H.

M. Dantus, M. J. Rosker, A. H. Zewail, J. Chem. Phys. 89, 6128 (1988).
[CrossRef]

Zhang, J. Z.

J. Z. Zhang, E. Heller, D. Huber, D. G. Imre, D. Tannor, J. Chem. Phys. 89, 3602 (1988).
[CrossRef]

Chem. Phys. Lett. (2)

M. A. Dugan, J. S. Melinger, A. C. Albrecht, Chem. Phys. Lett. 147, 411(1988).
[CrossRef]

P. M. Felker, G. V. Hartland, Chem. Phys. Lett. 134, 503 (1987).
[CrossRef]

IEEE J. Quantum Electron. (2)

S. Ruhman, A. G. Joly, K. Nelson, IEEE J. Quantum Electron. 24, 460 (1988).
[CrossRef]

H. Kalt, R. Renner, C. Klingshirn, IEEE J. Quantum Electron. QE-22, 1312 (1986).
[CrossRef]

J. Chem. Phys. (2)

M. Dantus, M. J. Rosker, A. H. Zewail, J. Chem. Phys. 89, 6128 (1988).
[CrossRef]

J. Z. Zhang, E. Heller, D. Huber, D. G. Imre, D. Tannor, J. Chem. Phys. 89, 3602 (1988).
[CrossRef]

J. Opt. Soc. Am. B (2)

Phys. Rev. A (1)

N. Morita, T. Yajima, Phys. Rev. A 30, 2525 (1984).
[CrossRef]

Phys. Rev. Lett. (4)

D. DeBeer, E. Usadi, S. R. Hartmann, Phys. Rev. Lett. 60, 1262 (1988).
[CrossRef] [PubMed]

P. C. Becker, H. L. Fragnito, J. Y. Bigot, C. H. Brito Cruz, R. L. Fork, C. V. Shank, Phys. Rev. Lett. 63, 505 (1989).
[CrossRef] [PubMed]

M. J. Rosker, F. W. Wise, C. L. Tang, Phys. Rev. Lett. 57, 321 (1986).
[CrossRef] [PubMed]

J. M. Y. Ha, H. J. Maris, W. M. Risen, J. Tauc, Phys. Rev. Lett. 57, 3302 (1986).
[CrossRef] [PubMed]

Other (3)

C. Hayden, R. Trevino, Lawrence Livermore Laboratory, Livermore, California 94550 (personal communication).

Y. J. Xie, Ph.D. dissertation (State University of New York at Buffalo, Amherst, N.Y., 1989).

G. Herzberg, Electronic Spectra of Polyatomic Molecules (Van Nostrand Reinhold, New York, 1966).

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Figures (4)

Fig. 1
Fig. 1

Schematic of the SDIL experiment. DC1 and DC2, dye cells; BS’s, beam splitters; PD, photodiode; CL, cylindrical lens; PMT, photomultiplier tube.

Fig. 2
Fig. 2

SDIL signal for Rhodamine 590 in polyester at 300 K. Crosses, 2k1k2; dots, 2k2k1.

Fig. 3
Fig. 3

SDIL signal for Rhodamine 590 in polyester at 120 K. Crosses, 2k1k2; dots, 2k2k1. The solid curves are theoretical fits with the formulation in Ref. 12.

Fig. 4
Fig. 4

SDIL signal for Rhodamine 560 at 300 K. The oscillations are due to molecular vibrations. The solid curve is for visual aid only.

Equations (2)

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R e υ e υ = ψ υ ψ υ R e e ( Q ) ,
R e e ( Q ) = ψ e ( q , Q ) | M e | ψ e ( q , Q ) ,

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