Abstract

By using time-resolved coherent Raman scattering, closely spaced vibrational resonances are simultaneously excited and subsequently monitored over long, nanosecond time intervals. Coherent superposition of molecular transitions leads to dramatic oscillations of the picosecond anti-Stokes scattering signals. Experimental data are presented for the ν1 mode of CH4 in supersonic expansions at low rotational temperatures (TROT ≥ 25). Our time-domain data are in good agreement with spectroscopic results. The corresponding frequency resolution of ≲3 × 10−3 cm−1 suggests that this method of Fourier-transform Raman spectroscopy may prove useful in high-resolution molecular spectroscopy.

© 1984 Optical Society of America

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  1. P. Huber-Wälchli, D. M. Guthals, J. W. Nibler, Chem. Phys. Lett. 67, 233 (1979).
    [Crossref]
  2. M. D. Duncan, P. Oesterlin, R. L. Byer, Opt. Lett. 6, 90 (1981).
    [Crossref] [PubMed]
  3. J. J. Valentini, P. Esherick, A. Owyoung, Chem. Phys. Lett. 75, 590 (1980).
    [Crossref]
  4. E. K. Gustafson, J. C. McDaniel, R. L. Byer, Opt. Lett. 7, 434 (1982).
    [Crossref] [PubMed]
  5. A. Laubereau, W. Kaiser, Rev. Mod. Phys. 50, 607 (1978); A. Laubereau, G. Wochner, W. Kaiser, Opt. Commun. 17, 91 (1976).
    [Crossref]
  6. S. A. Magnitsky, V. G. Tunkin, Sov. J. Quantum Electron. 11, 1218 (1981).
    [Crossref]
  7. H. Graener, A. Laubereau, Appl. Phys. B 29, 213 (1982); H.-J. Hartmann, H. Graener, H. R. Telle, A. Laubereau, in Applications of Picosecond Spectroscopy in Chemistry, K. B. Eisenthal, ed., NATO ASI Series (Riedel, Dordrecht, The Netherlands, 1983).
    [Crossref]
  8. J. B. Cross, J. J. Valentini, Rev. Sci. Instrum. 53, 38 (1982).
    [Crossref]
  9. A. Owyoung, C. W. Patterson, R. S. McDowell, Chem. Phys. Lett. 59, 156 (1978).
    [Crossref]
  10. P. Huber-Wälchli, J. W. Nibler, J. Chem. Phys. 76, 273 (1982).
    [Crossref]
  11. G. Pubanz, J. W. Nibler (unpublished results).
  12. After completion of this work we learned that related measurements have been performed by Yu. E. Diakov, S. Yu. Nikitin, S. A. Magnitsky, A. P. Tarasevich and presented in a paper at the Ultrafast Phenomena in Spectroscopy Meeting, Minsk, USSR, 1983.

1982 (4)

E. K. Gustafson, J. C. McDaniel, R. L. Byer, Opt. Lett. 7, 434 (1982).
[Crossref] [PubMed]

H. Graener, A. Laubereau, Appl. Phys. B 29, 213 (1982); H.-J. Hartmann, H. Graener, H. R. Telle, A. Laubereau, in Applications of Picosecond Spectroscopy in Chemistry, K. B. Eisenthal, ed., NATO ASI Series (Riedel, Dordrecht, The Netherlands, 1983).
[Crossref]

J. B. Cross, J. J. Valentini, Rev. Sci. Instrum. 53, 38 (1982).
[Crossref]

P. Huber-Wälchli, J. W. Nibler, J. Chem. Phys. 76, 273 (1982).
[Crossref]

1981 (2)

S. A. Magnitsky, V. G. Tunkin, Sov. J. Quantum Electron. 11, 1218 (1981).
[Crossref]

M. D. Duncan, P. Oesterlin, R. L. Byer, Opt. Lett. 6, 90 (1981).
[Crossref] [PubMed]

1980 (1)

J. J. Valentini, P. Esherick, A. Owyoung, Chem. Phys. Lett. 75, 590 (1980).
[Crossref]

1979 (1)

P. Huber-Wälchli, D. M. Guthals, J. W. Nibler, Chem. Phys. Lett. 67, 233 (1979).
[Crossref]

1978 (2)

A. Owyoung, C. W. Patterson, R. S. McDowell, Chem. Phys. Lett. 59, 156 (1978).
[Crossref]

A. Laubereau, W. Kaiser, Rev. Mod. Phys. 50, 607 (1978); A. Laubereau, G. Wochner, W. Kaiser, Opt. Commun. 17, 91 (1976).
[Crossref]

Byer, R. L.

Cross, J. B.

J. B. Cross, J. J. Valentini, Rev. Sci. Instrum. 53, 38 (1982).
[Crossref]

Diakov, Yu. E.

After completion of this work we learned that related measurements have been performed by Yu. E. Diakov, S. Yu. Nikitin, S. A. Magnitsky, A. P. Tarasevich and presented in a paper at the Ultrafast Phenomena in Spectroscopy Meeting, Minsk, USSR, 1983.

Duncan, M. D.

Esherick, P.

J. J. Valentini, P. Esherick, A. Owyoung, Chem. Phys. Lett. 75, 590 (1980).
[Crossref]

Graener, H.

H. Graener, A. Laubereau, Appl. Phys. B 29, 213 (1982); H.-J. Hartmann, H. Graener, H. R. Telle, A. Laubereau, in Applications of Picosecond Spectroscopy in Chemistry, K. B. Eisenthal, ed., NATO ASI Series (Riedel, Dordrecht, The Netherlands, 1983).
[Crossref]

Gustafson, E. K.

Guthals, D. M.

P. Huber-Wälchli, D. M. Guthals, J. W. Nibler, Chem. Phys. Lett. 67, 233 (1979).
[Crossref]

Huber-Wälchli, P.

P. Huber-Wälchli, J. W. Nibler, J. Chem. Phys. 76, 273 (1982).
[Crossref]

P. Huber-Wälchli, D. M. Guthals, J. W. Nibler, Chem. Phys. Lett. 67, 233 (1979).
[Crossref]

Kaiser, W.

A. Laubereau, W. Kaiser, Rev. Mod. Phys. 50, 607 (1978); A. Laubereau, G. Wochner, W. Kaiser, Opt. Commun. 17, 91 (1976).
[Crossref]

Laubereau, A.

H. Graener, A. Laubereau, Appl. Phys. B 29, 213 (1982); H.-J. Hartmann, H. Graener, H. R. Telle, A. Laubereau, in Applications of Picosecond Spectroscopy in Chemistry, K. B. Eisenthal, ed., NATO ASI Series (Riedel, Dordrecht, The Netherlands, 1983).
[Crossref]

A. Laubereau, W. Kaiser, Rev. Mod. Phys. 50, 607 (1978); A. Laubereau, G. Wochner, W. Kaiser, Opt. Commun. 17, 91 (1976).
[Crossref]

Magnitsky, S. A.

S. A. Magnitsky, V. G. Tunkin, Sov. J. Quantum Electron. 11, 1218 (1981).
[Crossref]

After completion of this work we learned that related measurements have been performed by Yu. E. Diakov, S. Yu. Nikitin, S. A. Magnitsky, A. P. Tarasevich and presented in a paper at the Ultrafast Phenomena in Spectroscopy Meeting, Minsk, USSR, 1983.

McDaniel, J. C.

McDowell, R. S.

A. Owyoung, C. W. Patterson, R. S. McDowell, Chem. Phys. Lett. 59, 156 (1978).
[Crossref]

Nibler, J. W.

P. Huber-Wälchli, J. W. Nibler, J. Chem. Phys. 76, 273 (1982).
[Crossref]

P. Huber-Wälchli, D. M. Guthals, J. W. Nibler, Chem. Phys. Lett. 67, 233 (1979).
[Crossref]

G. Pubanz, J. W. Nibler (unpublished results).

Nikitin, S. Yu.

After completion of this work we learned that related measurements have been performed by Yu. E. Diakov, S. Yu. Nikitin, S. A. Magnitsky, A. P. Tarasevich and presented in a paper at the Ultrafast Phenomena in Spectroscopy Meeting, Minsk, USSR, 1983.

Oesterlin, P.

Owyoung, A.

J. J. Valentini, P. Esherick, A. Owyoung, Chem. Phys. Lett. 75, 590 (1980).
[Crossref]

A. Owyoung, C. W. Patterson, R. S. McDowell, Chem. Phys. Lett. 59, 156 (1978).
[Crossref]

Patterson, C. W.

A. Owyoung, C. W. Patterson, R. S. McDowell, Chem. Phys. Lett. 59, 156 (1978).
[Crossref]

Pubanz, G.

G. Pubanz, J. W. Nibler (unpublished results).

Tarasevich, A. P.

After completion of this work we learned that related measurements have been performed by Yu. E. Diakov, S. Yu. Nikitin, S. A. Magnitsky, A. P. Tarasevich and presented in a paper at the Ultrafast Phenomena in Spectroscopy Meeting, Minsk, USSR, 1983.

Tunkin, V. G.

S. A. Magnitsky, V. G. Tunkin, Sov. J. Quantum Electron. 11, 1218 (1981).
[Crossref]

Valentini, J. J.

J. B. Cross, J. J. Valentini, Rev. Sci. Instrum. 53, 38 (1982).
[Crossref]

J. J. Valentini, P. Esherick, A. Owyoung, Chem. Phys. Lett. 75, 590 (1980).
[Crossref]

Appl. Phys. B (1)

H. Graener, A. Laubereau, Appl. Phys. B 29, 213 (1982); H.-J. Hartmann, H. Graener, H. R. Telle, A. Laubereau, in Applications of Picosecond Spectroscopy in Chemistry, K. B. Eisenthal, ed., NATO ASI Series (Riedel, Dordrecht, The Netherlands, 1983).
[Crossref]

Chem. Phys. Lett. (3)

P. Huber-Wälchli, D. M. Guthals, J. W. Nibler, Chem. Phys. Lett. 67, 233 (1979).
[Crossref]

J. J. Valentini, P. Esherick, A. Owyoung, Chem. Phys. Lett. 75, 590 (1980).
[Crossref]

A. Owyoung, C. W. Patterson, R. S. McDowell, Chem. Phys. Lett. 59, 156 (1978).
[Crossref]

J. Chem. Phys. (1)

P. Huber-Wälchli, J. W. Nibler, J. Chem. Phys. 76, 273 (1982).
[Crossref]

Opt. Lett. (2)

Rev. Mod. Phys. (1)

A. Laubereau, W. Kaiser, Rev. Mod. Phys. 50, 607 (1978); A. Laubereau, G. Wochner, W. Kaiser, Opt. Commun. 17, 91 (1976).
[Crossref]

Rev. Sci. Instrum. (1)

J. B. Cross, J. J. Valentini, Rev. Sci. Instrum. 53, 38 (1982).
[Crossref]

Sov. J. Quantum Electron. (1)

S. A. Magnitsky, V. G. Tunkin, Sov. J. Quantum Electron. 11, 1218 (1981).
[Crossref]

Other (2)

G. Pubanz, J. W. Nibler (unpublished results).

After completion of this work we learned that related measurements have been performed by Yu. E. Diakov, S. Yu. Nikitin, S. A. Magnitsky, A. P. Tarasevich and presented in a paper at the Ultrafast Phenomena in Spectroscopy Meeting, Minsk, USSR, 1983.

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Figures (3)

Fig. 1
Fig. 1

Schematic of the experimental system for time-resolved CARS of free jet expansions with four different (excitation and probing frequencies); inset: variable nanosecond optical delay VD with picosecond accuracy.

Fig. 2
Fig. 2

Coherent probe scattering signal Scoh(tD) versus delay time between excitation and probing pulses for the ν1 Q band of pure CH4. The filled theoretical curve (solid line) yields TROT = 78 ± 5 K; dashed line, instrumental response function; inset: calculated spectral intensity distribution corresponding to the observed signal transient.

Fig. 3
Fig. 3

Same as Fig. 2 for argon–methane mixture 2:1; yielding TROT = 25 ± 3 K. A frequency resolution of ~3 × 10−3 cm−1 is estimated.

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