Abstract

A time-resolved coherent anti-Stokes Raman technique is demonstrated that yields a spectral resolution beyond the linewidth obtained in spontaneous Raman spectroscopy. Two picosecond dye lasers, independently tunable with low timing jitter, are used. The coherent material excitation is generated by long pump pulses and monitored by short delayed probing pulses. Transiently narrowed Raman spectra are recorded by scanning the lasers over the resonances of interest and simultaneously monitoring the coherent scattering signal as a function of the excitation frequency. The technique is applied to molecular vibrations in liquids. The differences between the technique presented and standard coherent anti-Stokes Raman spectroscopy are demonstrated.

© 1985 Optical Society of America

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  1. I.-J. Ma, J. Mertens, G. zu Putlitz, G. Schütte, Z. Phys. 208, 352 (1968).
    [CrossRef]
  2. G. Copley, B. P. Kibble, G. W. Series, J. Phys. B 1, 724 (1968).
    [CrossRef]
  3. H. Figger, H. Walther, Z. Phys. 267,1 (1974).
    [CrossRef]
  4. H. Metcalf, W. Phillips, Opt. Lett. 5, 540 (1980).
    [CrossRef]
  5. P. Meystre, M. O. Scully, H. Walther, Opt. Commun. 33, 153 (1980).
    [CrossRef]
  6. W. Zinth, Opt. Commun. 34, 479 (1980).
    [CrossRef]
  7. W. Zinth, M. C. Nuss, W. Kaiser, Chem. Phys. Lett. 88, 257 (1982).
    [CrossRef]
  8. W. Zinth, M. C. Nuss, W. Kaiser, Opt. Commun. 44, 262 (1983).
    [CrossRef]
  9. A. Penzkofer, A. Laubereau, W. Kaiser, Prog. Quantum Electron. 6, 55 (1979).
    [CrossRef]
  10. W. Zinth, A. Laubereau, W. Kaiser, Opt. Commun. 26, 457 (1978).
    [CrossRef]
  11. F. M. Kamga, M. G. Sceats, Opt. Lett. 5, 126 (1980).
    [CrossRef]
  12. J. Kuhl, D. v. d. Linde, in Picosecond Phenomena III, Vol. 23 of Springer Series in Chemical Physics, K. B. Eisenthal, R. M. Hochstrasser, W. Kaiser, A. Laubereau, eds. (Springer-Verlag, Heidelberg, 1982), p. 201.
    [CrossRef]
  13. J. M. Clemens, J. Najbar, I. Bronstein-Bonte, R. M. Hochstrasser, Opt. Commun. 47, 271 (1983).
    [CrossRef]
  14. D. A. Long, F. S. Murfin, E. L. Thomas, Trans. Faraday Soc. 59, 12 (1963).
    [CrossRef]
  15. H. Takahashi, K. Mahola, E. K. Plyler, J. Mol. Spectrosc. 21, 217 (1966).
    [CrossRef]
  16. B. P. Asthana, H. Takahashi, W. Kiefer, Chem. Phys. Lett. 94, 41 (1983).
    [CrossRef]
  17. W. Zinth, M. C. Nuss, W. Kaiser, Phys. Rev. A 30, 1139 (1984).
    [CrossRef]

1984 (1)

W. Zinth, M. C. Nuss, W. Kaiser, Phys. Rev. A 30, 1139 (1984).
[CrossRef]

1983 (3)

J. M. Clemens, J. Najbar, I. Bronstein-Bonte, R. M. Hochstrasser, Opt. Commun. 47, 271 (1983).
[CrossRef]

B. P. Asthana, H. Takahashi, W. Kiefer, Chem. Phys. Lett. 94, 41 (1983).
[CrossRef]

W. Zinth, M. C. Nuss, W. Kaiser, Opt. Commun. 44, 262 (1983).
[CrossRef]

1982 (1)

W. Zinth, M. C. Nuss, W. Kaiser, Chem. Phys. Lett. 88, 257 (1982).
[CrossRef]

1980 (4)

P. Meystre, M. O. Scully, H. Walther, Opt. Commun. 33, 153 (1980).
[CrossRef]

W. Zinth, Opt. Commun. 34, 479 (1980).
[CrossRef]

F. M. Kamga, M. G. Sceats, Opt. Lett. 5, 126 (1980).
[CrossRef]

H. Metcalf, W. Phillips, Opt. Lett. 5, 540 (1980).
[CrossRef]

1979 (1)

A. Penzkofer, A. Laubereau, W. Kaiser, Prog. Quantum Electron. 6, 55 (1979).
[CrossRef]

1978 (1)

W. Zinth, A. Laubereau, W. Kaiser, Opt. Commun. 26, 457 (1978).
[CrossRef]

1974 (1)

H. Figger, H. Walther, Z. Phys. 267,1 (1974).
[CrossRef]

1968 (2)

I.-J. Ma, J. Mertens, G. zu Putlitz, G. Schütte, Z. Phys. 208, 352 (1968).
[CrossRef]

G. Copley, B. P. Kibble, G. W. Series, J. Phys. B 1, 724 (1968).
[CrossRef]

1966 (1)

H. Takahashi, K. Mahola, E. K. Plyler, J. Mol. Spectrosc. 21, 217 (1966).
[CrossRef]

1963 (1)

D. A. Long, F. S. Murfin, E. L. Thomas, Trans. Faraday Soc. 59, 12 (1963).
[CrossRef]

Asthana, B. P.

B. P. Asthana, H. Takahashi, W. Kiefer, Chem. Phys. Lett. 94, 41 (1983).
[CrossRef]

Bronstein-Bonte, I.

J. M. Clemens, J. Najbar, I. Bronstein-Bonte, R. M. Hochstrasser, Opt. Commun. 47, 271 (1983).
[CrossRef]

Clemens, J. M.

J. M. Clemens, J. Najbar, I. Bronstein-Bonte, R. M. Hochstrasser, Opt. Commun. 47, 271 (1983).
[CrossRef]

Copley, G.

G. Copley, B. P. Kibble, G. W. Series, J. Phys. B 1, 724 (1968).
[CrossRef]

Figger, H.

H. Figger, H. Walther, Z. Phys. 267,1 (1974).
[CrossRef]

Hochstrasser, R. M.

J. M. Clemens, J. Najbar, I. Bronstein-Bonte, R. M. Hochstrasser, Opt. Commun. 47, 271 (1983).
[CrossRef]

Kaiser, W.

W. Zinth, M. C. Nuss, W. Kaiser, Phys. Rev. A 30, 1139 (1984).
[CrossRef]

W. Zinth, M. C. Nuss, W. Kaiser, Opt. Commun. 44, 262 (1983).
[CrossRef]

W. Zinth, M. C. Nuss, W. Kaiser, Chem. Phys. Lett. 88, 257 (1982).
[CrossRef]

A. Penzkofer, A. Laubereau, W. Kaiser, Prog. Quantum Electron. 6, 55 (1979).
[CrossRef]

W. Zinth, A. Laubereau, W. Kaiser, Opt. Commun. 26, 457 (1978).
[CrossRef]

Kamga, F. M.

Kibble, B. P.

G. Copley, B. P. Kibble, G. W. Series, J. Phys. B 1, 724 (1968).
[CrossRef]

Kiefer, W.

B. P. Asthana, H. Takahashi, W. Kiefer, Chem. Phys. Lett. 94, 41 (1983).
[CrossRef]

Kuhl, J.

J. Kuhl, D. v. d. Linde, in Picosecond Phenomena III, Vol. 23 of Springer Series in Chemical Physics, K. B. Eisenthal, R. M. Hochstrasser, W. Kaiser, A. Laubereau, eds. (Springer-Verlag, Heidelberg, 1982), p. 201.
[CrossRef]

Laubereau, A.

A. Penzkofer, A. Laubereau, W. Kaiser, Prog. Quantum Electron. 6, 55 (1979).
[CrossRef]

W. Zinth, A. Laubereau, W. Kaiser, Opt. Commun. 26, 457 (1978).
[CrossRef]

Linde, D. v. d.

J. Kuhl, D. v. d. Linde, in Picosecond Phenomena III, Vol. 23 of Springer Series in Chemical Physics, K. B. Eisenthal, R. M. Hochstrasser, W. Kaiser, A. Laubereau, eds. (Springer-Verlag, Heidelberg, 1982), p. 201.
[CrossRef]

Long, D. A.

D. A. Long, F. S. Murfin, E. L. Thomas, Trans. Faraday Soc. 59, 12 (1963).
[CrossRef]

Ma, I.-J.

I.-J. Ma, J. Mertens, G. zu Putlitz, G. Schütte, Z. Phys. 208, 352 (1968).
[CrossRef]

Mahola, K.

H. Takahashi, K. Mahola, E. K. Plyler, J. Mol. Spectrosc. 21, 217 (1966).
[CrossRef]

Mertens, J.

I.-J. Ma, J. Mertens, G. zu Putlitz, G. Schütte, Z. Phys. 208, 352 (1968).
[CrossRef]

Metcalf, H.

Meystre, P.

P. Meystre, M. O. Scully, H. Walther, Opt. Commun. 33, 153 (1980).
[CrossRef]

Murfin, F. S.

D. A. Long, F. S. Murfin, E. L. Thomas, Trans. Faraday Soc. 59, 12 (1963).
[CrossRef]

Najbar, J.

J. M. Clemens, J. Najbar, I. Bronstein-Bonte, R. M. Hochstrasser, Opt. Commun. 47, 271 (1983).
[CrossRef]

Nuss, M. C.

W. Zinth, M. C. Nuss, W. Kaiser, Phys. Rev. A 30, 1139 (1984).
[CrossRef]

W. Zinth, M. C. Nuss, W. Kaiser, Opt. Commun. 44, 262 (1983).
[CrossRef]

W. Zinth, M. C. Nuss, W. Kaiser, Chem. Phys. Lett. 88, 257 (1982).
[CrossRef]

Penzkofer, A.

A. Penzkofer, A. Laubereau, W. Kaiser, Prog. Quantum Electron. 6, 55 (1979).
[CrossRef]

Phillips, W.

Plyler, E. K.

H. Takahashi, K. Mahola, E. K. Plyler, J. Mol. Spectrosc. 21, 217 (1966).
[CrossRef]

Sceats, M. G.

Schütte, G.

I.-J. Ma, J. Mertens, G. zu Putlitz, G. Schütte, Z. Phys. 208, 352 (1968).
[CrossRef]

Scully, M. O.

P. Meystre, M. O. Scully, H. Walther, Opt. Commun. 33, 153 (1980).
[CrossRef]

Series, G. W.

G. Copley, B. P. Kibble, G. W. Series, J. Phys. B 1, 724 (1968).
[CrossRef]

Takahashi, H.

B. P. Asthana, H. Takahashi, W. Kiefer, Chem. Phys. Lett. 94, 41 (1983).
[CrossRef]

H. Takahashi, K. Mahola, E. K. Plyler, J. Mol. Spectrosc. 21, 217 (1966).
[CrossRef]

Thomas, E. L.

D. A. Long, F. S. Murfin, E. L. Thomas, Trans. Faraday Soc. 59, 12 (1963).
[CrossRef]

Walther, H.

P. Meystre, M. O. Scully, H. Walther, Opt. Commun. 33, 153 (1980).
[CrossRef]

H. Figger, H. Walther, Z. Phys. 267,1 (1974).
[CrossRef]

Zinth, W.

W. Zinth, M. C. Nuss, W. Kaiser, Phys. Rev. A 30, 1139 (1984).
[CrossRef]

W. Zinth, M. C. Nuss, W. Kaiser, Opt. Commun. 44, 262 (1983).
[CrossRef]

W. Zinth, M. C. Nuss, W. Kaiser, Chem. Phys. Lett. 88, 257 (1982).
[CrossRef]

W. Zinth, Opt. Commun. 34, 479 (1980).
[CrossRef]

W. Zinth, A. Laubereau, W. Kaiser, Opt. Commun. 26, 457 (1978).
[CrossRef]

zu Putlitz, G.

I.-J. Ma, J. Mertens, G. zu Putlitz, G. Schütte, Z. Phys. 208, 352 (1968).
[CrossRef]

Chem. Phys. Lett. (2)

W. Zinth, M. C. Nuss, W. Kaiser, Chem. Phys. Lett. 88, 257 (1982).
[CrossRef]

B. P. Asthana, H. Takahashi, W. Kiefer, Chem. Phys. Lett. 94, 41 (1983).
[CrossRef]

J. Mol. Spectrosc. (1)

H. Takahashi, K. Mahola, E. K. Plyler, J. Mol. Spectrosc. 21, 217 (1966).
[CrossRef]

J. Phys. B (1)

G. Copley, B. P. Kibble, G. W. Series, J. Phys. B 1, 724 (1968).
[CrossRef]

Opt. Commun. (5)

P. Meystre, M. O. Scully, H. Walther, Opt. Commun. 33, 153 (1980).
[CrossRef]

W. Zinth, Opt. Commun. 34, 479 (1980).
[CrossRef]

W. Zinth, M. C. Nuss, W. Kaiser, Opt. Commun. 44, 262 (1983).
[CrossRef]

W. Zinth, A. Laubereau, W. Kaiser, Opt. Commun. 26, 457 (1978).
[CrossRef]

J. M. Clemens, J. Najbar, I. Bronstein-Bonte, R. M. Hochstrasser, Opt. Commun. 47, 271 (1983).
[CrossRef]

Opt. Lett. (2)

Phys. Rev. A (1)

W. Zinth, M. C. Nuss, W. Kaiser, Phys. Rev. A 30, 1139 (1984).
[CrossRef]

Prog. Quantum Electron. (1)

A. Penzkofer, A. Laubereau, W. Kaiser, Prog. Quantum Electron. 6, 55 (1979).
[CrossRef]

Trans. Faraday Soc. (1)

D. A. Long, F. S. Murfin, E. L. Thomas, Trans. Faraday Soc. 59, 12 (1963).
[CrossRef]

Z. Phys. (2)

I.-J. Ma, J. Mertens, G. zu Putlitz, G. Schütte, Z. Phys. 208, 352 (1968).
[CrossRef]

H. Figger, H. Walther, Z. Phys. 267,1 (1974).
[CrossRef]

Other (1)

J. Kuhl, D. v. d. Linde, in Picosecond Phenomena III, Vol. 23 of Springer Series in Chemical Physics, K. B. Eisenthal, R. M. Hochstrasser, W. Kaiser, A. Laubereau, eds. (Springer-Verlag, Heidelberg, 1982), p. 201.
[CrossRef]

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Figures (4)

Fig. 1
Fig. 1

(a) Semilogarithmic plot of the measured autocorrelation function of the DCM dye laser operated at 640 nm. The FWHH is 4.9 psec. (b) Cross correlation of the Rhodamine 6G laser and the DCM dye laser with FWHH 6.2 psec.

Fig. 2
Fig. 2

Experimental setup for high-resolution Raman spectroscopy consisting of delay lines DL1 and DL2, polarizers, photomultiplier PMT, and dye jet as saturable absorber SA.

Fig. 3
Fig. 3

(a) Spontaneous Raman spectrum of the ν1 mode (990 cm−1) of pyridine taken with a resolution of 0.5 cm−1. (b) Comparison of CARS and narrowed CARS measurements of the same Raman line. Both spectra were taken with the setup of Fig. 2. In the narrowed CARS experiment the weak probe pulse was delayed with respect to the excitation pulses by approximately 20 psec.

Fig. 4
Fig. 4

(a) Spontaneous Raman spectrum of a mixture pyridine–methanol with 0.5-M concentration of pyridine taken with a Raman spectrometer with 0.5-cm−1 resolution. (b) Coherent anti-Stokes Raman spectrum of the same mixture taken at tD = 0 (dashed curve) and tD = 15 psec (solid curve). Two peaks can be resolved under the broad band around 998-cm−1 in the delayed transient CARS experiment.

Equations (4)

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E A x E L 2 E S * χ ( 3 ) = E L 2 E S * ( χ RES ( 3 ) + χ NR ( 3 ) ) ,
E AS x E L 2 q * + χ NR ( 3 ) E L E L 2 E S * .
2 q t 2 + 2 T 2 q t + ω 0 q = Ã ( t ) ,
q ( t D , Δ ω ) exp ( t D / T 2 ) t D d t exp ( i Δ ω t ) A ( t ) exp ( t / T 2 ) ,

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