Abstract

We report the first measurements to our knowledge of the effects of two-photon Raman saturation on fully resolved, homogeneously broadened coherent anti-Stokes Raman spectroscopy (CARS) line shapes. Saturation dips and line broadening were observed with a high-resolution scanning CARS experiment using a single-mode, frequency-doubled Nd:YAG laser and a pulse-amplified cw dye laser. Saturated line shapes are compared with the results of numerical solutions of the time-dependent density matrix equations.

© 1986 Optical Society of America

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  1. S. A. J. Druet, B. Attal, T. K. Gustafson, J.-P. E. Taran, Phys. Rev. A 18, 1529 (1978).
    [CrossRef]
  2. A. D. Wilson-Gordon, R. Klimovsky-Barid, H. Friedmann, Phys. Rev. A 25, 1580 (1982).
    [CrossRef]
  3. V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
    [CrossRef]
  4. A. M. Brodnikovskii, S. M. Gladkov, N. I. Koroteev, Opt. Commun. 40, 312 (1982).
    [CrossRef]
  5. A. M. Brodnikovskii, V. N. Zadkov, M. G. Karimov, N. I. Koroteev, Opt. Spectrosc. (USSR) 54, 227 (1983).
  6. M. D. Duncan, P. Oesterlin, F. K. Konig, R. L. Byer, Chem. Phys. Lett. 80, 253 (1981).
    [CrossRef]
  7. A. Owyoung, P. Esherick, Opt. Lett. 5, 421 (1980).
    [CrossRef] [PubMed]
  8. W. E. Lamb, Phys. Rev. 134, A1429 (1964).
    [CrossRef]
  9. R. L. Schmitt, L. A. Rahn, Appl. Opt. 25, 629 (1986).
    [CrossRef] [PubMed]
  10. L. A. Rahn, R. L. Farrow, M. L. Koszykowski, P. L. Mattern, Phys. Rev. Lett. 45, 620 (1980).
    [CrossRef]
  11. A. Penzkofer, A. Laubereau, W. Kaiser, Prog. Quantum Electron. 6, 55 (1979).
    [CrossRef]
  12. G. J. Rosasco, W. Lempert, W. S. Hurst, A. Fein, Chem. Phys. Lett. 97, 435 (1983).
    [CrossRef]
  13. G. S. Agarwal, S. Singh, Phys. Rev. A 25, 3195 (1982).
    [CrossRef]
  14. V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
    [CrossRef]

1986 (1)

1984 (2)

V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
[CrossRef]

V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
[CrossRef]

1983 (2)

A. M. Brodnikovskii, V. N. Zadkov, M. G. Karimov, N. I. Koroteev, Opt. Spectrosc. (USSR) 54, 227 (1983).

G. J. Rosasco, W. Lempert, W. S. Hurst, A. Fein, Chem. Phys. Lett. 97, 435 (1983).
[CrossRef]

1982 (3)

G. S. Agarwal, S. Singh, Phys. Rev. A 25, 3195 (1982).
[CrossRef]

A. M. Brodnikovskii, S. M. Gladkov, N. I. Koroteev, Opt. Commun. 40, 312 (1982).
[CrossRef]

A. D. Wilson-Gordon, R. Klimovsky-Barid, H. Friedmann, Phys. Rev. A 25, 1580 (1982).
[CrossRef]

1981 (1)

M. D. Duncan, P. Oesterlin, F. K. Konig, R. L. Byer, Chem. Phys. Lett. 80, 253 (1981).
[CrossRef]

1980 (2)

A. Owyoung, P. Esherick, Opt. Lett. 5, 421 (1980).
[CrossRef] [PubMed]

L. A. Rahn, R. L. Farrow, M. L. Koszykowski, P. L. Mattern, Phys. Rev. Lett. 45, 620 (1980).
[CrossRef]

1979 (1)

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

1978 (1)

S. A. J. Druet, B. Attal, T. K. Gustafson, J.-P. E. Taran, Phys. Rev. A 18, 1529 (1978).
[CrossRef]

1964 (1)

W. E. Lamb, Phys. Rev. 134, A1429 (1964).
[CrossRef]

Agarwal, G. S.

G. S. Agarwal, S. Singh, Phys. Rev. A 25, 3195 (1982).
[CrossRef]

Attal, B.

S. A. J. Druet, B. Attal, T. K. Gustafson, J.-P. E. Taran, Phys. Rev. A 18, 1529 (1978).
[CrossRef]

Brodnikovskii, A. M.

A. M. Brodnikovskii, V. N. Zadkov, M. G. Karimov, N. I. Koroteev, Opt. Spectrosc. (USSR) 54, 227 (1983).

A. M. Brodnikovskii, S. M. Gladkov, N. I. Koroteev, Opt. Commun. 40, 312 (1982).
[CrossRef]

Byer, R. L.

M. D. Duncan, P. Oesterlin, F. K. Konig, R. L. Byer, Chem. Phys. Lett. 80, 253 (1981).
[CrossRef]

Druet, S. A. J.

S. A. J. Druet, B. Attal, T. K. Gustafson, J.-P. E. Taran, Phys. Rev. A 18, 1529 (1978).
[CrossRef]

Duncan, M. D.

M. D. Duncan, P. Oesterlin, F. K. Konig, R. L. Byer, Chem. Phys. Lett. 80, 253 (1981).
[CrossRef]

Esherick, P.

Farrow, R. L.

L. A. Rahn, R. L. Farrow, M. L. Koszykowski, P. L. Mattern, Phys. Rev. Lett. 45, 620 (1980).
[CrossRef]

Fein, A.

G. J. Rosasco, W. Lempert, W. S. Hurst, A. Fein, Chem. Phys. Lett. 97, 435 (1983).
[CrossRef]

Friedmann, H.

A. D. Wilson-Gordon, R. Klimovsky-Barid, H. Friedmann, Phys. Rev. A 25, 1580 (1982).
[CrossRef]

Gladkov, S. M.

A. M. Brodnikovskii, S. M. Gladkov, N. I. Koroteev, Opt. Commun. 40, 312 (1982).
[CrossRef]

Gustafson, T. K.

S. A. J. Druet, B. Attal, T. K. Gustafson, J.-P. E. Taran, Phys. Rev. A 18, 1529 (1978).
[CrossRef]

Hurst, W. S.

G. J. Rosasco, W. Lempert, W. S. Hurst, A. Fein, Chem. Phys. Lett. 97, 435 (1983).
[CrossRef]

Kaiser, W.

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

Karimov, M. G.

A. M. Brodnikovskii, V. N. Zadkov, M. G. Karimov, N. I. Koroteev, Opt. Spectrosc. (USSR) 54, 227 (1983).

Klimovsky-Barid, R.

A. D. Wilson-Gordon, R. Klimovsky-Barid, H. Friedmann, Phys. Rev. A 25, 1580 (1982).
[CrossRef]

Konig, F. K.

M. D. Duncan, P. Oesterlin, F. K. Konig, R. L. Byer, Chem. Phys. Lett. 80, 253 (1981).
[CrossRef]

Koroteev, N. I.

V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
[CrossRef]

V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
[CrossRef]

A. M. Brodnikovskii, V. N. Zadkov, M. G. Karimov, N. I. Koroteev, Opt. Spectrosc. (USSR) 54, 227 (1983).

A. M. Brodnikovskii, S. M. Gladkov, N. I. Koroteev, Opt. Commun. 40, 312 (1982).
[CrossRef]

Koszykowski, M. L.

L. A. Rahn, R. L. Farrow, M. L. Koszykowski, P. L. Mattern, Phys. Rev. Lett. 45, 620 (1980).
[CrossRef]

Lamb, W. E.

W. E. Lamb, Phys. Rev. 134, A1429 (1964).
[CrossRef]

Laubereau, A.

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

Lempert, W.

G. J. Rosasco, W. Lempert, W. S. Hurst, A. Fein, Chem. Phys. Lett. 97, 435 (1983).
[CrossRef]

Mattern, P. L.

L. A. Rahn, R. L. Farrow, M. L. Koszykowski, P. L. Mattern, Phys. Rev. Lett. 45, 620 (1980).
[CrossRef]

Oesterlin, P.

M. D. Duncan, P. Oesterlin, F. K. Konig, R. L. Byer, Chem. Phys. Lett. 80, 253 (1981).
[CrossRef]

Owyoung, A.

Penzkofer, A.

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

Rahn, L. A.

R. L. Schmitt, L. A. Rahn, Appl. Opt. 25, 629 (1986).
[CrossRef] [PubMed]

L. A. Rahn, R. L. Farrow, M. L. Koszykowski, P. L. Mattern, Phys. Rev. Lett. 45, 620 (1980).
[CrossRef]

Rosasco, G. J.

G. J. Rosasco, W. Lempert, W. S. Hurst, A. Fein, Chem. Phys. Lett. 97, 435 (1983).
[CrossRef]

Schmitt, R. L.

Singh, S.

G. S. Agarwal, S. Singh, Phys. Rev. A 25, 3195 (1982).
[CrossRef]

Taran, J.-P. E.

S. A. J. Druet, B. Attal, T. K. Gustafson, J.-P. E. Taran, Phys. Rev. A 18, 1529 (1978).
[CrossRef]

Wilson-Gordon, A. D.

A. D. Wilson-Gordon, R. Klimovsky-Barid, H. Friedmann, Phys. Rev. A 25, 1580 (1982).
[CrossRef]

Zadkov, V. N.

V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
[CrossRef]

V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
[CrossRef]

A. M. Brodnikovskii, V. N. Zadkov, M. G. Karimov, N. I. Koroteev, Opt. Spectrosc. (USSR) 54, 227 (1983).

Appl. Opt. (1)

Chem. Phys. Lett. (4)

M. D. Duncan, P. Oesterlin, F. K. Konig, R. L. Byer, Chem. Phys. Lett. 80, 253 (1981).
[CrossRef]

V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
[CrossRef]

G. J. Rosasco, W. Lempert, W. S. Hurst, A. Fein, Chem. Phys. Lett. 97, 435 (1983).
[CrossRef]

V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
[CrossRef]

Opt. Commun. (1)

A. M. Brodnikovskii, S. M. Gladkov, N. I. Koroteev, Opt. Commun. 40, 312 (1982).
[CrossRef]

Opt. Lett. (1)

Opt. Spectrosc. (USSR) (1)

A. M. Brodnikovskii, V. N. Zadkov, M. G. Karimov, N. I. Koroteev, Opt. Spectrosc. (USSR) 54, 227 (1983).

Phys. Rev. (1)

W. E. Lamb, Phys. Rev. 134, A1429 (1964).
[CrossRef]

Phys. Rev. A (3)

S. A. J. Druet, B. Attal, T. K. Gustafson, J.-P. E. Taran, Phys. Rev. A 18, 1529 (1978).
[CrossRef]

A. D. Wilson-Gordon, R. Klimovsky-Barid, H. Friedmann, Phys. Rev. A 25, 1580 (1982).
[CrossRef]

G. S. Agarwal, S. Singh, Phys. Rev. A 25, 3195 (1982).
[CrossRef]

Phys. Rev. Lett. (1)

L. A. Rahn, R. L. Farrow, M. L. Koszykowski, P. L. Mattern, Phys. Rev. Lett. 45, 620 (1980).
[CrossRef]

Prog. Quantum Electron. (1)

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

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Figures (3)

Fig. 1
Fig. 1

Experimental Q(12) spectra of N2 at 25 Torr (data points) for two different measured Stokes laser intensities (indicated by labels) and a pump laser intensity of ~37 GW/cm2, obtained with scanning CARS. The dip in the higher-intensity peak results from two-photon saturation of the Raman transition as the pump/Stokes frequency difference is scanned across the line. The solid curves are straight lines connecting the data points.

Fig. 2
Fig. 2

Experimental Q(12) spectra of N2 at 100 Torr (data points) illustrating changes in line profile with variations in Stokes intensity. The pump intensity was ~37 GW/cm2, and the Stokes intensities were as labeled. The solid lines are theoretical line shapes, calculated using one third of the measured pump/Stokes field intensity product.

Fig. 3
Fig. 3

Saturation curve measured for the line-center intensity of Q(12) at 100Torr (data points). The CARS signal is normalized by Ip so that the signal would be linearly dependent on IpIS in the absence of saturation. Ip was held nearly constant (~37 GW/cm2) for all measurements. The uncertainty of the data is ±10%, based on the reproducibility of the measurements. The solid line shows calculated CARS intensities plotted with the theoretical IpIS scaled up by a factor of 3 relative to experimental values.

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