Abstract

Using a powerful, excimer-laser-pumped broadband coherent anti-Stokes Raman scattering (CARS) system, we have observed considerable changes in the populations of room-temperature nitrogen under atmospheric pressure. Pump-induced populations in the first, second, and third vibronic bands of N2 at room temperature resulted in an apparent vibrational temperature of 2550 K. The implications for broadband N2 CARS thermometry are discussed.

© 1987 Optical Society of America

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References

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  1. P. D. Maker, R. W. Terhune, Phys. Rev. 137, 801 (1965).
    [CrossRef]
  2. J. W. Nibler, J. R. McDonald, A. B. Harvey, Opt. Commun. 18, 371 (1976).
    [CrossRef]
  3. R. J. Hall, A. C. Eckbreth, in Laser Applications, J. F. Ready, R. K. Erf, eds. (Academic, New York, 1984), Vol. 5.
  4. I. L. Shumay, V. N. Zadkov, D. J. Heinzen, M. M. Kash, M. S. Feld, Opt. Lett. 11, 233 (1986).
    [CrossRef] [PubMed]
  5. V. N. Zadkov, N. I. Koroteev, M. V. Rychov, A. B. Feodorov, Appl. Phys. B 34, 167 (1984).
    [CrossRef]
  6. M. D. Duncan, P. Oesterlin, F. König, R. L. Byer, Chem. Phys. Lett. 80, 253 (1981).
    [CrossRef]
  7. A. Owyoung, P. Esherick, Opt. Lett. 5, 421 (1980).
    [CrossRef] [PubMed]
  8. M. Sparks, Phys. Rev. Lett. 32, 450 (1974).
    [CrossRef]
  9. W. B. Roh, P. W. Schreiber, J. P. E. Taran, Appl. Phys. Lett. 29, 174 (1976).
    [CrossRef]
  10. G. Marowsky, A. Gierulski, B. Dick, U. Sowada, R. Vehrenkamp, Appl. Phys. B 39, 47 (1986).
    [CrossRef]
  11. B. Dick, A. Gierulski, Appl. Phys. B 40, 1 (1986).
    [CrossRef]
  12. A. Slenczka, diploma thesis (University of Göttingen, Göttingen, Federal Republic of Germany, 1987).
  13. A. Gierulski, A. Slenczka, presented at the EICOLS Conference, Aare, Sweden, June 1987.
  14. G. Herzberg, Molecular Spectra and Molecular Structure. I. Spectra of Diatomic Molecules (Van Nostrand Reinhold, New York, 1950).
  15. T. Dreier, U. Wellhausen, J. Wolfrum, G. Marowsky, Appl. Phys. B 29, 31 (1982).
    [CrossRef]
  16. D. R. Snelling, R. A. Sawchuk, R. E. Mueller, Appl. Opt. 24, 2771 (1985).
    [CrossRef] [PubMed]
  17. A. Leipertz, Habilitation thesis (University of Bochum, Bochum, Federal Republic of Germany, 1982)
  18. D. C. Hanna, M. A. Yuratich, D. Cotter, Nonlinear Optics of Free Atoms and Molecules (Springer-Verlag, Berlin, 1979).
  19. V. N. Zadkov, N. I. Koroteev, Chem. Phys. Lett. 105, 108 (1984).
    [CrossRef]
  20. W. M. Tolles, J. W. Nibler, J. R. McDonald, A. B. Harvey, Appl. Spectrosc. 31, 253 (1977).
    [CrossRef]
  21. A. D. Wilson-Gordon, H. Friedmann, Chem. Phys. Lett. 89, 273 (1982).
    [CrossRef]
  22. Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), Chap. 10, p. 141.

1986 (3)

I. L. Shumay, V. N. Zadkov, D. J. Heinzen, M. M. Kash, M. S. Feld, Opt. Lett. 11, 233 (1986).
[CrossRef] [PubMed]

G. Marowsky, A. Gierulski, B. Dick, U. Sowada, R. Vehrenkamp, Appl. Phys. B 39, 47 (1986).
[CrossRef]

B. Dick, A. Gierulski, Appl. Phys. B 40, 1 (1986).
[CrossRef]

1985 (1)

1984 (2)

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

V. N. Zadkov, N. I. Koroteev, M. V. Rychov, A. B. Feodorov, Appl. Phys. B 34, 167 (1984).
[CrossRef]

1982 (2)

T. Dreier, U. Wellhausen, J. Wolfrum, G. Marowsky, Appl. Phys. B 29, 31 (1982).
[CrossRef]

A. D. Wilson-Gordon, H. Friedmann, Chem. Phys. Lett. 89, 273 (1982).
[CrossRef]

1981 (1)

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

1980 (1)

1977 (1)

1976 (2)

W. B. Roh, P. W. Schreiber, J. P. E. Taran, Appl. Phys. Lett. 29, 174 (1976).
[CrossRef]

J. W. Nibler, J. R. McDonald, A. B. Harvey, Opt. Commun. 18, 371 (1976).
[CrossRef]

1974 (1)

M. Sparks, Phys. Rev. Lett. 32, 450 (1974).
[CrossRef]

1965 (1)

P. D. Maker, R. W. Terhune, Phys. Rev. 137, 801 (1965).
[CrossRef]

Byer, R. L.

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

Cotter, D.

D. C. Hanna, M. A. Yuratich, D. Cotter, Nonlinear Optics of Free Atoms and Molecules (Springer-Verlag, Berlin, 1979).

Dick, B.

G. Marowsky, A. Gierulski, B. Dick, U. Sowada, R. Vehrenkamp, Appl. Phys. B 39, 47 (1986).
[CrossRef]

B. Dick, A. Gierulski, Appl. Phys. B 40, 1 (1986).
[CrossRef]

Dreier, T.

T. Dreier, U. Wellhausen, J. Wolfrum, G. Marowsky, Appl. Phys. B 29, 31 (1982).
[CrossRef]

Duncan, M. D.

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

Eckbreth, A. C.

R. J. Hall, A. C. Eckbreth, in Laser Applications, J. F. Ready, R. K. Erf, eds. (Academic, New York, 1984), Vol. 5.

Esherick, P.

Feld, M. S.

Feodorov, A. B.

V. N. Zadkov, N. I. Koroteev, M. V. Rychov, A. B. Feodorov, Appl. Phys. B 34, 167 (1984).
[CrossRef]

Friedmann, H.

A. D. Wilson-Gordon, H. Friedmann, Chem. Phys. Lett. 89, 273 (1982).
[CrossRef]

Gierulski, A.

B. Dick, A. Gierulski, Appl. Phys. B 40, 1 (1986).
[CrossRef]

G. Marowsky, A. Gierulski, B. Dick, U. Sowada, R. Vehrenkamp, Appl. Phys. B 39, 47 (1986).
[CrossRef]

A. Gierulski, A. Slenczka, presented at the EICOLS Conference, Aare, Sweden, June 1987.

Hall, R. J.

R. J. Hall, A. C. Eckbreth, in Laser Applications, J. F. Ready, R. K. Erf, eds. (Academic, New York, 1984), Vol. 5.

Hanna, D. C.

D. C. Hanna, M. A. Yuratich, D. Cotter, Nonlinear Optics of Free Atoms and Molecules (Springer-Verlag, Berlin, 1979).

Harvey, A. B.

W. M. Tolles, J. W. Nibler, J. R. McDonald, A. B. Harvey, Appl. Spectrosc. 31, 253 (1977).
[CrossRef]

J. W. Nibler, J. R. McDonald, A. B. Harvey, Opt. Commun. 18, 371 (1976).
[CrossRef]

Heinzen, D. J.

Herzberg, G.

G. Herzberg, Molecular Spectra and Molecular Structure. I. Spectra of Diatomic Molecules (Van Nostrand Reinhold, New York, 1950).

Kash, M. M.

König, F.

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

Koroteev, N. I.

V. N. Zadkov, N. I. Koroteev, M. V. Rychov, A. B. Feodorov, Appl. Phys. B 34, 167 (1984).
[CrossRef]

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

Leipertz, A.

A. Leipertz, Habilitation thesis (University of Bochum, Bochum, Federal Republic of Germany, 1982)

Maker, P. D.

P. D. Maker, R. W. Terhune, Phys. Rev. 137, 801 (1965).
[CrossRef]

Marowsky, G.

G. Marowsky, A. Gierulski, B. Dick, U. Sowada, R. Vehrenkamp, Appl. Phys. B 39, 47 (1986).
[CrossRef]

T. Dreier, U. Wellhausen, J. Wolfrum, G. Marowsky, Appl. Phys. B 29, 31 (1982).
[CrossRef]

McDonald, J. R.

W. M. Tolles, J. W. Nibler, J. R. McDonald, A. B. Harvey, Appl. Spectrosc. 31, 253 (1977).
[CrossRef]

J. W. Nibler, J. R. McDonald, A. B. Harvey, Opt. Commun. 18, 371 (1976).
[CrossRef]

Mueller, R. E.

Nibler, J. W.

W. M. Tolles, J. W. Nibler, J. R. McDonald, A. B. Harvey, Appl. Spectrosc. 31, 253 (1977).
[CrossRef]

J. W. Nibler, J. R. McDonald, A. B. Harvey, Opt. Commun. 18, 371 (1976).
[CrossRef]

Oesterlin, P.

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

Owyoung, A.

Roh, W. B.

W. B. Roh, P. W. Schreiber, J. P. E. Taran, Appl. Phys. Lett. 29, 174 (1976).
[CrossRef]

Rychov, M. V.

V. N. Zadkov, N. I. Koroteev, M. V. Rychov, A. B. Feodorov, Appl. Phys. B 34, 167 (1984).
[CrossRef]

Sawchuk, R. A.

Schreiber, P. W.

W. B. Roh, P. W. Schreiber, J. P. E. Taran, Appl. Phys. Lett. 29, 174 (1976).
[CrossRef]

Shen, Y. R.

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), Chap. 10, p. 141.

Shumay, I. L.

Slenczka, A.

A. Slenczka, diploma thesis (University of Göttingen, Göttingen, Federal Republic of Germany, 1987).

A. Gierulski, A. Slenczka, presented at the EICOLS Conference, Aare, Sweden, June 1987.

Snelling, D. R.

Sowada, U.

G. Marowsky, A. Gierulski, B. Dick, U. Sowada, R. Vehrenkamp, Appl. Phys. B 39, 47 (1986).
[CrossRef]

Sparks, M.

M. Sparks, Phys. Rev. Lett. 32, 450 (1974).
[CrossRef]

Taran, J. P. E.

W. B. Roh, P. W. Schreiber, J. P. E. Taran, Appl. Phys. Lett. 29, 174 (1976).
[CrossRef]

Terhune, R. W.

P. D. Maker, R. W. Terhune, Phys. Rev. 137, 801 (1965).
[CrossRef]

Tolles, W. M.

Vehrenkamp, R.

G. Marowsky, A. Gierulski, B. Dick, U. Sowada, R. Vehrenkamp, Appl. Phys. B 39, 47 (1986).
[CrossRef]

Wellhausen, U.

T. Dreier, U. Wellhausen, J. Wolfrum, G. Marowsky, Appl. Phys. B 29, 31 (1982).
[CrossRef]

Wilson-Gordon, A. D.

A. D. Wilson-Gordon, H. Friedmann, Chem. Phys. Lett. 89, 273 (1982).
[CrossRef]

Wolfrum, J.

T. Dreier, U. Wellhausen, J. Wolfrum, G. Marowsky, Appl. Phys. B 29, 31 (1982).
[CrossRef]

Yuratich, M. A.

D. C. Hanna, M. A. Yuratich, D. Cotter, Nonlinear Optics of Free Atoms and Molecules (Springer-Verlag, Berlin, 1979).

Zadkov, V. N.

I. L. Shumay, V. N. Zadkov, D. J. Heinzen, M. M. Kash, M. S. Feld, Opt. Lett. 11, 233 (1986).
[CrossRef] [PubMed]

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

V. N. Zadkov, N. I. Koroteev, M. V. Rychov, A. B. Feodorov, Appl. Phys. B 34, 167 (1984).
[CrossRef]

Appl. Opt. (1)

Appl. Phys. B (4)

T. Dreier, U. Wellhausen, J. Wolfrum, G. Marowsky, Appl. Phys. B 29, 31 (1982).
[CrossRef]

G. Marowsky, A. Gierulski, B. Dick, U. Sowada, R. Vehrenkamp, Appl. Phys. B 39, 47 (1986).
[CrossRef]

B. Dick, A. Gierulski, Appl. Phys. B 40, 1 (1986).
[CrossRef]

V. N. Zadkov, N. I. Koroteev, M. V. Rychov, A. B. Feodorov, Appl. Phys. B 34, 167 (1984).
[CrossRef]

Appl. Phys. Lett. (1)

W. B. Roh, P. W. Schreiber, J. P. E. Taran, Appl. Phys. Lett. 29, 174 (1976).
[CrossRef]

Appl. Spectrosc. (1)

Chem. Phys. Lett. (3)

A. D. Wilson-Gordon, H. Friedmann, Chem. Phys. Lett. 89, 273 (1982).
[CrossRef]

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

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

Opt. Commun. (1)

J. W. Nibler, J. R. McDonald, A. B. Harvey, Opt. Commun. 18, 371 (1976).
[CrossRef]

Opt. Lett. (2)

Phys. Rev. (1)

P. D. Maker, R. W. Terhune, Phys. Rev. 137, 801 (1965).
[CrossRef]

Phys. Rev. Lett. (1)

M. Sparks, Phys. Rev. Lett. 32, 450 (1974).
[CrossRef]

Other (7)

R. J. Hall, A. C. Eckbreth, in Laser Applications, J. F. Ready, R. K. Erf, eds. (Academic, New York, 1984), Vol. 5.

A. Leipertz, Habilitation thesis (University of Bochum, Bochum, Federal Republic of Germany, 1982)

D. C. Hanna, M. A. Yuratich, D. Cotter, Nonlinear Optics of Free Atoms and Molecules (Springer-Verlag, Berlin, 1979).

A. Slenczka, diploma thesis (University of Göttingen, Göttingen, Federal Republic of Germany, 1987).

A. Gierulski, A. Slenczka, presented at the EICOLS Conference, Aare, Sweden, June 1987.

G. Herzberg, Molecular Spectra and Molecular Structure. I. Spectra of Diatomic Molecules (Van Nostrand Reinhold, New York, 1950).

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), Chap. 10, p. 141.

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Figures (2)

Fig. 1
Fig. 1

CARS spectra of atmospheric N2 obtained with the pump- and Stokes-laser power densities indicated. At the high input power density (lower figure) the population of higher vibronic states is clearly visible. For clarity the spectra have been enlarged by factors of 10 and 4, respectively.

Fig. 2
Fig. 2

Square root of the N2 CARS signal from υ = 0 versus pump-laser intensity. The solid symbols denote the measured data points, the open circles the corrected experimental points according to the theory outlined in the text. Typical experimental error bars are shown. The good agreement with the expected I CARS dependence has been obtained by correcting the visual fit to the experimental points according to Eq. (5).

Equations (6)

Equations on this page are rendered with MathJax. Learn more.

I CARS = A ( Δ N ) 2 I p 2 I s ,
d ( Δ N ) / d t = ( Δ N ) a ( Δ N ) / τ 2 ,
n 2 ( t ) = a / 2 b [ 1 exp ( b t ) ] .
n ̅ 2 ( τ p ) = 1 / τ p 0 τ p n 2 ( t ) d t
n ̅ 2 ( τ p ) = a 2 ( a + 1 / τ 2 ) { 1 + exp [ τ p ( a + 1 / τ 2 ) ] 1 τ p ( a + 1 / τ 2 ) } ,
30 GW / cm 2 I p 110 GW / cm 2 .

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