Abstract

The application of Doppler-free two-photon electronic spectroscopy for the in situ monitoring of stratospheric gases has been analyzed. Expressions have been derived for the optimum detection pressure and maximum volumetric sensitivity. The results indicate that detection limits of the order of 105 to 107 molecules/cm3 are feasible for molecular species with strong two-photon uv transitions that undergo efficient radiative relaxation from the excited state. The minimum detectable concentration of trace gas has been plotted vs altitude.

© 1976 Optical Society of America

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References

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  1. F. S. Rowland, M. J. Molina, Rev. Geophys. Space Phys. 13, 1 (1975).
    [CrossRef]
  2. G. B. Lubkin, Phys. Today 28, 34 (Oct.1975).
    [CrossRef]
  3. L. B. Kreuzer, J. Appl. Phys. 42, 2934 (1971).
    [CrossRef]
  4. L. S. Vasilenko, V. P. Chebotaev, A. V. Shishaev, JETP Lett. 12, 133 (1970).
  5. M. P. Levenson, N. Bloembergen, Phys. Rev. Lett. 32, 645 (1974).
    [CrossRef]
  6. F. Biraben, B. Cagnac, G. Grynberg, Phys. Rev. Lett. 32, 643 (1974).
    [CrossRef]
  7. T. W. Hansch, K. Harvey, G. Meisel, A. L. Schawlow, Opt. Commun. 11, 50 (1974).
    [CrossRef]
  8. W. K. Bischel, P. J. Kelley, C. K. Rhodes, Phys. Rev. Lett. 34, 300 (1975).
    [CrossRef]
  9. J. A. Gelbwachs, P. F. Jones, J. E. Wessel, App. Phys. Lett. 27, 551 (1975).
    [CrossRef]
  10. P. L. Kelley, H. Kildal, H. R. Schlossberg, Chem. Phys. Lett. 27, 62 (1974).
    [CrossRef]
  11. S. Valley, Ed., Handbook of Geophysics (MacMillan, New York, 1960), Chap. 1.

1975 (4)

F. S. Rowland, M. J. Molina, Rev. Geophys. Space Phys. 13, 1 (1975).
[CrossRef]

G. B. Lubkin, Phys. Today 28, 34 (Oct.1975).
[CrossRef]

W. K. Bischel, P. J. Kelley, C. K. Rhodes, Phys. Rev. Lett. 34, 300 (1975).
[CrossRef]

J. A. Gelbwachs, P. F. Jones, J. E. Wessel, App. Phys. Lett. 27, 551 (1975).
[CrossRef]

1974 (4)

P. L. Kelley, H. Kildal, H. R. Schlossberg, Chem. Phys. Lett. 27, 62 (1974).
[CrossRef]

M. P. Levenson, N. Bloembergen, Phys. Rev. Lett. 32, 645 (1974).
[CrossRef]

F. Biraben, B. Cagnac, G. Grynberg, Phys. Rev. Lett. 32, 643 (1974).
[CrossRef]

T. W. Hansch, K. Harvey, G. Meisel, A. L. Schawlow, Opt. Commun. 11, 50 (1974).
[CrossRef]

1971 (1)

L. B. Kreuzer, J. Appl. Phys. 42, 2934 (1971).
[CrossRef]

1970 (1)

L. S. Vasilenko, V. P. Chebotaev, A. V. Shishaev, JETP Lett. 12, 133 (1970).

Biraben, F.

F. Biraben, B. Cagnac, G. Grynberg, Phys. Rev. Lett. 32, 643 (1974).
[CrossRef]

Bischel, W. K.

W. K. Bischel, P. J. Kelley, C. K. Rhodes, Phys. Rev. Lett. 34, 300 (1975).
[CrossRef]

Bloembergen, N.

M. P. Levenson, N. Bloembergen, Phys. Rev. Lett. 32, 645 (1974).
[CrossRef]

Cagnac, B.

F. Biraben, B. Cagnac, G. Grynberg, Phys. Rev. Lett. 32, 643 (1974).
[CrossRef]

Chebotaev, V. P.

L. S. Vasilenko, V. P. Chebotaev, A. V. Shishaev, JETP Lett. 12, 133 (1970).

Gelbwachs, J. A.

J. A. Gelbwachs, P. F. Jones, J. E. Wessel, App. Phys. Lett. 27, 551 (1975).
[CrossRef]

Grynberg, G.

F. Biraben, B. Cagnac, G. Grynberg, Phys. Rev. Lett. 32, 643 (1974).
[CrossRef]

Hansch, T. W.

T. W. Hansch, K. Harvey, G. Meisel, A. L. Schawlow, Opt. Commun. 11, 50 (1974).
[CrossRef]

Harvey, K.

T. W. Hansch, K. Harvey, G. Meisel, A. L. Schawlow, Opt. Commun. 11, 50 (1974).
[CrossRef]

Jones, P. F.

J. A. Gelbwachs, P. F. Jones, J. E. Wessel, App. Phys. Lett. 27, 551 (1975).
[CrossRef]

Kelley, P. J.

W. K. Bischel, P. J. Kelley, C. K. Rhodes, Phys. Rev. Lett. 34, 300 (1975).
[CrossRef]

Kelley, P. L.

P. L. Kelley, H. Kildal, H. R. Schlossberg, Chem. Phys. Lett. 27, 62 (1974).
[CrossRef]

Kildal, H.

P. L. Kelley, H. Kildal, H. R. Schlossberg, Chem. Phys. Lett. 27, 62 (1974).
[CrossRef]

Kreuzer, L. B.

L. B. Kreuzer, J. Appl. Phys. 42, 2934 (1971).
[CrossRef]

Levenson, M. P.

M. P. Levenson, N. Bloembergen, Phys. Rev. Lett. 32, 645 (1974).
[CrossRef]

Lubkin, G. B.

G. B. Lubkin, Phys. Today 28, 34 (Oct.1975).
[CrossRef]

Meisel, G.

T. W. Hansch, K. Harvey, G. Meisel, A. L. Schawlow, Opt. Commun. 11, 50 (1974).
[CrossRef]

Molina, M. J.

F. S. Rowland, M. J. Molina, Rev. Geophys. Space Phys. 13, 1 (1975).
[CrossRef]

Rhodes, C. K.

W. K. Bischel, P. J. Kelley, C. K. Rhodes, Phys. Rev. Lett. 34, 300 (1975).
[CrossRef]

Rowland, F. S.

F. S. Rowland, M. J. Molina, Rev. Geophys. Space Phys. 13, 1 (1975).
[CrossRef]

Schawlow, A. L.

T. W. Hansch, K. Harvey, G. Meisel, A. L. Schawlow, Opt. Commun. 11, 50 (1974).
[CrossRef]

Schlossberg, H. R.

P. L. Kelley, H. Kildal, H. R. Schlossberg, Chem. Phys. Lett. 27, 62 (1974).
[CrossRef]

Shishaev, A. V.

L. S. Vasilenko, V. P. Chebotaev, A. V. Shishaev, JETP Lett. 12, 133 (1970).

Vasilenko, L. S.

L. S. Vasilenko, V. P. Chebotaev, A. V. Shishaev, JETP Lett. 12, 133 (1970).

Wessel, J. E.

J. A. Gelbwachs, P. F. Jones, J. E. Wessel, App. Phys. Lett. 27, 551 (1975).
[CrossRef]

App. Phys. Lett. (1)

J. A. Gelbwachs, P. F. Jones, J. E. Wessel, App. Phys. Lett. 27, 551 (1975).
[CrossRef]

Chem. Phys. Lett. (1)

P. L. Kelley, H. Kildal, H. R. Schlossberg, Chem. Phys. Lett. 27, 62 (1974).
[CrossRef]

J. Appl. Phys. (1)

L. B. Kreuzer, J. Appl. Phys. 42, 2934 (1971).
[CrossRef]

JETP Lett. (1)

L. S. Vasilenko, V. P. Chebotaev, A. V. Shishaev, JETP Lett. 12, 133 (1970).

Opt. Commun. (1)

T. W. Hansch, K. Harvey, G. Meisel, A. L. Schawlow, Opt. Commun. 11, 50 (1974).
[CrossRef]

Phys. Rev. Lett. (3)

W. K. Bischel, P. J. Kelley, C. K. Rhodes, Phys. Rev. Lett. 34, 300 (1975).
[CrossRef]

M. P. Levenson, N. Bloembergen, Phys. Rev. Lett. 32, 645 (1974).
[CrossRef]

F. Biraben, B. Cagnac, G. Grynberg, Phys. Rev. Lett. 32, 643 (1974).
[CrossRef]

Phys. Today (1)

G. B. Lubkin, Phys. Today 28, 34 (Oct.1975).
[CrossRef]

Rev. Geophys. Space Phys. (1)

F. S. Rowland, M. J. Molina, Rev. Geophys. Space Phys. 13, 1 (1975).
[CrossRef]

Other (1)

S. Valley, Ed., Handbook of Geophysics (MacMillan, New York, 1960), Chap. 1.

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Figures (2)

Fig. 1
Fig. 1

Experimental configuration for Doppler-free two-photon detection of stratospheric gases.

Fig. 2
Fig. 2

Minimum detectable molecular concentration vs altitude for molecular species with radiative lifetimes of 100 nsec and 1 nsec. The solid curves correspond to detection at ambient pressure. The dashed curve represents the detection limit when the pressure inside the sample cell is maintained at po (see text).

Equations (12)

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β 2 ω β ω = ( μ el E h ν el ) 2 δ ν D γ = I I 0 Δ ν D γ ,
C = β 2 ω n L P t 2 h ν L η f η c ,
C m = t 1 / 2 .
n m = 2 g ν L I 0 ( Δ ν D / γ ) β ω ( L / A ) P 2 t 1 / 2 η f η c ,
L A ~ λ - 1 = ν L c ,
n m = 2 h c I 0 ( Δ ν D / γ ) β ω η f P 2 t 1 / 2 η c .
γ = k 1 p + 1 π τ
η f = τ / τ r 1 + τ k 2 p ,
n m = 2 h c I 0 Δ ν D β ω P 2 t 1 / 2 η c τ r τ ( k 1 p + 1 π τ ) ( 1 + τ k 2 p ) .
S = n m 3.5 × 10 16 p ,
p o = ( 1 π k 1 k 2 τ 2 ) 1 / 2
S m = 2 h c I 0 3.5 × 10 16 π β ω P 2 t 1 / 2 η c Δ ν D τ r τ [ ( π k 1 1 / 2 + k 2 1 / 2 ) ] 2 .

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