Abstract

Various two-photon excitation schemes for laser-induced-fluorescence spectroscopy in atomic hydrogen have been experimentally investigated. The results are compared with one another and with theoretical predictions. A tunable narrow-bandwidth ArF excimer laser (oscillator–amplifier system) in combination with a Raman cell was used as the light source. Atomic hydrogen at room temperature and at densities of ~1014 cm−3 was provided by a flow-tube reactor. Excitation was from the ground state to the excited n = 3 and n = 4 states, and fluorescence light was observed at Balmer-α and -β wavelengths, respectively. Various wavelength combinations [(205 nm × 2) and (193 + 219 nm) for excitation to n = 3 and (193 + 195 nm) for excitation to n = 4], polarizations (linear, circular, and unpolarized), and bandwidths (110, 11, and 0.8 cm −1) were used for the excitation process.

© 1994 Optical Society of America

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  1. J. H. Tung, A. Z. Tang, G. J. Salamo, and F. T. Chan, J. Opt. Soc. Am. B 3, 837 (1986).
    [CrossRef]
  2. W. Lochte-Holtgreven, ed., Plasma Diagnostics (North-Holland, Amsterdam, 1968).
  3. J. E. M. Goldsmith and N. M. Laurendeau, Opt. Lett. 15, 576 (1990).
    [CrossRef] [PubMed]
  4. V. Schultz-von der Gathen, T. Bornemann, and H. F. Döbele, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Füllich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 75.
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    [CrossRef] [PubMed]
  6. W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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  14. U. Czarnetzki, K. Miyazaki, T. Kajiwara, K. Muraoka, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, J. Vac. Sci. Tech. A 12, 831 (1994).
    [CrossRef]
  15. T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

Allen, L.

B. R. Marx, J. Simons, and L. Allen, J. Phys. B 11, L273 (1978).
[CrossRef]

Basting, D.

W. Mückenheim, P. Lokai, B. Burghardt, and D. Basting, Appl. Phys. B 45, 259 (1988).
[CrossRef]

Bornemann, T.

V. Schultz-von der Gathen, T. Bornemann, and H. F. Döbele, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Füllich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 75.

Burghardt, B.

W. Mückenheim, P. Lokai, B. Burghardt, and D. Basting, Appl. Phys. B 45, 259 (1988).
[CrossRef]

Chan, F. T.

J. H. Tung, A. Z. Tang, G. J. Salamo, and F. T. Chan, J. Opt. Soc. Am. B 3, 837 (1986).
[CrossRef]

Czarnetzki, U.

U. Czarnetzki, K. Miyazaki, T. Kajiwara, K. Muraoka, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, J. Vac. Sci. Tech. A 12, 831 (1994).
[CrossRef]

Döbele, H. F.

V. Schultz-von der Gathen, T. Bornemann, and H. F. Döbele, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Füllich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 75.

Gathen, V. Schultz-von der

V. Schultz-von der Gathen, T. Bornemann, and H. F. Döbele, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Füllich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 75.

Glennon, B. M.

W. L. Wiese, M. W. Smith, and B. M. Glennon, Atomic Transition Probabilities, Vol. 1, Natl. Stand. Ref. Data Series, Nat. Bur. Stand. 4 (1966).

Goldsmith, J. E. M.

J. E. M. Goldsmith and N. M. Laurendeau, Opt. Lett. 15, 576 (1990).
[CrossRef] [PubMed]

Heitmann, U.

U. Heitmann, M. Kötteritzsch, S. Heitz, and A. Hesse, Appl. Phys. B 55, 419 (1992).
[CrossRef]

Heitz, S.

U. Heitmann, M. Kötteritzsch, S. Heitz, and A. Hesse, Appl. Phys. B 55, 419 (1992).
[CrossRef]

Hesse, A.

U. Heitmann, M. Kötteritzsch, S. Heitz, and A. Hesse, Appl. Phys. B 55, 419 (1992).
[CrossRef]

Kajiwara, T.

W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
[CrossRef]

U. Czarnetzki, K. Miyazaki, T. Kajiwara, K. Muraoka, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, J. Vac. Sci. Tech. A 12, 831 (1994).
[CrossRef]

T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

Kano, S. S.

M. D. Levenson and S. S. Kano, Introduction to Nonlinear Laser Spectroscopy (Academic, Boston, 1988).

Klages, C.-P.

U. Meier, K. Kohse-Hoinghaus, L. Schäfer, and C.-P. Klages, Appl. Opt. 29, 4993 (1990).
[CrossRef] [PubMed]

Kohse-Hoinghaus, K.

U. Meier, K. Kohse-Hoinghaus, L. Schäfer, and C.-P. Klages, Appl. Opt. 29, 4993 (1990).
[CrossRef] [PubMed]

Kötteritzsch, M.

U. Heitmann, M. Kötteritzsch, S. Heitz, and A. Hesse, Appl. Phys. B 55, 419 (1992).
[CrossRef]

Laurendeau, N. M.

J. E. M. Goldsmith and N. M. Laurendeau, Opt. Lett. 15, 576 (1990).
[CrossRef] [PubMed]

Levenson, M. D.

M. D. Levenson and S. S. Kano, Introduction to Nonlinear Laser Spectroscopy (Academic, Boston, 1988).

Lokai, P.

W. Mückenheim, P. Lokai, B. Burghardt, and D. Basting, Appl. Phys. B 45, 259 (1988).
[CrossRef]

Loudon, R.

R. Loudon, The Quantum Theory of Light (Clarendon, Oxford, 1973).

Maeda, M.

W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
[CrossRef]

T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

U. Czarnetzki, K. Miyazaki, T. Kajiwara, K. Muraoka, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, J. Vac. Sci. Tech. A 12, 831 (1994).
[CrossRef]

Marx, B. R.

B. R. Marx, J. Simons, and L. Allen, J. Phys. B 11, L273 (1978).
[CrossRef]

Masuda, M.

W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
[CrossRef]

T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

Matsuda, A.

U. Czarnetzki, K. Miyazaki, T. Kajiwara, K. Muraoka, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, J. Vac. Sci. Tech. A 12, 831 (1994).
[CrossRef]

W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
[CrossRef]

Meier, U.

U. Meier, K. Kohse-Hoinghaus, L. Schäfer, and C.-P. Klages, Appl. Opt. 29, 4993 (1990).
[CrossRef] [PubMed]

Miyazaki, K.

U. Czarnetzki, K. Miyazaki, T. Kajiwara, K. Muraoka, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, J. Vac. Sci. Tech. A 12, 831 (1994).
[CrossRef]

Mückenheim, W.

W. Mückenheim, P. Lokai, B. Burghardt, and D. Basting, Appl. Phys. B 45, 259 (1988).
[CrossRef]

Muraoka, K.

W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
[CrossRef]

U. Czarnetzki, K. Miyazaki, T. Kajiwara, K. Muraoka, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, J. Vac. Sci. Tech. A 12, 831 (1994).
[CrossRef]

T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

Obiki, T.

T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

Okada, T.

T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

U. Czarnetzki, K. Miyazaki, T. Kajiwara, K. Muraoka, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, J. Vac. Sci. Tech. A 12, 831 (1994).
[CrossRef]

W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
[CrossRef]

Park, W. Z.

W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
[CrossRef]

Salamo, G. J.

J. H. Tung, A. Z. Tang, G. J. Salamo, and F. T. Chan, J. Opt. Soc. Am. B 3, 837 (1986).
[CrossRef]

Schäfer, L.

U. Meier, K. Kohse-Hoinghaus, L. Schäfer, and C.-P. Klages, Appl. Opt. 29, 4993 (1990).
[CrossRef] [PubMed]

Setser, D. W.

D. W. Setser, Reactive Intermediates in the Gas Phase (Academic, New York, 1979).

Shinkawa, T.

T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

Simons, J.

B. R. Marx, J. Simons, and L. Allen, J. Phys. B 11, L273 (1978).
[CrossRef]

Smith, M. W.

W. L. Wiese, M. W. Smith, and B. M. Glennon, Atomic Transition Probabilities, Vol. 1, Natl. Stand. Ref. Data Series, Nat. Bur. Stand. 4 (1966).

Suzuki, A.

W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
[CrossRef]

U. Czarnetzki, K. Miyazaki, T. Kajiwara, K. Muraoka, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, J. Vac. Sci. Tech. A 12, 831 (1994).
[CrossRef]

Tang, A. Z.

J. H. Tung, A. Z. Tang, G. J. Salamo, and F. T. Chan, J. Opt. Soc. Am. B 3, 837 (1986).
[CrossRef]

Tanigawa, M.

W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
[CrossRef]

Tung, J. H.

J. H. Tung, A. Z. Tang, G. J. Salamo, and F. T. Chan, J. Opt. Soc. Am. B 3, 837 (1986).
[CrossRef]

Uchino, K.

T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

Udo, S.

T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

Wiese, W. L.

W. L. Wiese, M. W. Smith, and B. M. Glennon, Atomic Transition Probabilities, Vol. 1, Natl. Stand. Ref. Data Series, Nat. Bur. Stand. 4 (1966).

Other

J. H. Tung, A. Z. Tang, G. J. Salamo, and F. T. Chan, J. Opt. Soc. Am. B 3, 837 (1986).
[CrossRef]

W. Lochte-Holtgreven, ed., Plasma Diagnostics (North-Holland, Amsterdam, 1968).

J. E. M. Goldsmith and N. M. Laurendeau, Opt. Lett. 15, 576 (1990).
[CrossRef] [PubMed]

V. Schultz-von der Gathen, T. Bornemann, and H. F. Döbele, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Füllich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 75.

U. Meier, K. Kohse-Hoinghaus, L. Schäfer, and C.-P. Klages, Appl. Opt. 29, 4993 (1990).
[CrossRef] [PubMed]

W. Z. Park, M. Tanigawa, T. Kajiwara, K. Muraoka, M. Masuda, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, Jpn. J. Appl. Phys. 31, 2917 (1992).
[CrossRef]

W. Mückenheim, P. Lokai, B. Burghardt, and D. Basting, Appl. Phys. B 45, 259 (1988).
[CrossRef]

U. Heitmann, M. Kötteritzsch, S. Heitz, and A. Hesse, Appl. Phys. B 55, 419 (1992).
[CrossRef]

R. Loudon, The Quantum Theory of Light (Clarendon, Oxford, 1973).

M. D. Levenson and S. S. Kano, Introduction to Nonlinear Laser Spectroscopy (Academic, Boston, 1988).

B. R. Marx, J. Simons, and L. Allen, J. Phys. B 11, L273 (1978).
[CrossRef]

W. L. Wiese, M. W. Smith, and B. M. Glennon, Atomic Transition Probabilities, Vol. 1, Natl. Stand. Ref. Data Series, Nat. Bur. Stand. 4 (1966).

D. W. Setser, Reactive Intermediates in the Gas Phase (Academic, New York, 1979).

U. Czarnetzki, K. Miyazaki, T. Kajiwara, K. Muraoka, T. Okada, M. Maeda, A. Suzuki, and A. Matsuda, J. Vac. Sci. Tech. A 12, 831 (1994).
[CrossRef]

T. Kajiwara, T. Shinkawa, K. Uchino, M. Masuda, K. Muraoka, T. Okada, M. Maeda, S. Udo, and T. Obiki, in Proceedings of the Fifth International Symposium on Laser-Aided Plasma Diagnostics, Vol. 9 of Konferenzen des Forschunpzentrums Fülich (Forschunpzentrum Fülich GmbH, Bad Honnef, Germany, 1977), p. 59.

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Figures (4)

Fig. 1
Fig. 1

Simplified energy-level diagrams of atomic hydrogen and different excitation schemes and related fluorescence transitions. For better visibility the Lyman-α emission channel is shown only in diagram a. The schemes investigated in this paper are shown in diagrams c and d.

Fig. 2
Fig. 2

Calculated average number of photons emitted per atom as a function of the laser intensity. For details of the different schemes, see Table 4.

Fig. 3
Fig. 3

(a) Measured detection sensitivity S. (b) Energy-normalized sensitivity S0. The value of S0 for scheme 5 is 3.4 × 10−14 mV cm3 mJ−2. For details of the different schemes, see Table 4. In scheme 6, the detection was at the Balmer-β wavelength.

Fig. 4
Fig. 4

Comparison of the experimental data for the normalized sensitivity with calculations and interpolation to higher temperatures. All sensitivities are normalized to the case of two-photon excitation at 205 nm with 11-cm−1 bandwidth radiation (scheme 1). A typical error bar is shown in (b). For details of the different schemes, see Table 4.

Tables (4)

Tables Icon

Table 1 Calculated Two-Photon Absorption Cross Section Divided by the Spectral Linewidth Function and the Two-Photon Statistical Factora

Tables Icon

Table 2 Polarization Factors for Two-Photon Absorption of Two Independent Beams

Tables Icon

Table 3 Polarization Factors for Two-Photon Absorption of a Single Chaotic Light Beam

Tables Icon

Table 4 Excitation Schemes Investigated and Important Parameters of the Exciting Radiationa

Equations (7)

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

M = n ( f r e 2 n n r e 1 i ω n i - ω 1 + f r e 1 n n r e 2 i ω n i - ω 2 ) .
M = n f re n n re i ω n i - ω .
σ 2 γ = ( ω 1 ω 2 ) 1 / 2 π e 4 2 c 2 0 2 3 M 2 g ( Δ Ω ) G .
g ( Δ Ω = 0 ) = [ 4 ln ( 2 ) π ] 1 / 2 1 ( Δ ω D 2 + Δ ω 1 2 + Δ ω 2 2 ) 1 / 2 .
N ˙ * = N σ 2 γ ( ω 1 ω 2 ) 1 / 2 I 1 I 2 .
I 2 = G I 2 .
S = S FL / N ,             S 0 = S / E 2 .

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