Abstract

We report the first two-photon-excited hydrogen-atom fluorescence measurements in flames made to our knowledge. The n = 3 level of the H atom was excited by 205.1-nm radiation generated by Raman shifting a 224-nm beam produced by frequency mixing. Fluorescence was observed at 656.3 nm as a result of radiative decay from n = 3 to n = 2, the Balmer-α transition. A novel technique, photoionization-controlled loss spectroscopy, is proposed to eliminate the quenching dependence of the fluorescence signal.

© 1983 Optical Society of America

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  1. K. Schofield, M. Steinberg, Opt. Eng. 20, 501 (1981).
  2. W. K. Bischel, B. E. Perry, D. R. Crosley, Appl. Opt. 21, 1419 (1982).
    [CrossRef] [PubMed]
  3. M. Alden, H. Edner, P. Grafstrom, S. Svanberg, Opt. Commun. 42, 244 (1982).
    [CrossRef]
  4. T. W. Hänsch, S. A. Lee, R. Wallenstein, C. Wieman, Phys. Rev. Lett. 34, 307 (1975).
    [CrossRef]
  5. J. Bokor, R. R. Freeman, J. C. White, R. H. Storz, Phys. Rev. A 24, 612 (1981).
    [CrossRef]
  6. G. C. Bjorklund, C. P. Ausschnitt, R. R. Freeman, R. H. Storz, Appl. Phys. Lett. 33, 54 (1978).
    [CrossRef]
  7. C. P. Ausschnitt, G. C. Bjorklund, R. R. Freeman, Appl. Phys. Lett. 33, 851 (1978).
    [CrossRef]
  8. J. E. M. Goldsmith, Opt. Lett. 7, 437 (1982).
    [CrossRef] [PubMed]
  9. J. E. M. Goldsmith, J. Chem. Phys. 78, 1610 (1983).
    [CrossRef]
  10. H. A. Bethe, E. E. Salpeter, Quantum Mechanics of One- and Two-Electron Atoms (Academic, New York, 1957).
  11. J. M. Harris, F. E. Lytle, T. C. McCain, Anal. Chem. 48, 2095 (1976).
    [CrossRef]
  12. R. C. Peterson, Ph.D. Thesis (Purdue University, West Lafayette, Indiana, 1981).
  13. R. P. Lucht, D. W. Sweeney, N. M. Laurendeau, Combust. Flame 50, 189 (1983).
    [CrossRef]
  14. W. K. Bischel, J. Bokor, D. J. Kligler, C. K. Rhodes, IEEE J. Quantum Electron. 15, 380 (1979).
    [CrossRef]
  15. D. R. Bates, R. Astron. Soc. Mon. Notes 106, 423 (1946).

1983 (2)

J. E. M. Goldsmith, J. Chem. Phys. 78, 1610 (1983).
[CrossRef]

R. P. Lucht, D. W. Sweeney, N. M. Laurendeau, Combust. Flame 50, 189 (1983).
[CrossRef]

1982 (3)

1981 (2)

J. Bokor, R. R. Freeman, J. C. White, R. H. Storz, Phys. Rev. A 24, 612 (1981).
[CrossRef]

K. Schofield, M. Steinberg, Opt. Eng. 20, 501 (1981).

1979 (1)

W. K. Bischel, J. Bokor, D. J. Kligler, C. K. Rhodes, IEEE J. Quantum Electron. 15, 380 (1979).
[CrossRef]

1978 (2)

G. C. Bjorklund, C. P. Ausschnitt, R. R. Freeman, R. H. Storz, Appl. Phys. Lett. 33, 54 (1978).
[CrossRef]

C. P. Ausschnitt, G. C. Bjorklund, R. R. Freeman, Appl. Phys. Lett. 33, 851 (1978).
[CrossRef]

1976 (1)

J. M. Harris, F. E. Lytle, T. C. McCain, Anal. Chem. 48, 2095 (1976).
[CrossRef]

1975 (1)

T. W. Hänsch, S. A. Lee, R. Wallenstein, C. Wieman, Phys. Rev. Lett. 34, 307 (1975).
[CrossRef]

1946 (1)

D. R. Bates, R. Astron. Soc. Mon. Notes 106, 423 (1946).

Alden, M.

M. Alden, H. Edner, P. Grafstrom, S. Svanberg, Opt. Commun. 42, 244 (1982).
[CrossRef]

Ausschnitt, C. P.

C. P. Ausschnitt, G. C. Bjorklund, R. R. Freeman, Appl. Phys. Lett. 33, 851 (1978).
[CrossRef]

G. C. Bjorklund, C. P. Ausschnitt, R. R. Freeman, R. H. Storz, Appl. Phys. Lett. 33, 54 (1978).
[CrossRef]

Bates, D. R.

D. R. Bates, R. Astron. Soc. Mon. Notes 106, 423 (1946).

Bethe, H. A.

H. A. Bethe, E. E. Salpeter, Quantum Mechanics of One- and Two-Electron Atoms (Academic, New York, 1957).

Bischel, W. K.

W. K. Bischel, B. E. Perry, D. R. Crosley, Appl. Opt. 21, 1419 (1982).
[CrossRef] [PubMed]

W. K. Bischel, J. Bokor, D. J. Kligler, C. K. Rhodes, IEEE J. Quantum Electron. 15, 380 (1979).
[CrossRef]

Bjorklund, G. C.

G. C. Bjorklund, C. P. Ausschnitt, R. R. Freeman, R. H. Storz, Appl. Phys. Lett. 33, 54 (1978).
[CrossRef]

C. P. Ausschnitt, G. C. Bjorklund, R. R. Freeman, Appl. Phys. Lett. 33, 851 (1978).
[CrossRef]

Bokor, J.

J. Bokor, R. R. Freeman, J. C. White, R. H. Storz, Phys. Rev. A 24, 612 (1981).
[CrossRef]

W. K. Bischel, J. Bokor, D. J. Kligler, C. K. Rhodes, IEEE J. Quantum Electron. 15, 380 (1979).
[CrossRef]

Crosley, D. R.

Edner, H.

M. Alden, H. Edner, P. Grafstrom, S. Svanberg, Opt. Commun. 42, 244 (1982).
[CrossRef]

Freeman, R. R.

J. Bokor, R. R. Freeman, J. C. White, R. H. Storz, Phys. Rev. A 24, 612 (1981).
[CrossRef]

C. P. Ausschnitt, G. C. Bjorklund, R. R. Freeman, Appl. Phys. Lett. 33, 851 (1978).
[CrossRef]

G. C. Bjorklund, C. P. Ausschnitt, R. R. Freeman, R. H. Storz, Appl. Phys. Lett. 33, 54 (1978).
[CrossRef]

Goldsmith, J. E. M.

J. E. M. Goldsmith, J. Chem. Phys. 78, 1610 (1983).
[CrossRef]

J. E. M. Goldsmith, Opt. Lett. 7, 437 (1982).
[CrossRef] [PubMed]

Grafstrom, P.

M. Alden, H. Edner, P. Grafstrom, S. Svanberg, Opt. Commun. 42, 244 (1982).
[CrossRef]

Hänsch, T. W.

T. W. Hänsch, S. A. Lee, R. Wallenstein, C. Wieman, Phys. Rev. Lett. 34, 307 (1975).
[CrossRef]

Harris, J. M.

J. M. Harris, F. E. Lytle, T. C. McCain, Anal. Chem. 48, 2095 (1976).
[CrossRef]

Kligler, D. J.

W. K. Bischel, J. Bokor, D. J. Kligler, C. K. Rhodes, IEEE J. Quantum Electron. 15, 380 (1979).
[CrossRef]

Laurendeau, N. M.

R. P. Lucht, D. W. Sweeney, N. M. Laurendeau, Combust. Flame 50, 189 (1983).
[CrossRef]

Lee, S. A.

T. W. Hänsch, S. A. Lee, R. Wallenstein, C. Wieman, Phys. Rev. Lett. 34, 307 (1975).
[CrossRef]

Lucht, R. P.

R. P. Lucht, D. W. Sweeney, N. M. Laurendeau, Combust. Flame 50, 189 (1983).
[CrossRef]

Lytle, F. E.

J. M. Harris, F. E. Lytle, T. C. McCain, Anal. Chem. 48, 2095 (1976).
[CrossRef]

McCain, T. C.

J. M. Harris, F. E. Lytle, T. C. McCain, Anal. Chem. 48, 2095 (1976).
[CrossRef]

Perry, B. E.

Peterson, R. C.

R. C. Peterson, Ph.D. Thesis (Purdue University, West Lafayette, Indiana, 1981).

Rhodes, C. K.

W. K. Bischel, J. Bokor, D. J. Kligler, C. K. Rhodes, IEEE J. Quantum Electron. 15, 380 (1979).
[CrossRef]

Salpeter, E. E.

H. A. Bethe, E. E. Salpeter, Quantum Mechanics of One- and Two-Electron Atoms (Academic, New York, 1957).

Schofield, K.

K. Schofield, M. Steinberg, Opt. Eng. 20, 501 (1981).

Steinberg, M.

K. Schofield, M. Steinberg, Opt. Eng. 20, 501 (1981).

Storz, R. H.

J. Bokor, R. R. Freeman, J. C. White, R. H. Storz, Phys. Rev. A 24, 612 (1981).
[CrossRef]

G. C. Bjorklund, C. P. Ausschnitt, R. R. Freeman, R. H. Storz, Appl. Phys. Lett. 33, 54 (1978).
[CrossRef]

Svanberg, S.

M. Alden, H. Edner, P. Grafstrom, S. Svanberg, Opt. Commun. 42, 244 (1982).
[CrossRef]

Sweeney, D. W.

R. P. Lucht, D. W. Sweeney, N. M. Laurendeau, Combust. Flame 50, 189 (1983).
[CrossRef]

Wallenstein, R.

T. W. Hänsch, S. A. Lee, R. Wallenstein, C. Wieman, Phys. Rev. Lett. 34, 307 (1975).
[CrossRef]

White, J. C.

J. Bokor, R. R. Freeman, J. C. White, R. H. Storz, Phys. Rev. A 24, 612 (1981).
[CrossRef]

Wieman, C.

T. W. Hänsch, S. A. Lee, R. Wallenstein, C. Wieman, Phys. Rev. Lett. 34, 307 (1975).
[CrossRef]

Anal. Chem. (1)

J. M. Harris, F. E. Lytle, T. C. McCain, Anal. Chem. 48, 2095 (1976).
[CrossRef]

Appl. Opt. (1)

Appl. Phys. Lett. (2)

G. C. Bjorklund, C. P. Ausschnitt, R. R. Freeman, R. H. Storz, Appl. Phys. Lett. 33, 54 (1978).
[CrossRef]

C. P. Ausschnitt, G. C. Bjorklund, R. R. Freeman, Appl. Phys. Lett. 33, 851 (1978).
[CrossRef]

Combust. Flame (1)

R. P. Lucht, D. W. Sweeney, N. M. Laurendeau, Combust. Flame 50, 189 (1983).
[CrossRef]

IEEE J. Quantum Electron. (1)

W. K. Bischel, J. Bokor, D. J. Kligler, C. K. Rhodes, IEEE J. Quantum Electron. 15, 380 (1979).
[CrossRef]

J. Chem. Phys. (1)

J. E. M. Goldsmith, J. Chem. Phys. 78, 1610 (1983).
[CrossRef]

Opt. Commun. (1)

M. Alden, H. Edner, P. Grafstrom, S. Svanberg, Opt. Commun. 42, 244 (1982).
[CrossRef]

Opt. Eng. (1)

K. Schofield, M. Steinberg, Opt. Eng. 20, 501 (1981).

Opt. Lett. (1)

Phys. Rev. A (1)

J. Bokor, R. R. Freeman, J. C. White, R. H. Storz, Phys. Rev. A 24, 612 (1981).
[CrossRef]

Phys. Rev. Lett. (1)

T. W. Hänsch, S. A. Lee, R. Wallenstein, C. Wieman, Phys. Rev. Lett. 34, 307 (1975).
[CrossRef]

R. Astron. Soc. Mon. Notes (1)

D. R. Bates, R. Astron. Soc. Mon. Notes 106, 423 (1946).

Other (2)

R. C. Peterson, Ph.D. Thesis (Purdue University, West Lafayette, Indiana, 1981).

H. A. Bethe, E. E. Salpeter, Quantum Mechanics of One- and Two-Electron Atoms (Academic, New York, 1957).

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Figures (5)

Fig. 1
Fig. 1

Energy-level schematic for (a) TPEF and (b) PICLS of the H atom.

Fig. 2
Fig. 2

Experimental system for TPEF measurement of hydrogen: DM, dichroic mirror; FR, full reflector; L, lens (focal length in millimeters); BD, beam dump.

Fig. 3
Fig. 3

Fluorescence intensity at 656.3 nm versus excitation wavelength for the two-photon n = 1 to n = 3 transition in H.

Fig. 4
Fig. 4

Temporal scans of the square of the intensity of the exciting laser pulse at 205 nm (proportional to the two-photon absorption rate) and the resulting fluorescence pulse at 656.3 nm. The H2–O2–Ar flame pressure is 20 Torr, and the equivalence ratio is 1.4.

Fig. 5
Fig. 5

Comparison of H-atom profiles measured by TPEF and profiles calculated by using a one-dimensional computer code.12 The flame pressure and the total mass flow rate are 72 Torr and 0.2 gmol/min, respectively, for all three stoichiometries. The flow-rate ratio N O 2 / ( N O 2 + N Ar ) is 0.21 for all flames. The TPEF profiles are normalized to the calculated results in the stoichiometric flame at 9.0 mm above the burner. For reference purposes the zone of rapid increase in OH concentration and temperature ends at approximately 6 mm above the burner.

Equations (4)

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d N 3 / d t = N 1 W 13 N 3 ( W 3 i + Q 3 + A 3 ) ,
N 3 = N 1 W 13 / W 3 i
W 13 = α I 1 2 / h c ω 1 ,
W 3 i = σ 3 i I 2 / h c ω 2 ,

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