Abstract

We report the preliminary results of our experiments with stimulated Raman scattering in para-hydrogen crystal aimed at developing a continuously tunable laboratory laser source of mid-infrared radiation. With laser pulses at 532 nm, a conversion efficiency for the first Stokes beam of as much as 20% in the forward direction was observed through a single-pass, 5-cm-long crystal. Generation of mid-infrared pulses at 4.5 µm was achieved by use of the output of a near-infrared pulsed laser (1.6 µm, 3 ns), and an absorption spectrum of gaseous CD4 molecules was successfully recorded. These results suggest use of the solid para-hydrogen Raman shifter as a promising light source for mid-infrared spectroscopy.

© 2003 Optical Society of America

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References

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  1. For example, R. Casaes, R. Provençal, J. Paul, and R. J. Saykally, J. Chem. Phys. 116, 6640 (2002).
  2. E. J. Woodbury and W. K. Ng, Proc. IRE 50, 2367 (1962).
  3. J. Cahen, M. Clerc, and P. Rigny, Opt. Commun. 21, 387 (1977).
    [CrossRef]
  4. N. Bloembergen, Nonlinear Optics (Benjamin, New York, 1965).
  5. G. Eckhardt, R. W. Hellwarth, F. J. McClung, S. E. Schwarz, D. Weiner, and E. J. Woodbury, Phys. Rev. Lett. 9, 455 (1962).
    [CrossRef]
  6. B. P. Stoicheff, in Proceedings of the International School of Physics, Enrico Fermi, Course XXXI, C. H. Townes and P. A. Miles, eds. (Academic, New York, 1963), pp. 306–325.
  7. W. R. Trutna and R. L. Byer, Appl. Opt. 19, 301 (1980).
    [CrossRef] [PubMed]
  8. R. Sussmann, Th. Weber, E. Riedle, and H. J. Neusser, Opt. Commun. 88, 408 (1992).
    [CrossRef]
  9. T. Momose, D. P. Weliky, and T. Oka, J. Mol. Spectrosc. 153, 760 (1992).
    [CrossRef]
  10. M. Katsuragawa and K. Hakuta, Opt. Lett. 25, 177 (2000).
    [CrossRef]
  11. S. Y. Lee, “Infrared studies on solid hydrogen, deuterium and hydrogen–deuteride using Fourier-transform spectroscopy,” Ph.D. dissertation (Ohio State University, Columbus, Ohio, 1987).
  12. T. Momose and T. Shida, Bull. Chem. Soc. Jpn. 71, 1 (1998).
    [CrossRef]
  13. D. P. Weliky, K. E. Kerr, T. J. Byers, Y. Zhang, T. Momose, and T. Oka, J. Chem. Phys. 105, 4461 (1996).
  14. B. J. McCall, A. J. Huneycutt, R. J. Saykally, C. M. Lindsay, T. Oka, M. Fushitani, Y. Miyamoto, and T. Momose are preparing a manuscript, “Stimulated Stokes downconversion in liquid and solid parahydrogen,” to be submitted to Appl. Phys.

2002 (1)

For example, R. Casaes, R. Provençal, J. Paul, and R. J. Saykally, J. Chem. Phys. 116, 6640 (2002).

2000 (1)

1998 (1)

T. Momose and T. Shida, Bull. Chem. Soc. Jpn. 71, 1 (1998).
[CrossRef]

1996 (1)

D. P. Weliky, K. E. Kerr, T. J. Byers, Y. Zhang, T. Momose, and T. Oka, J. Chem. Phys. 105, 4461 (1996).

1992 (2)

R. Sussmann, Th. Weber, E. Riedle, and H. J. Neusser, Opt. Commun. 88, 408 (1992).
[CrossRef]

T. Momose, D. P. Weliky, and T. Oka, J. Mol. Spectrosc. 153, 760 (1992).
[CrossRef]

1980 (1)

1977 (1)

J. Cahen, M. Clerc, and P. Rigny, Opt. Commun. 21, 387 (1977).
[CrossRef]

1962 (2)

G. Eckhardt, R. W. Hellwarth, F. J. McClung, S. E. Schwarz, D. Weiner, and E. J. Woodbury, Phys. Rev. Lett. 9, 455 (1962).
[CrossRef]

E. J. Woodbury and W. K. Ng, Proc. IRE 50, 2367 (1962).

Bloembergen, N.

N. Bloembergen, Nonlinear Optics (Benjamin, New York, 1965).

Byer, R. L.

Byers, T. J.

D. P. Weliky, K. E. Kerr, T. J. Byers, Y. Zhang, T. Momose, and T. Oka, J. Chem. Phys. 105, 4461 (1996).

Cahen, J.

J. Cahen, M. Clerc, and P. Rigny, Opt. Commun. 21, 387 (1977).
[CrossRef]

Casaes, R.

For example, R. Casaes, R. Provençal, J. Paul, and R. J. Saykally, J. Chem. Phys. 116, 6640 (2002).

Clerc, M.

J. Cahen, M. Clerc, and P. Rigny, Opt. Commun. 21, 387 (1977).
[CrossRef]

Eckhardt, G.

G. Eckhardt, R. W. Hellwarth, F. J. McClung, S. E. Schwarz, D. Weiner, and E. J. Woodbury, Phys. Rev. Lett. 9, 455 (1962).
[CrossRef]

Fushitani, M.

B. J. McCall, A. J. Huneycutt, R. J. Saykally, C. M. Lindsay, T. Oka, M. Fushitani, Y. Miyamoto, and T. Momose are preparing a manuscript, “Stimulated Stokes downconversion in liquid and solid parahydrogen,” to be submitted to Appl. Phys.

Hakuta, K.

Hellwarth, R. W.

G. Eckhardt, R. W. Hellwarth, F. J. McClung, S. E. Schwarz, D. Weiner, and E. J. Woodbury, Phys. Rev. Lett. 9, 455 (1962).
[CrossRef]

Huneycutt, A. J.

B. J. McCall, A. J. Huneycutt, R. J. Saykally, C. M. Lindsay, T. Oka, M. Fushitani, Y. Miyamoto, and T. Momose are preparing a manuscript, “Stimulated Stokes downconversion in liquid and solid parahydrogen,” to be submitted to Appl. Phys.

Katsuragawa, M.

Kerr, K. E.

D. P. Weliky, K. E. Kerr, T. J. Byers, Y. Zhang, T. Momose, and T. Oka, J. Chem. Phys. 105, 4461 (1996).

Lee, S. Y.

S. Y. Lee, “Infrared studies on solid hydrogen, deuterium and hydrogen–deuteride using Fourier-transform spectroscopy,” Ph.D. dissertation (Ohio State University, Columbus, Ohio, 1987).

Lindsay, C. M.

B. J. McCall, A. J. Huneycutt, R. J. Saykally, C. M. Lindsay, T. Oka, M. Fushitani, Y. Miyamoto, and T. Momose are preparing a manuscript, “Stimulated Stokes downconversion in liquid and solid parahydrogen,” to be submitted to Appl. Phys.

McCall, B. J.

B. J. McCall, A. J. Huneycutt, R. J. Saykally, C. M. Lindsay, T. Oka, M. Fushitani, Y. Miyamoto, and T. Momose are preparing a manuscript, “Stimulated Stokes downconversion in liquid and solid parahydrogen,” to be submitted to Appl. Phys.

McClung, F. J.

G. Eckhardt, R. W. Hellwarth, F. J. McClung, S. E. Schwarz, D. Weiner, and E. J. Woodbury, Phys. Rev. Lett. 9, 455 (1962).
[CrossRef]

Miyamoto, Y.

B. J. McCall, A. J. Huneycutt, R. J. Saykally, C. M. Lindsay, T. Oka, M. Fushitani, Y. Miyamoto, and T. Momose are preparing a manuscript, “Stimulated Stokes downconversion in liquid and solid parahydrogen,” to be submitted to Appl. Phys.

Momose, T.

T. Momose and T. Shida, Bull. Chem. Soc. Jpn. 71, 1 (1998).
[CrossRef]

D. P. Weliky, K. E. Kerr, T. J. Byers, Y. Zhang, T. Momose, and T. Oka, J. Chem. Phys. 105, 4461 (1996).

T. Momose, D. P. Weliky, and T. Oka, J. Mol. Spectrosc. 153, 760 (1992).
[CrossRef]

B. J. McCall, A. J. Huneycutt, R. J. Saykally, C. M. Lindsay, T. Oka, M. Fushitani, Y. Miyamoto, and T. Momose are preparing a manuscript, “Stimulated Stokes downconversion in liquid and solid parahydrogen,” to be submitted to Appl. Phys.

Neusser, H. J.

R. Sussmann, Th. Weber, E. Riedle, and H. J. Neusser, Opt. Commun. 88, 408 (1992).
[CrossRef]

Ng, W. K.

E. J. Woodbury and W. K. Ng, Proc. IRE 50, 2367 (1962).

Oka, T.

D. P. Weliky, K. E. Kerr, T. J. Byers, Y. Zhang, T. Momose, and T. Oka, J. Chem. Phys. 105, 4461 (1996).

T. Momose, D. P. Weliky, and T. Oka, J. Mol. Spectrosc. 153, 760 (1992).
[CrossRef]

B. J. McCall, A. J. Huneycutt, R. J. Saykally, C. M. Lindsay, T. Oka, M. Fushitani, Y. Miyamoto, and T. Momose are preparing a manuscript, “Stimulated Stokes downconversion in liquid and solid parahydrogen,” to be submitted to Appl. Phys.

Paul, J.

For example, R. Casaes, R. Provençal, J. Paul, and R. J. Saykally, J. Chem. Phys. 116, 6640 (2002).

Provençal, R.

For example, R. Casaes, R. Provençal, J. Paul, and R. J. Saykally, J. Chem. Phys. 116, 6640 (2002).

Riedle, E.

R. Sussmann, Th. Weber, E. Riedle, and H. J. Neusser, Opt. Commun. 88, 408 (1992).
[CrossRef]

Rigny, P.

J. Cahen, M. Clerc, and P. Rigny, Opt. Commun. 21, 387 (1977).
[CrossRef]

Saykally, R. J.

For example, R. Casaes, R. Provençal, J. Paul, and R. J. Saykally, J. Chem. Phys. 116, 6640 (2002).

B. J. McCall, A. J. Huneycutt, R. J. Saykally, C. M. Lindsay, T. Oka, M. Fushitani, Y. Miyamoto, and T. Momose are preparing a manuscript, “Stimulated Stokes downconversion in liquid and solid parahydrogen,” to be submitted to Appl. Phys.

Schwarz, S. E.

G. Eckhardt, R. W. Hellwarth, F. J. McClung, S. E. Schwarz, D. Weiner, and E. J. Woodbury, Phys. Rev. Lett. 9, 455 (1962).
[CrossRef]

Shida, T.

T. Momose and T. Shida, Bull. Chem. Soc. Jpn. 71, 1 (1998).
[CrossRef]

Stoicheff, B. P.

B. P. Stoicheff, in Proceedings of the International School of Physics, Enrico Fermi, Course XXXI, C. H. Townes and P. A. Miles, eds. (Academic, New York, 1963), pp. 306–325.

Sussmann, R.

R. Sussmann, Th. Weber, E. Riedle, and H. J. Neusser, Opt. Commun. 88, 408 (1992).
[CrossRef]

Trutna, W. R.

Weber, Th.

R. Sussmann, Th. Weber, E. Riedle, and H. J. Neusser, Opt. Commun. 88, 408 (1992).
[CrossRef]

Weiner, D.

G. Eckhardt, R. W. Hellwarth, F. J. McClung, S. E. Schwarz, D. Weiner, and E. J. Woodbury, Phys. Rev. Lett. 9, 455 (1962).
[CrossRef]

Weliky, D. P.

D. P. Weliky, K. E. Kerr, T. J. Byers, Y. Zhang, T. Momose, and T. Oka, J. Chem. Phys. 105, 4461 (1996).

T. Momose, D. P. Weliky, and T. Oka, J. Mol. Spectrosc. 153, 760 (1992).
[CrossRef]

Woodbury, E. J.

G. Eckhardt, R. W. Hellwarth, F. J. McClung, S. E. Schwarz, D. Weiner, and E. J. Woodbury, Phys. Rev. Lett. 9, 455 (1962).
[CrossRef]

E. J. Woodbury and W. K. Ng, Proc. IRE 50, 2367 (1962).

Zhang, Y.

D. P. Weliky, K. E. Kerr, T. J. Byers, Y. Zhang, T. Momose, and T. Oka, J. Chem. Phys. 105, 4461 (1996).

Appl. Opt. (1)

Bull. Chem. Soc. Jpn. (1)

T. Momose and T. Shida, Bull. Chem. Soc. Jpn. 71, 1 (1998).
[CrossRef]

J. Chem. Phys. (2)

D. P. Weliky, K. E. Kerr, T. J. Byers, Y. Zhang, T. Momose, and T. Oka, J. Chem. Phys. 105, 4461 (1996).

For example, R. Casaes, R. Provençal, J. Paul, and R. J. Saykally, J. Chem. Phys. 116, 6640 (2002).

J. Mol. Spectrosc. (1)

T. Momose, D. P. Weliky, and T. Oka, J. Mol. Spectrosc. 153, 760 (1992).
[CrossRef]

Opt. Commun. (2)

J. Cahen, M. Clerc, and P. Rigny, Opt. Commun. 21, 387 (1977).
[CrossRef]

R. Sussmann, Th. Weber, E. Riedle, and H. J. Neusser, Opt. Commun. 88, 408 (1992).
[CrossRef]

Opt. Lett. (1)

Phys. Rev. Lett. (1)

G. Eckhardt, R. W. Hellwarth, F. J. McClung, S. E. Schwarz, D. Weiner, and E. J. Woodbury, Phys. Rev. Lett. 9, 455 (1962).
[CrossRef]

Proc. IRE (1)

E. J. Woodbury and W. K. Ng, Proc. IRE 50, 2367 (1962).

Other (4)

N. Bloembergen, Nonlinear Optics (Benjamin, New York, 1965).

B. P. Stoicheff, in Proceedings of the International School of Physics, Enrico Fermi, Course XXXI, C. H. Townes and P. A. Miles, eds. (Academic, New York, 1963), pp. 306–325.

S. Y. Lee, “Infrared studies on solid hydrogen, deuterium and hydrogen–deuteride using Fourier-transform spectroscopy,” Ph.D. dissertation (Ohio State University, Columbus, Ohio, 1987).

B. J. McCall, A. J. Huneycutt, R. J. Saykally, C. M. Lindsay, T. Oka, M. Fushitani, Y. Miyamoto, and T. Momose are preparing a manuscript, “Stimulated Stokes downconversion in liquid and solid parahydrogen,” to be submitted to Appl. Phys.

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Figures (3)

Fig. 1
Fig. 1

Top, output pulse energy and bottom, conversion efficiency of a para-hydrogen crystal for the first (683-nm), second (953-nm), and third (1575-nm) Stokes and the first anti-Stokes (436 nm) as a function of the 532-nm input pulse energy.

Fig. 2
Fig. 2

Output pulse energy of the 4.3µm first Stokes emission of a para-hydrogen crystal as a function of the 1.6µm input pulse energy.

Fig. 3
Fig. 3

Absorption spectrum of the ν3 transition of CD4. Upper trace, spectrum measured with the output of a SRS cell pumped with 1.6µm radiation; lower trace, spectrum recorded by a conventional Fourier-transform infrared (FTIR) spectrometer.

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