Abstract

The theoretical basis for photoacoustic Raman spectroscopy (PARS) is developed. An expression for the Raman gain coefficient is derived. This gain coefficient is used to determine the change in the internal translational energy of a gaseous sample that is produced by illumination with two laser beams whose frequency difference corresponds to a Raman frequency shift. The magnitude of the pressure change associated with this nonlinear Raman process was deduced for a simple quasi-equilibrium model appropriate for modulated cw laser excitation and for a kinetic model applicable to pulsed laser excitation. The kinetic model explicitly accounts for the various pumping and relaxation rates associated with the PARS process.

© 1981 Optical Society of America

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  1. J. J. Barrett, "Photoacoustic Raman spectroscopy of gases," in Chemical Applications of Nonlinear Raman Spectroscopy, A. B. Harvey, ed. (Academic, New York, 1981), pp. 89–169.
  2. J. J. Barrett and M. J. Berry, "Photoacoustic Raman scattering in gases," in Proceedings of the Sixth International Conference on Raman Spectroscopy, E. Schmid, R. Krishnan, W. Kiefer, and H. Schrötter, eds. (Heyden, London, 1978), Vol. 1, pp. 466–467; "Photoacoustic Raman spectroscopy using cw laser sources," Appl. Phys. Lett. 34,144–146 (1979).
  3. G. A. West, D. R. Siebert, and J. J. Barrett, "Gas phase photoacoustic Raman spectroscopy using pulsed laser excitation," J. Appl. Phys. 51, 2823–2828 (1980).
  4. D. R. Siebert, G. A. West, and J. J. Barrett, "Gaseous trace analysis using pulsed photoacoustic Raman spectroscopy," Appl. Opt. 19, 53–60 (1980).
  5. Preliminary results were reported by J. J. Barrett at the Second Chemical Congress of the North American Continent, Las Vegas, Nev., August 24–29, 1980, and at the 1980 Federation of Analytical Chemistry and Spectroscopy Societies (FACSS) Meeting, Philadelphia, Pa., September 28-October 3, 1980.
  6. G. A. West and J. J. Barrett, "Pure rotational stimulated Raman photoacoustic spectroscopy," Opt. Lett. 4, 395–397 (1979).
  7. G. A. West and J. J. Barrett, "Photoacoustic pure rotational Raman spectroscopy," in The Proceedings of the VII International Conference on Raman Spectroscopy (North-Holland, Amsterdam, 1980), pp. 696–697.
  8. A. G. Bell, "On the production and reproduction of sound by light," Proc. Am. Assoc. Adv. Sci. 29, 115–136 (1880); "Upon the production of sound by radiant energy," Philos. Mag. 11, 510–528 (1881).
  9. J. Tyndall, "Action of an intermittent beam of radiant heat upon gaseous matter," Proc. R. Soc. London 31, 307–317 (1881).
  10. E. L. Kerr and J. G. Atwood, "The laser illuminated absorptivity spectrophone: a method for measurement of weak absorptivity in gases at laser wavelengths," Appl. Opt. 7, 915–921 (1968).
  11. L. B. Kreuzer, "Ultralow gas concentration infrared absorption spectroscopy," J. Appl. Phys. 42, 2934–2943 (1971).
  12. L. B. Kreuzer and C. K. N. Patel, "Nitric oxide air pollution: detection by optoacoustic spectroscopy," Science 173, 45–47 (1971).
  13. L. B. Kreuzer, N. D. Kenyon, and C. K. N. Patel, "Air pollution: sensitive detection of ten pollutant gases by carbon monoxide and carbon dioxide lasers," Science 177, 347–349 (1972).
  14. L. B. Kreuzer, "Laser optoacoustic spectroscopy—A new technique of gas analysis," Anal. Chem. 46, 239A–244A (1974).
  15. C. K. N. Patel, E. G. Burkhardt, and C. A. Lambert, "Spectroscopic measurements of stratospheric nitric oxide and water vapor," Science 184, 1173–1176 (1974).
  16. E. Kritchman, S. Shtrikman, and M. Slatkine, "Resonant optoacoustic cells for trace gas analysis," J. Opt. Soc. Am. 68, 1257–1271 (1978).
  17. K. V. Reddy, R. G. Bray, and M. J. Berry, "Dye laser-induced photochemistry," in Advances in Laser Chemistry, A. H. Zewail, ed. (Springer-Verlag, Berlin, 1978), pp. 48–61.
  18. M. W. Tolles, J. W. Nibler, J. R. McDonald, and A. B. Harvey, "A review of the theory and application of coherent anti-Stokes Raman spectroscopy (CARS)," Appl. Spectroso. 31, 253–271 (1977).
  19. D. Heiman, R. W. Hellwarth, M. D. Levenson, and G. Martin, "Raman-induced Kerr effect," Phys. Rev. Lett. 36, 189–192 (1976).
  20. A. Owyoung, "Coherent Raman gain spectroscopy using cw laser sources," IEEE J. Quantum Electron. QE-14, 192–203 (1978).
  21. M. Maier, W. Kaiser, and J. A. Giordmaine, "Backward stimulated Raman scattering," Phys. Rev. 177, 580–599 (1969).
  22. M. Maier, "Applications of stimulated Raman scattering," Appl. Phys. 11, 209–231 (1976).

1980 (2)

G. A. West, D. R. Siebert, and J. J. Barrett, "Gas phase photoacoustic Raman spectroscopy using pulsed laser excitation," J. Appl. Phys. 51, 2823–2828 (1980).

D. R. Siebert, G. A. West, and J. J. Barrett, "Gaseous trace analysis using pulsed photoacoustic Raman spectroscopy," Appl. Opt. 19, 53–60 (1980).

1979 (1)

1978 (2)

E. Kritchman, S. Shtrikman, and M. Slatkine, "Resonant optoacoustic cells for trace gas analysis," J. Opt. Soc. Am. 68, 1257–1271 (1978).

A. Owyoung, "Coherent Raman gain spectroscopy using cw laser sources," IEEE J. Quantum Electron. QE-14, 192–203 (1978).

1977 (1)

M. W. Tolles, J. W. Nibler, J. R. McDonald, and A. B. Harvey, "A review of the theory and application of coherent anti-Stokes Raman spectroscopy (CARS)," Appl. Spectroso. 31, 253–271 (1977).

1976 (2)

D. Heiman, R. W. Hellwarth, M. D. Levenson, and G. Martin, "Raman-induced Kerr effect," Phys. Rev. Lett. 36, 189–192 (1976).

M. Maier, "Applications of stimulated Raman scattering," Appl. Phys. 11, 209–231 (1976).

1974 (2)

L. B. Kreuzer, "Laser optoacoustic spectroscopy—A new technique of gas analysis," Anal. Chem. 46, 239A–244A (1974).

C. K. N. Patel, E. G. Burkhardt, and C. A. Lambert, "Spectroscopic measurements of stratospheric nitric oxide and water vapor," Science 184, 1173–1176 (1974).

1972 (1)

L. B. Kreuzer, N. D. Kenyon, and C. K. N. Patel, "Air pollution: sensitive detection of ten pollutant gases by carbon monoxide and carbon dioxide lasers," Science 177, 347–349 (1972).

1971 (2)

L. B. Kreuzer, "Ultralow gas concentration infrared absorption spectroscopy," J. Appl. Phys. 42, 2934–2943 (1971).

L. B. Kreuzer and C. K. N. Patel, "Nitric oxide air pollution: detection by optoacoustic spectroscopy," Science 173, 45–47 (1971).

1969 (1)

M. Maier, W. Kaiser, and J. A. Giordmaine, "Backward stimulated Raman scattering," Phys. Rev. 177, 580–599 (1969).

1968 (1)

1881 (1)

J. Tyndall, "Action of an intermittent beam of radiant heat upon gaseous matter," Proc. R. Soc. London 31, 307–317 (1881).

1880 (1)

A. G. Bell, "On the production and reproduction of sound by light," Proc. Am. Assoc. Adv. Sci. 29, 115–136 (1880); "Upon the production of sound by radiant energy," Philos. Mag. 11, 510–528 (1881).

Atwood, J. G.

Barrett, J. J.

G. A. West, D. R. Siebert, and J. J. Barrett, "Gas phase photoacoustic Raman spectroscopy using pulsed laser excitation," J. Appl. Phys. 51, 2823–2828 (1980).

D. R. Siebert, G. A. West, and J. J. Barrett, "Gaseous trace analysis using pulsed photoacoustic Raman spectroscopy," Appl. Opt. 19, 53–60 (1980).

G. A. West and J. J. Barrett, "Pure rotational stimulated Raman photoacoustic spectroscopy," Opt. Lett. 4, 395–397 (1979).

J. J. Barrett, "Photoacoustic Raman spectroscopy of gases," in Chemical Applications of Nonlinear Raman Spectroscopy, A. B. Harvey, ed. (Academic, New York, 1981), pp. 89–169.

Preliminary results were reported by J. J. Barrett at the Second Chemical Congress of the North American Continent, Las Vegas, Nev., August 24–29, 1980, and at the 1980 Federation of Analytical Chemistry and Spectroscopy Societies (FACSS) Meeting, Philadelphia, Pa., September 28-October 3, 1980.

G. A. West and J. J. Barrett, "Photoacoustic pure rotational Raman spectroscopy," in The Proceedings of the VII International Conference on Raman Spectroscopy (North-Holland, Amsterdam, 1980), pp. 696–697.

J. J. Barrett and M. J. Berry, "Photoacoustic Raman scattering in gases," in Proceedings of the Sixth International Conference on Raman Spectroscopy, E. Schmid, R. Krishnan, W. Kiefer, and H. Schrötter, eds. (Heyden, London, 1978), Vol. 1, pp. 466–467; "Photoacoustic Raman spectroscopy using cw laser sources," Appl. Phys. Lett. 34,144–146 (1979).

Bell, A. G.

A. G. Bell, "On the production and reproduction of sound by light," Proc. Am. Assoc. Adv. Sci. 29, 115–136 (1880); "Upon the production of sound by radiant energy," Philos. Mag. 11, 510–528 (1881).

Berry, M. J.

J. J. Barrett and M. J. Berry, "Photoacoustic Raman scattering in gases," in Proceedings of the Sixth International Conference on Raman Spectroscopy, E. Schmid, R. Krishnan, W. Kiefer, and H. Schrötter, eds. (Heyden, London, 1978), Vol. 1, pp. 466–467; "Photoacoustic Raman spectroscopy using cw laser sources," Appl. Phys. Lett. 34,144–146 (1979).

K. V. Reddy, R. G. Bray, and M. J. Berry, "Dye laser-induced photochemistry," in Advances in Laser Chemistry, A. H. Zewail, ed. (Springer-Verlag, Berlin, 1978), pp. 48–61.

Bray, R. G.

K. V. Reddy, R. G. Bray, and M. J. Berry, "Dye laser-induced photochemistry," in Advances in Laser Chemistry, A. H. Zewail, ed. (Springer-Verlag, Berlin, 1978), pp. 48–61.

Burkhardt, E. G.

C. K. N. Patel, E. G. Burkhardt, and C. A. Lambert, "Spectroscopic measurements of stratospheric nitric oxide and water vapor," Science 184, 1173–1176 (1974).

Giordmaine, J. A.

M. Maier, W. Kaiser, and J. A. Giordmaine, "Backward stimulated Raman scattering," Phys. Rev. 177, 580–599 (1969).

Harvey, A. B.

M. W. Tolles, J. W. Nibler, J. R. McDonald, and A. B. Harvey, "A review of the theory and application of coherent anti-Stokes Raman spectroscopy (CARS)," Appl. Spectroso. 31, 253–271 (1977).

Heiman, D.

D. Heiman, R. W. Hellwarth, M. D. Levenson, and G. Martin, "Raman-induced Kerr effect," Phys. Rev. Lett. 36, 189–192 (1976).

Hellwarth, R. W.

D. Heiman, R. W. Hellwarth, M. D. Levenson, and G. Martin, "Raman-induced Kerr effect," Phys. Rev. Lett. 36, 189–192 (1976).

Kaiser, W.

M. Maier, W. Kaiser, and J. A. Giordmaine, "Backward stimulated Raman scattering," Phys. Rev. 177, 580–599 (1969).

Kenyon, N. D.

L. B. Kreuzer, N. D. Kenyon, and C. K. N. Patel, "Air pollution: sensitive detection of ten pollutant gases by carbon monoxide and carbon dioxide lasers," Science 177, 347–349 (1972).

Kerr, E. L.

Kreuzer, L. B.

L. B. Kreuzer, "Laser optoacoustic spectroscopy—A new technique of gas analysis," Anal. Chem. 46, 239A–244A (1974).

L. B. Kreuzer, N. D. Kenyon, and C. K. N. Patel, "Air pollution: sensitive detection of ten pollutant gases by carbon monoxide and carbon dioxide lasers," Science 177, 347–349 (1972).

L. B. Kreuzer and C. K. N. Patel, "Nitric oxide air pollution: detection by optoacoustic spectroscopy," Science 173, 45–47 (1971).

L. B. Kreuzer, "Ultralow gas concentration infrared absorption spectroscopy," J. Appl. Phys. 42, 2934–2943 (1971).

Kritchman, E.

Lambert, C. A.

C. K. N. Patel, E. G. Burkhardt, and C. A. Lambert, "Spectroscopic measurements of stratospheric nitric oxide and water vapor," Science 184, 1173–1176 (1974).

Levenson, M. D.

D. Heiman, R. W. Hellwarth, M. D. Levenson, and G. Martin, "Raman-induced Kerr effect," Phys. Rev. Lett. 36, 189–192 (1976).

Maier, M.

M. Maier, "Applications of stimulated Raman scattering," Appl. Phys. 11, 209–231 (1976).

M. Maier, W. Kaiser, and J. A. Giordmaine, "Backward stimulated Raman scattering," Phys. Rev. 177, 580–599 (1969).

Martin, G.

D. Heiman, R. W. Hellwarth, M. D. Levenson, and G. Martin, "Raman-induced Kerr effect," Phys. Rev. Lett. 36, 189–192 (1976).

McDonald, J. R.

M. W. Tolles, J. W. Nibler, J. R. McDonald, and A. B. Harvey, "A review of the theory and application of coherent anti-Stokes Raman spectroscopy (CARS)," Appl. Spectroso. 31, 253–271 (1977).

Nibler, J. W.

M. W. Tolles, J. W. Nibler, J. R. McDonald, and A. B. Harvey, "A review of the theory and application of coherent anti-Stokes Raman spectroscopy (CARS)," Appl. Spectroso. 31, 253–271 (1977).

Owyoung, A.

A. Owyoung, "Coherent Raman gain spectroscopy using cw laser sources," IEEE J. Quantum Electron. QE-14, 192–203 (1978).

Patel, C. K. N.

C. K. N. Patel, E. G. Burkhardt, and C. A. Lambert, "Spectroscopic measurements of stratospheric nitric oxide and water vapor," Science 184, 1173–1176 (1974).

L. B. Kreuzer, N. D. Kenyon, and C. K. N. Patel, "Air pollution: sensitive detection of ten pollutant gases by carbon monoxide and carbon dioxide lasers," Science 177, 347–349 (1972).

L. B. Kreuzer and C. K. N. Patel, "Nitric oxide air pollution: detection by optoacoustic spectroscopy," Science 173, 45–47 (1971).

Reddy, K. V.

K. V. Reddy, R. G. Bray, and M. J. Berry, "Dye laser-induced photochemistry," in Advances in Laser Chemistry, A. H. Zewail, ed. (Springer-Verlag, Berlin, 1978), pp. 48–61.

Shtrikman, S.

Siebert, D. R.

G. A. West, D. R. Siebert, and J. J. Barrett, "Gas phase photoacoustic Raman spectroscopy using pulsed laser excitation," J. Appl. Phys. 51, 2823–2828 (1980).

D. R. Siebert, G. A. West, and J. J. Barrett, "Gaseous trace analysis using pulsed photoacoustic Raman spectroscopy," Appl. Opt. 19, 53–60 (1980).

Slatkine, M.

Tolles, M. W.

M. W. Tolles, J. W. Nibler, J. R. McDonald, and A. B. Harvey, "A review of the theory and application of coherent anti-Stokes Raman spectroscopy (CARS)," Appl. Spectroso. 31, 253–271 (1977).

Tyndall, J.

J. Tyndall, "Action of an intermittent beam of radiant heat upon gaseous matter," Proc. R. Soc. London 31, 307–317 (1881).

West, G. A.

G. A. West, D. R. Siebert, and J. J. Barrett, "Gas phase photoacoustic Raman spectroscopy using pulsed laser excitation," J. Appl. Phys. 51, 2823–2828 (1980).

D. R. Siebert, G. A. West, and J. J. Barrett, "Gaseous trace analysis using pulsed photoacoustic Raman spectroscopy," Appl. Opt. 19, 53–60 (1980).

G. A. West and J. J. Barrett, "Pure rotational stimulated Raman photoacoustic spectroscopy," Opt. Lett. 4, 395–397 (1979).

G. A. West and J. J. Barrett, "Photoacoustic pure rotational Raman spectroscopy," in The Proceedings of the VII International Conference on Raman Spectroscopy (North-Holland, Amsterdam, 1980), pp. 696–697.

Anal. Chem. (1)

L. B. Kreuzer, "Laser optoacoustic spectroscopy—A new technique of gas analysis," Anal. Chem. 46, 239A–244A (1974).

Appl. Opt. (2)

Appl. Phys. (1)

M. Maier, "Applications of stimulated Raman scattering," Appl. Phys. 11, 209–231 (1976).

Appl. Spectroso. (1)

M. W. Tolles, J. W. Nibler, J. R. McDonald, and A. B. Harvey, "A review of the theory and application of coherent anti-Stokes Raman spectroscopy (CARS)," Appl. Spectroso. 31, 253–271 (1977).

IEEE J. Quantum Electron. (1)

A. Owyoung, "Coherent Raman gain spectroscopy using cw laser sources," IEEE J. Quantum Electron. QE-14, 192–203 (1978).

J. Appl. Phys. (2)

G. A. West, D. R. Siebert, and J. J. Barrett, "Gas phase photoacoustic Raman spectroscopy using pulsed laser excitation," J. Appl. Phys. 51, 2823–2828 (1980).

L. B. Kreuzer, "Ultralow gas concentration infrared absorption spectroscopy," J. Appl. Phys. 42, 2934–2943 (1971).

J. Opt. Soc. Am. (1)

Opt. Lett. (1)

Phys. Rev. (1)

M. Maier, W. Kaiser, and J. A. Giordmaine, "Backward stimulated Raman scattering," Phys. Rev. 177, 580–599 (1969).

Phys. Rev. Lett. (1)

D. Heiman, R. W. Hellwarth, M. D. Levenson, and G. Martin, "Raman-induced Kerr effect," Phys. Rev. Lett. 36, 189–192 (1976).

Proc. Am. Assoc. Adv. Sci. (1)

A. G. Bell, "On the production and reproduction of sound by light," Proc. Am. Assoc. Adv. Sci. 29, 115–136 (1880); "Upon the production of sound by radiant energy," Philos. Mag. 11, 510–528 (1881).

Proc. R. Soc. London (1)

J. Tyndall, "Action of an intermittent beam of radiant heat upon gaseous matter," Proc. R. Soc. London 31, 307–317 (1881).

Science (3)

L. B. Kreuzer and C. K. N. Patel, "Nitric oxide air pollution: detection by optoacoustic spectroscopy," Science 173, 45–47 (1971).

L. B. Kreuzer, N. D. Kenyon, and C. K. N. Patel, "Air pollution: sensitive detection of ten pollutant gases by carbon monoxide and carbon dioxide lasers," Science 177, 347–349 (1972).

C. K. N. Patel, E. G. Burkhardt, and C. A. Lambert, "Spectroscopic measurements of stratospheric nitric oxide and water vapor," Science 184, 1173–1176 (1974).

Other (5)

K. V. Reddy, R. G. Bray, and M. J. Berry, "Dye laser-induced photochemistry," in Advances in Laser Chemistry, A. H. Zewail, ed. (Springer-Verlag, Berlin, 1978), pp. 48–61.

Preliminary results were reported by J. J. Barrett at the Second Chemical Congress of the North American Continent, Las Vegas, Nev., August 24–29, 1980, and at the 1980 Federation of Analytical Chemistry and Spectroscopy Societies (FACSS) Meeting, Philadelphia, Pa., September 28-October 3, 1980.

G. A. West and J. J. Barrett, "Photoacoustic pure rotational Raman spectroscopy," in The Proceedings of the VII International Conference on Raman Spectroscopy (North-Holland, Amsterdam, 1980), pp. 696–697.

J. J. Barrett, "Photoacoustic Raman spectroscopy of gases," in Chemical Applications of Nonlinear Raman Spectroscopy, A. B. Harvey, ed. (Academic, New York, 1981), pp. 89–169.

J. J. Barrett and M. J. Berry, "Photoacoustic Raman scattering in gases," in Proceedings of the Sixth International Conference on Raman Spectroscopy, E. Schmid, R. Krishnan, W. Kiefer, and H. Schrötter, eds. (Heyden, London, 1978), Vol. 1, pp. 466–467; "Photoacoustic Raman spectroscopy using cw laser sources," Appl. Phys. Lett. 34,144–146 (1979).

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