Abstract

The concentration and pressure dependence of dual-pump coherent anti-Stokes Raman spectroscopy (CARS) signals from nitrogen and methane was investigated. CARS spectra were acquired from a gas cell at pressures of 0.007 to 2.24 MPa and methane concentrations of 0.5 to 50%. The square root of the methane signal intensity divided by the nitrogen signal intensity was found to have a near-linear dependence on methane concentration at all pressures investigated. The pressure dependence of this integrated intensity ratio decreased with increasing pressure and became negligible at the highest pressures tested. The shot-to-shot variation at concentrations determined from single-laser-shot measurements was less than 7%. Single-laser-shot CARS spectra of nitrogen and methane were obtained from the cylinder of a firing direct-injection natural gas engine.

© 1998 Optical Society of America

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References

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  1. S. A. J. Druet, J. P. E. Taran, “CARS spectroscopy,” Prog. Quantum Electron. 7, 1–72 (1981).
    [CrossRef]
  2. R. J. Hall, A. C. Eckbreth, “Coherent anti-Stokes Raman spectroscopy (CARS): application to combustion diagnostics,” in Laser Applications, J. F. Ready, R. K. Erf, eds. (Academic, New York, 1984), Vol. 5, pp. 213–309.
  3. A. C. Eckbreth, “Coherent anti-Stokes Raman spectroscopy (CARS),” in Laser Diagnostics for Combustion Temperature and Species, W. A. Sirignano, ed. (Gordon and Breach, Amsterdam B. V., 1996), Vol. 3, pp. 221–300.
  4. L. P. Goss, “CARS instrumentation for combustion applications,” in Instrumentation for Flows With Combustion, A. Taylor, ed. (Academic, London, 1993), pp. 251–322.
  5. R. R. Antcliff, O. Jarrett, “Multispecies coherent anti-Stokes Raman scattering instrument for turbulent combustion,” Rev. Sci. Instrum. 58, 2075–2080 (1987).
    [CrossRef]
  6. T. J. Anderson, A. C. Eckbreth, “Simultaneous coherent anti-Stokes Raman spectroscopy measurements in hydrogen-fueled supersonic combustion,” AIAA J. Prop. 8, 7–15 (1992).
    [CrossRef]
  7. A. C. Eckbreth, T. J. Anderson, “Dual broadband CARS for simultaneous, multiple species measurements,” Appl. Opt. 24, 2731–2736 (1985).
    [CrossRef] [PubMed]
  8. R. E. Teets, “Three-color coherent anti-Stokes Raman scattering,” presented at the 1985 International Laser Science Conference, Dallas, Tex., 18–22 November 1985.
  9. R. P. Lucht, “Three-laser coherent anti-Stokes Raman scattering measurements of two species,” Opt. Lett. 12, 78–80 (1987).
    [CrossRef] [PubMed]
  10. R. D. Hancock, F. R. Schauer, R. P. Lucht, R. L. Farrow, “Dual-pump coherent anti-Stokes Raman scattering measurements of nitrogen and oxygen in a laminar jet diffusion flame,” Appl. Opt. 36, 3217–3226 (1997).
    [CrossRef] [PubMed]
  11. F. R. Schauer, S. M. Green, R. E. Lucht, R. D. Hancock, V. R. Katta, “Flame structure of stabilization region in a laminar hydrogen jet diffusion flame,” in Proceedings of the Thirty-First Technical Meeting on Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, Pt. Clear, Ala., 1997), pp. 170–175.
  12. J. P. Singh, F. Y. Yueh, “Comparative study of temperature measurements with folded BOXCARS and collinear CARS,” Combust. Flame 89, 77–94 (1992).
    [CrossRef]
  13. K. A. Marko, L. Rimai, “Space- and time-resolved coherent anti-Stokes Raman spectroscopy for combustion diagnostics,” Opt. Lett. 4, 211–213 (1979).
    [CrossRef] [PubMed]
  14. D. Klick, K. A. Marko, L. Rimai, “Broadband single-pulse CARS spectra in a fired internal combustion engine,” Appl. Opt. 20, 1178–1181 (1981).
    [CrossRef] [PubMed]
  15. D. Brüggemann, B. Wies, X. X. Zhang, T. Heinze, K. F. Knoche, “CARS spectroscopy for temperature and concentration measurements in a spark ignition engine,” in Combustion Flow Diagnostics, D. F. G. Durão, M. V. Heitor, J. H. Whitelaw, P. O. Witze, eds. (Kluwer Academic, Dordrecht, The Netherlands, 1992), pp. 495–511.
    [CrossRef]
  16. M. L. Willi, B. G. Richards, “Design and development of a direct injected, glow plug ignition-assisted, natural gas engine,” ASME J. Eng. Gas Turb. Power 117, 799–803 (1995).
    [CrossRef]
  17. P. J. Rubas, M. A. Paul, S. M. Green, R. E. Coverdill, R. P. Lucht, J. E. Peters, M. L. Willi, A. W. Wells, “Experimental program on fuel/air mixing and combustion in a direct-injection natural gas engine,” in Proceedings of the Thirtieth Technical Meeting for Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, St. Louis, Mo., 1996), pp. 22–27.
  18. P. E. Bengtsson, L. Martinsson, M. Alden, “Combined vibrational and rotational CARS for simultaneous measurements of temperature and concentrations of fuel, oxygen, and nitrogen,” Appl. Spectrosc. 49, 188–192 (1995).
    [CrossRef]
  19. S. M. Green, “A dual-pump CARS system for the simultaneous detection of nitrogen and methane,” Ph.D. dissertation (University of Illinois, Urbana, Ill., 1997).
  20. L. S. Yuen, J. E. Peters, R. E. Lucht, “Pressure dependence of laser-induced fluorescence from acetone,” Appl. Opt. 36, 3271–3277 (1997).
    [CrossRef] [PubMed]
  21. R. E. Sonntag, G. J. Van Wylen, “An introduction to the thermodynamics of mixtures,” in Introduction to Classical Thermodynamics: Classical and Statistical, 3rd ed. (Wiley, New York, 1991), pp. 336–361.
  22. W. B. Roh, P. W. Schreiber, “Pressure dependence of integrated CARS power,” Appl. Opt. 17, 1418–1424 (1978).
    [CrossRef] [PubMed]
  23. R. E. Palmer, “The CARSFT computer code for calculating coherent anti-Stokes Raman spectra: user and programmer information,” Sandia Rep. SAND89-8206 (Sandia National Laboratories, Livermore, Calif., 1989).

1997 (2)

1995 (2)

P. E. Bengtsson, L. Martinsson, M. Alden, “Combined vibrational and rotational CARS for simultaneous measurements of temperature and concentrations of fuel, oxygen, and nitrogen,” Appl. Spectrosc. 49, 188–192 (1995).
[CrossRef]

M. L. Willi, B. G. Richards, “Design and development of a direct injected, glow plug ignition-assisted, natural gas engine,” ASME J. Eng. Gas Turb. Power 117, 799–803 (1995).
[CrossRef]

1992 (2)

T. J. Anderson, A. C. Eckbreth, “Simultaneous coherent anti-Stokes Raman spectroscopy measurements in hydrogen-fueled supersonic combustion,” AIAA J. Prop. 8, 7–15 (1992).
[CrossRef]

J. P. Singh, F. Y. Yueh, “Comparative study of temperature measurements with folded BOXCARS and collinear CARS,” Combust. Flame 89, 77–94 (1992).
[CrossRef]

1987 (2)

R. R. Antcliff, O. Jarrett, “Multispecies coherent anti-Stokes Raman scattering instrument for turbulent combustion,” Rev. Sci. Instrum. 58, 2075–2080 (1987).
[CrossRef]

R. P. Lucht, “Three-laser coherent anti-Stokes Raman scattering measurements of two species,” Opt. Lett. 12, 78–80 (1987).
[CrossRef] [PubMed]

1985 (1)

1981 (2)

1979 (1)

1978 (1)

Alden, M.

Anderson, T. J.

T. J. Anderson, A. C. Eckbreth, “Simultaneous coherent anti-Stokes Raman spectroscopy measurements in hydrogen-fueled supersonic combustion,” AIAA J. Prop. 8, 7–15 (1992).
[CrossRef]

A. C. Eckbreth, T. J. Anderson, “Dual broadband CARS for simultaneous, multiple species measurements,” Appl. Opt. 24, 2731–2736 (1985).
[CrossRef] [PubMed]

Antcliff, R. R.

R. R. Antcliff, O. Jarrett, “Multispecies coherent anti-Stokes Raman scattering instrument for turbulent combustion,” Rev. Sci. Instrum. 58, 2075–2080 (1987).
[CrossRef]

Bengtsson, P. E.

Brüggemann, D.

D. Brüggemann, B. Wies, X. X. Zhang, T. Heinze, K. F. Knoche, “CARS spectroscopy for temperature and concentration measurements in a spark ignition engine,” in Combustion Flow Diagnostics, D. F. G. Durão, M. V. Heitor, J. H. Whitelaw, P. O. Witze, eds. (Kluwer Academic, Dordrecht, The Netherlands, 1992), pp. 495–511.
[CrossRef]

Coverdill, R. E.

P. J. Rubas, M. A. Paul, S. M. Green, R. E. Coverdill, R. P. Lucht, J. E. Peters, M. L. Willi, A. W. Wells, “Experimental program on fuel/air mixing and combustion in a direct-injection natural gas engine,” in Proceedings of the Thirtieth Technical Meeting for Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, St. Louis, Mo., 1996), pp. 22–27.

Druet, S. A. J.

S. A. J. Druet, J. P. E. Taran, “CARS spectroscopy,” Prog. Quantum Electron. 7, 1–72 (1981).
[CrossRef]

Eckbreth, A. C.

T. J. Anderson, A. C. Eckbreth, “Simultaneous coherent anti-Stokes Raman spectroscopy measurements in hydrogen-fueled supersonic combustion,” AIAA J. Prop. 8, 7–15 (1992).
[CrossRef]

A. C. Eckbreth, T. J. Anderson, “Dual broadband CARS for simultaneous, multiple species measurements,” Appl. Opt. 24, 2731–2736 (1985).
[CrossRef] [PubMed]

R. J. Hall, A. C. Eckbreth, “Coherent anti-Stokes Raman spectroscopy (CARS): application to combustion diagnostics,” in Laser Applications, J. F. Ready, R. K. Erf, eds. (Academic, New York, 1984), Vol. 5, pp. 213–309.

A. C. Eckbreth, “Coherent anti-Stokes Raman spectroscopy (CARS),” in Laser Diagnostics for Combustion Temperature and Species, W. A. Sirignano, ed. (Gordon and Breach, Amsterdam B. V., 1996), Vol. 3, pp. 221–300.

Farrow, R. L.

Goss, L. P.

L. P. Goss, “CARS instrumentation for combustion applications,” in Instrumentation for Flows With Combustion, A. Taylor, ed. (Academic, London, 1993), pp. 251–322.

Green, S. M.

P. J. Rubas, M. A. Paul, S. M. Green, R. E. Coverdill, R. P. Lucht, J. E. Peters, M. L. Willi, A. W. Wells, “Experimental program on fuel/air mixing and combustion in a direct-injection natural gas engine,” in Proceedings of the Thirtieth Technical Meeting for Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, St. Louis, Mo., 1996), pp. 22–27.

F. R. Schauer, S. M. Green, R. E. Lucht, R. D. Hancock, V. R. Katta, “Flame structure of stabilization region in a laminar hydrogen jet diffusion flame,” in Proceedings of the Thirty-First Technical Meeting on Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, Pt. Clear, Ala., 1997), pp. 170–175.

S. M. Green, “A dual-pump CARS system for the simultaneous detection of nitrogen and methane,” Ph.D. dissertation (University of Illinois, Urbana, Ill., 1997).

Hall, R. J.

R. J. Hall, A. C. Eckbreth, “Coherent anti-Stokes Raman spectroscopy (CARS): application to combustion diagnostics,” in Laser Applications, J. F. Ready, R. K. Erf, eds. (Academic, New York, 1984), Vol. 5, pp. 213–309.

Hancock, R. D.

R. D. Hancock, F. R. Schauer, R. P. Lucht, R. L. Farrow, “Dual-pump coherent anti-Stokes Raman scattering measurements of nitrogen and oxygen in a laminar jet diffusion flame,” Appl. Opt. 36, 3217–3226 (1997).
[CrossRef] [PubMed]

F. R. Schauer, S. M. Green, R. E. Lucht, R. D. Hancock, V. R. Katta, “Flame structure of stabilization region in a laminar hydrogen jet diffusion flame,” in Proceedings of the Thirty-First Technical Meeting on Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, Pt. Clear, Ala., 1997), pp. 170–175.

Heinze, T.

D. Brüggemann, B. Wies, X. X. Zhang, T. Heinze, K. F. Knoche, “CARS spectroscopy for temperature and concentration measurements in a spark ignition engine,” in Combustion Flow Diagnostics, D. F. G. Durão, M. V. Heitor, J. H. Whitelaw, P. O. Witze, eds. (Kluwer Academic, Dordrecht, The Netherlands, 1992), pp. 495–511.
[CrossRef]

Jarrett, O.

R. R. Antcliff, O. Jarrett, “Multispecies coherent anti-Stokes Raman scattering instrument for turbulent combustion,” Rev. Sci. Instrum. 58, 2075–2080 (1987).
[CrossRef]

Katta, V. R.

F. R. Schauer, S. M. Green, R. E. Lucht, R. D. Hancock, V. R. Katta, “Flame structure of stabilization region in a laminar hydrogen jet diffusion flame,” in Proceedings of the Thirty-First Technical Meeting on Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, Pt. Clear, Ala., 1997), pp. 170–175.

Klick, D.

Knoche, K. F.

D. Brüggemann, B. Wies, X. X. Zhang, T. Heinze, K. F. Knoche, “CARS spectroscopy for temperature and concentration measurements in a spark ignition engine,” in Combustion Flow Diagnostics, D. F. G. Durão, M. V. Heitor, J. H. Whitelaw, P. O. Witze, eds. (Kluwer Academic, Dordrecht, The Netherlands, 1992), pp. 495–511.
[CrossRef]

Lucht, R. E.

L. S. Yuen, J. E. Peters, R. E. Lucht, “Pressure dependence of laser-induced fluorescence from acetone,” Appl. Opt. 36, 3271–3277 (1997).
[CrossRef] [PubMed]

F. R. Schauer, S. M. Green, R. E. Lucht, R. D. Hancock, V. R. Katta, “Flame structure of stabilization region in a laminar hydrogen jet diffusion flame,” in Proceedings of the Thirty-First Technical Meeting on Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, Pt. Clear, Ala., 1997), pp. 170–175.

Lucht, R. P.

R. D. Hancock, F. R. Schauer, R. P. Lucht, R. L. Farrow, “Dual-pump coherent anti-Stokes Raman scattering measurements of nitrogen and oxygen in a laminar jet diffusion flame,” Appl. Opt. 36, 3217–3226 (1997).
[CrossRef] [PubMed]

R. P. Lucht, “Three-laser coherent anti-Stokes Raman scattering measurements of two species,” Opt. Lett. 12, 78–80 (1987).
[CrossRef] [PubMed]

P. J. Rubas, M. A. Paul, S. M. Green, R. E. Coverdill, R. P. Lucht, J. E. Peters, M. L. Willi, A. W. Wells, “Experimental program on fuel/air mixing and combustion in a direct-injection natural gas engine,” in Proceedings of the Thirtieth Technical Meeting for Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, St. Louis, Mo., 1996), pp. 22–27.

Marko, K. A.

Martinsson, L.

Palmer, R. E.

R. E. Palmer, “The CARSFT computer code for calculating coherent anti-Stokes Raman spectra: user and programmer information,” Sandia Rep. SAND89-8206 (Sandia National Laboratories, Livermore, Calif., 1989).

Paul, M. A.

P. J. Rubas, M. A. Paul, S. M. Green, R. E. Coverdill, R. P. Lucht, J. E. Peters, M. L. Willi, A. W. Wells, “Experimental program on fuel/air mixing and combustion in a direct-injection natural gas engine,” in Proceedings of the Thirtieth Technical Meeting for Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, St. Louis, Mo., 1996), pp. 22–27.

Peters, J. E.

L. S. Yuen, J. E. Peters, R. E. Lucht, “Pressure dependence of laser-induced fluorescence from acetone,” Appl. Opt. 36, 3271–3277 (1997).
[CrossRef] [PubMed]

P. J. Rubas, M. A. Paul, S. M. Green, R. E. Coverdill, R. P. Lucht, J. E. Peters, M. L. Willi, A. W. Wells, “Experimental program on fuel/air mixing and combustion in a direct-injection natural gas engine,” in Proceedings of the Thirtieth Technical Meeting for Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, St. Louis, Mo., 1996), pp. 22–27.

Richards, B. G.

M. L. Willi, B. G. Richards, “Design and development of a direct injected, glow plug ignition-assisted, natural gas engine,” ASME J. Eng. Gas Turb. Power 117, 799–803 (1995).
[CrossRef]

Rimai, L.

Roh, W. B.

Rubas, P. J.

P. J. Rubas, M. A. Paul, S. M. Green, R. E. Coverdill, R. P. Lucht, J. E. Peters, M. L. Willi, A. W. Wells, “Experimental program on fuel/air mixing and combustion in a direct-injection natural gas engine,” in Proceedings of the Thirtieth Technical Meeting for Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, St. Louis, Mo., 1996), pp. 22–27.

Schauer, F. R.

R. D. Hancock, F. R. Schauer, R. P. Lucht, R. L. Farrow, “Dual-pump coherent anti-Stokes Raman scattering measurements of nitrogen and oxygen in a laminar jet diffusion flame,” Appl. Opt. 36, 3217–3226 (1997).
[CrossRef] [PubMed]

F. R. Schauer, S. M. Green, R. E. Lucht, R. D. Hancock, V. R. Katta, “Flame structure of stabilization region in a laminar hydrogen jet diffusion flame,” in Proceedings of the Thirty-First Technical Meeting on Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, Pt. Clear, Ala., 1997), pp. 170–175.

Schreiber, P. W.

Singh, J. P.

J. P. Singh, F. Y. Yueh, “Comparative study of temperature measurements with folded BOXCARS and collinear CARS,” Combust. Flame 89, 77–94 (1992).
[CrossRef]

Sonntag, R. E.

R. E. Sonntag, G. J. Van Wylen, “An introduction to the thermodynamics of mixtures,” in Introduction to Classical Thermodynamics: Classical and Statistical, 3rd ed. (Wiley, New York, 1991), pp. 336–361.

Taran, J. P. E.

S. A. J. Druet, J. P. E. Taran, “CARS spectroscopy,” Prog. Quantum Electron. 7, 1–72 (1981).
[CrossRef]

Teets, R. E.

R. E. Teets, “Three-color coherent anti-Stokes Raman scattering,” presented at the 1985 International Laser Science Conference, Dallas, Tex., 18–22 November 1985.

Van Wylen, G. J.

R. E. Sonntag, G. J. Van Wylen, “An introduction to the thermodynamics of mixtures,” in Introduction to Classical Thermodynamics: Classical and Statistical, 3rd ed. (Wiley, New York, 1991), pp. 336–361.

Wells, A. W.

P. J. Rubas, M. A. Paul, S. M. Green, R. E. Coverdill, R. P. Lucht, J. E. Peters, M. L. Willi, A. W. Wells, “Experimental program on fuel/air mixing and combustion in a direct-injection natural gas engine,” in Proceedings of the Thirtieth Technical Meeting for Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, St. Louis, Mo., 1996), pp. 22–27.

Wies, B.

D. Brüggemann, B. Wies, X. X. Zhang, T. Heinze, K. F. Knoche, “CARS spectroscopy for temperature and concentration measurements in a spark ignition engine,” in Combustion Flow Diagnostics, D. F. G. Durão, M. V. Heitor, J. H. Whitelaw, P. O. Witze, eds. (Kluwer Academic, Dordrecht, The Netherlands, 1992), pp. 495–511.
[CrossRef]

Willi, M. L.

M. L. Willi, B. G. Richards, “Design and development of a direct injected, glow plug ignition-assisted, natural gas engine,” ASME J. Eng. Gas Turb. Power 117, 799–803 (1995).
[CrossRef]

P. J. Rubas, M. A. Paul, S. M. Green, R. E. Coverdill, R. P. Lucht, J. E. Peters, M. L. Willi, A. W. Wells, “Experimental program on fuel/air mixing and combustion in a direct-injection natural gas engine,” in Proceedings of the Thirtieth Technical Meeting for Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, St. Louis, Mo., 1996), pp. 22–27.

Yueh, F. Y.

J. P. Singh, F. Y. Yueh, “Comparative study of temperature measurements with folded BOXCARS and collinear CARS,” Combust. Flame 89, 77–94 (1992).
[CrossRef]

Yuen, L. S.

Zhang, X. X.

D. Brüggemann, B. Wies, X. X. Zhang, T. Heinze, K. F. Knoche, “CARS spectroscopy for temperature and concentration measurements in a spark ignition engine,” in Combustion Flow Diagnostics, D. F. G. Durão, M. V. Heitor, J. H. Whitelaw, P. O. Witze, eds. (Kluwer Academic, Dordrecht, The Netherlands, 1992), pp. 495–511.
[CrossRef]

AIAA J. Prop. (1)

T. J. Anderson, A. C. Eckbreth, “Simultaneous coherent anti-Stokes Raman spectroscopy measurements in hydrogen-fueled supersonic combustion,” AIAA J. Prop. 8, 7–15 (1992).
[CrossRef]

Appl. Opt. (5)

Appl. Spectrosc. (1)

ASME J. Eng. Gas Turb. Power (1)

M. L. Willi, B. G. Richards, “Design and development of a direct injected, glow plug ignition-assisted, natural gas engine,” ASME J. Eng. Gas Turb. Power 117, 799–803 (1995).
[CrossRef]

Combust. Flame (1)

J. P. Singh, F. Y. Yueh, “Comparative study of temperature measurements with folded BOXCARS and collinear CARS,” Combust. Flame 89, 77–94 (1992).
[CrossRef]

Opt. Lett. (2)

Prog. Quantum Electron. (1)

S. A. J. Druet, J. P. E. Taran, “CARS spectroscopy,” Prog. Quantum Electron. 7, 1–72 (1981).
[CrossRef]

Rev. Sci. Instrum. (1)

R. R. Antcliff, O. Jarrett, “Multispecies coherent anti-Stokes Raman scattering instrument for turbulent combustion,” Rev. Sci. Instrum. 58, 2075–2080 (1987).
[CrossRef]

Other (10)

R. J. Hall, A. C. Eckbreth, “Coherent anti-Stokes Raman spectroscopy (CARS): application to combustion diagnostics,” in Laser Applications, J. F. Ready, R. K. Erf, eds. (Academic, New York, 1984), Vol. 5, pp. 213–309.

A. C. Eckbreth, “Coherent anti-Stokes Raman spectroscopy (CARS),” in Laser Diagnostics for Combustion Temperature and Species, W. A. Sirignano, ed. (Gordon and Breach, Amsterdam B. V., 1996), Vol. 3, pp. 221–300.

L. P. Goss, “CARS instrumentation for combustion applications,” in Instrumentation for Flows With Combustion, A. Taylor, ed. (Academic, London, 1993), pp. 251–322.

D. Brüggemann, B. Wies, X. X. Zhang, T. Heinze, K. F. Knoche, “CARS spectroscopy for temperature and concentration measurements in a spark ignition engine,” in Combustion Flow Diagnostics, D. F. G. Durão, M. V. Heitor, J. H. Whitelaw, P. O. Witze, eds. (Kluwer Academic, Dordrecht, The Netherlands, 1992), pp. 495–511.
[CrossRef]

F. R. Schauer, S. M. Green, R. E. Lucht, R. D. Hancock, V. R. Katta, “Flame structure of stabilization region in a laminar hydrogen jet diffusion flame,” in Proceedings of the Thirty-First Technical Meeting on Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, Pt. Clear, Ala., 1997), pp. 170–175.

P. J. Rubas, M. A. Paul, S. M. Green, R. E. Coverdill, R. P. Lucht, J. E. Peters, M. L. Willi, A. W. Wells, “Experimental program on fuel/air mixing and combustion in a direct-injection natural gas engine,” in Proceedings of the Thirtieth Technical Meeting for Combustion Fundamentals and Applications (Central States Section, the Combustion Institute, St. Louis, Mo., 1996), pp. 22–27.

R. E. Teets, “Three-color coherent anti-Stokes Raman scattering,” presented at the 1985 International Laser Science Conference, Dallas, Tex., 18–22 November 1985.

S. M. Green, “A dual-pump CARS system for the simultaneous detection of nitrogen and methane,” Ph.D. dissertation (University of Illinois, Urbana, Ill., 1997).

R. E. Sonntag, G. J. Van Wylen, “An introduction to the thermodynamics of mixtures,” in Introduction to Classical Thermodynamics: Classical and Statistical, 3rd ed. (Wiley, New York, 1991), pp. 336–361.

R. E. Palmer, “The CARSFT computer code for calculating coherent anti-Stokes Raman spectra: user and programmer information,” Sandia Rep. SAND89-8206 (Sandia National Laboratories, Livermore, Calif., 1989).

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Figures (15)

Fig. 1
Fig. 1

Energy-level diagram for dual-pump CARS detection of nitrogen and methane. The frequencies of pump 1 (ω1), pump 2 (ω2), and the Stokes beam (ω S ) are 18,797, 18,213, and 15,882 cm-1, respectively. The frequency of the anti-Stokes signal (ω aS ) is 21,128 cm-1.

Fig. 2
Fig. 2

CARS signal generation with use of annular phase matching. The CARS signal is generated as an annulus outside of the pump beams. The probe volume, defined by the region where over 90% of the signal is generated, is approximately 5 mm long and 50 μm in diameter.19

Fig. 3
Fig. 3

Beam separation and mixing for annular CARS design. M, mirror; AM, annular mirror; BS, beam splitter; T, telescope; 1/2, half-wave plate; GP, Glan polarizer.

Fig. 4
Fig. 4

DING engine spacer plate design for CARS optical access. The spacer plate is approximately 1 in. thick and the CARS windows are 30 mm × 15 mm × 19 mm thick. For demonstration measurements, the probe volume was positioned 12 mm directly below the injector and glow plug, as shown.

Fig. 5
Fig. 5

Nitrogen and methane spectra acquired in a high-pressure gas cell with use of annular CARS. The equivalence ratios correspond to relative methane concentrations of 0.5, 1, 2, 5, 10, 25, and 50%. The spectra were averaged for 100 laser shots and were acquired at a fixed pressure of 1.03 MPa. Each spectrum was normalized to a maximum value of 1.

Fig. 6
Fig. 6

Variation of nitrogen and methane spectra with an increase in pressure. These spectra were acquired in a high-pressure gas cell with use of annular CARS and were averaged for 200 laser shots at a fixed methane concentration of 5%. Each spectrum was normalized to a maximum value of 1. Total pressure variation is 0.17–9.9 atm.

Fig. 7
Fig. 7

Spectra acquired in a high-pressure gas cell while scanning the narrow-band dye laser (pump 2). These spectra were acquired at a fixed pressure and relative methane concentration of 1.03 MPa and 5%, respectively, and averaged for 100 laser shots. A different nonresonant background signal was acquired for each spectrum. Each spectrum was normalized to a maximum value of 1.

Fig. 8
Fig. 8

Data series of the square root of the integrated intensity ratio for relative methane concentrations of 2, 5, and 10%, respectively. Four hundred spectra were acquired at a fixed pressure of 1.03 MPa for each concentration. In each case, the mean value is given by X and the standard deviation by σ.

Fig. 9
Fig. 9

Histogram (PDF) of the square root of the integrated intensity ratio for a methane concentration of 5%. Four hundred single-shot spectra were acquired at a fixed pressure of 1.03 MPa. The x axis is normalized by the mean value of 0.88 and the y axis by the value in the largest bin. The standard deviation is 6.6%.

Fig. 10
Fig. 10

Integrated intensity ratio variation with methane concentration. All the spectra were acquired at a constant pressure of 1.03 MPa. The mean values from the single-shot data and data acquired with pure methane are included. A least-squares fit to the commercial methane points is shown.

Fig. 11
Fig. 11

Variation of the integrated intensity ratio with pressure and methane concentration. The spectra were obtained for pressures from 0.017 to 2.24 MPa and for methane concentrations from 0.5 to 50%. The spectra were averaged for 100–200 laser shots.

Fig. 12
Fig. 12

Collisional narrowing effects on the peak signal intensity and peak intensity ratio. Nitrogen peak intensity was determined from the Sandia carsft code.23 The peak intensity of methane was determined experimentally. The equivalence ratio was 0.84 (10% methane) and the pressure was 1.03 MPa.

Fig. 13
Fig. 13

Dependence of the square root of the integrated intensity ratio with pressure. Data were acquired with commercial methane, and each spectrum was averaged over 100 laser shots. Correlation coefficients for each curve fit are 0.99 or higher.

Fig. 14
Fig. 14

Single-shot methane–nitrogen spectra obtained from a firing DING engine. Measurements were obtained 12 mm below the fuel injector and glow plug. These spectra represent the range of methane concentrations observed at this location in the cylinder. The intensity scale for each spectrum is the same.

Fig. 15
Fig. 15

Histogram (PDF) of the square root of the integrated intensity ratio from single-shot measurements acquired from the DING engine cylinder. The probe volume was positioned at the same location described in Fig. 4. The mean value of the square root of the integrated intensity ratio is 0.91 with a standard deviation of 132%.

Equations (8)

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I aS ω aS       | χ ω 1 - ω S + χ ω 2 - ω S | 2 I 1 ω 1 I 2 ω 2 × I S ω S δ ω 1 + ω 2 - ω S - ω aS d ω 1 d ω 2 d ω S
χ ω i - ω S = 1 2 χ r ω i - ω S + 1 2 χ nr ,
χ r = J 2 π c 4 Δ N J d σ / d Ω J h ω S 4 ω J - ω i + ω S - i Γ J ,
ω aS 1 = ω k R + ω 2 ω aS 2 = ω m R + ω 1 .
ω S = ω 1 - ω vib CH 4 = 15,882   cm - 1     λ S = 629.6   nm , ω 2 = ω vib N 2 + ω S = 18,213   cm - 1     λ 2 = 549.1   nm , ω aS = ω 1 + ω 2 - ω S = 21,128   cm - 1     λ aS = 473.3   nm .
ϕ = 7.52   η CH 4 η N 2   =   7.52   η CH 4 1 - η CH 4 ,
integrated   intensity   ratio = spectral   peak CH 4 d ω aS 1 / 2 spectral   peak N 2 d ω aS 1 / 2 ,
integrated   intensity   ratio     20 η CH 4 ,

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