Abstract

Nonplanar, crossed-beam phase matching has been employed to obtain pure rotational coherent anti-Stokes Raman spectroscopy (CARS) [and coherent Stokes Raman spectroscopy (CSRS)] spectra to within a few wavenumbers of the incident pump frequency. Using this approach, the rotational CARS (and CSRS) radiation is spatially separated from the pump and Stokes beams; therefore small Raman shifts can be observed with a single monochromator.

© 1980 Optical Society of America

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References

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  1. R. F. Begley, A. B. Harvey, R. L. Byer, Appl. Phys. Lett. 25, 387–390 (1974).
    [CrossRef]
  2. P. R. Régnier, F. Moya, J. P. E. Taran, AIAA J. 12, 826–831 (1974).
    [CrossRef]
  3. I. R. Beattie, T. R. Gilson, D. A. Greenhalgh, Nature 276, 378–379 (1978).
    [CrossRef]
  4. A. C. Eckbreth, Appl. Phys. Lett. 32, 421–423 (1978).
    [CrossRef]
  5. G. Laufer, R. B. Miles, Opt. Commun. 28, 250–254 (1979).
    [CrossRef]
  6. A. Compaan, S. Chandra, Opt. Lett. 4, 170–172 (1979).
    [CrossRef] [PubMed]
  7. K. A. Marko, L. Rimai, Opt. Lett. 4, 211–213 (1979).
    [CrossRef] [PubMed]
  8. L. P. Goss, J. W Fleming, A. B. Harvey, Opt. Lett. 5, 345–347 (1980).
    [CrossRef] [PubMed]
  9. R. L. Farrow, P. L. Mattern, L. A. Rahn, “Crossed-beam background-free CARS measurements in a methane diffusion flame,” presented at the VIIth International Conference on Raman Spectroscopy, Ottawa, Canada, August 1980.
  10. A. C. Eckbreth, R. J. Hall, J. A Shirley, “Investigations of coherent anti-Stokes Raman spectroscopy (CARS) for practical combustion diagnostics,” presented at the AGARD Propulsion and Energetics Panel 55th (A) Specialists Meeting on Testing and Measurement Techniques in Heat Transfer and Combustion, Brussels, Belgium, May 1980.
  11. Y. Prior, Appl. Opt. 19, 1741–1743 (1980).
    [CrossRef]
  12. A. C. Eckbreth, R. J. Hall, J. A. Shirley, “Investigations of coherent anti-Stokes Raman spectroscopy (CARS) for combustion diagnostics,” presented at 17th Aerospace Sciences Meeting, New Orleans, La., January 1979.
  13. R. J. Hall, J. F. Verdieck, A. C. Eckbreth, “Pressure-induced narrowing of the CARS spectrum of N2,” Opt. Commun. (to be published).
  14. S. Bhagavantam, Scattering of Light and the Raman Effect (Chemical Publishing Co., Brooklyn, N.Y., 1942).
  15. G. A. West, J. J. Barrett, 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, to be published).
    [CrossRef] [PubMed]
  16. K. S. Jammu, G. E. St. John, H. L. Welsh, Can. J. Phys. 44, 797–814 (1966).
    [CrossRef]

1980 (2)

1979 (4)

1978 (2)

I. R. Beattie, T. R. Gilson, D. A. Greenhalgh, Nature 276, 378–379 (1978).
[CrossRef]

A. C. Eckbreth, Appl. Phys. Lett. 32, 421–423 (1978).
[CrossRef]

1974 (2)

R. F. Begley, A. B. Harvey, R. L. Byer, Appl. Phys. Lett. 25, 387–390 (1974).
[CrossRef]

P. R. Régnier, F. Moya, J. P. E. Taran, AIAA J. 12, 826–831 (1974).
[CrossRef]

1966 (1)

K. S. Jammu, G. E. St. John, H. L. Welsh, Can. J. Phys. 44, 797–814 (1966).
[CrossRef]

Barrett, J. J.

Beattie, I. R.

I. R. Beattie, T. R. Gilson, D. A. Greenhalgh, Nature 276, 378–379 (1978).
[CrossRef]

Begley, R. F.

R. F. Begley, A. B. Harvey, R. L. Byer, Appl. Phys. Lett. 25, 387–390 (1974).
[CrossRef]

Bhagavantam, S.

S. Bhagavantam, Scattering of Light and the Raman Effect (Chemical Publishing Co., Brooklyn, N.Y., 1942).

Byer, R. L.

R. F. Begley, A. B. Harvey, R. L. Byer, Appl. Phys. Lett. 25, 387–390 (1974).
[CrossRef]

Chandra, S.

Compaan, A.

Eckbreth, A. C.

A. C. Eckbreth, Appl. Phys. Lett. 32, 421–423 (1978).
[CrossRef]

A. C. Eckbreth, R. J. Hall, J. A. Shirley, “Investigations of coherent anti-Stokes Raman spectroscopy (CARS) for combustion diagnostics,” presented at 17th Aerospace Sciences Meeting, New Orleans, La., January 1979.

R. J. Hall, J. F. Verdieck, A. C. Eckbreth, “Pressure-induced narrowing of the CARS spectrum of N2,” Opt. Commun. (to be published).

A. C. Eckbreth, R. J. Hall, J. A Shirley, “Investigations of coherent anti-Stokes Raman spectroscopy (CARS) for practical combustion diagnostics,” presented at the AGARD Propulsion and Energetics Panel 55th (A) Specialists Meeting on Testing and Measurement Techniques in Heat Transfer and Combustion, Brussels, Belgium, May 1980.

Farrow, R. L.

R. L. Farrow, P. L. Mattern, L. A. Rahn, “Crossed-beam background-free CARS measurements in a methane diffusion flame,” presented at the VIIth International Conference on Raman Spectroscopy, Ottawa, Canada, August 1980.

Fleming, J. W

Gilson, T. R.

I. R. Beattie, T. R. Gilson, D. A. Greenhalgh, Nature 276, 378–379 (1978).
[CrossRef]

Goss, L. P.

Greenhalgh, D. A.

I. R. Beattie, T. R. Gilson, D. A. Greenhalgh, Nature 276, 378–379 (1978).
[CrossRef]

Hall, R. J.

A. C. Eckbreth, R. J. Hall, J. A. Shirley, “Investigations of coherent anti-Stokes Raman spectroscopy (CARS) for combustion diagnostics,” presented at 17th Aerospace Sciences Meeting, New Orleans, La., January 1979.

A. C. Eckbreth, R. J. Hall, J. A Shirley, “Investigations of coherent anti-Stokes Raman spectroscopy (CARS) for practical combustion diagnostics,” presented at the AGARD Propulsion and Energetics Panel 55th (A) Specialists Meeting on Testing and Measurement Techniques in Heat Transfer and Combustion, Brussels, Belgium, May 1980.

R. J. Hall, J. F. Verdieck, A. C. Eckbreth, “Pressure-induced narrowing of the CARS spectrum of N2,” Opt. Commun. (to be published).

Harvey, A. B.

L. P. Goss, J. W Fleming, A. B. Harvey, Opt. Lett. 5, 345–347 (1980).
[CrossRef] [PubMed]

R. F. Begley, A. B. Harvey, R. L. Byer, Appl. Phys. Lett. 25, 387–390 (1974).
[CrossRef]

Jammu, K. S.

K. S. Jammu, G. E. St. John, H. L. Welsh, Can. J. Phys. 44, 797–814 (1966).
[CrossRef]

Laufer, G.

G. Laufer, R. B. Miles, Opt. Commun. 28, 250–254 (1979).
[CrossRef]

Marko, K. A.

Mattern, P. L.

R. L. Farrow, P. L. Mattern, L. A. Rahn, “Crossed-beam background-free CARS measurements in a methane diffusion flame,” presented at the VIIth International Conference on Raman Spectroscopy, Ottawa, Canada, August 1980.

Miles, R. B.

G. Laufer, R. B. Miles, Opt. Commun. 28, 250–254 (1979).
[CrossRef]

Moya, F.

P. R. Régnier, F. Moya, J. P. E. Taran, AIAA J. 12, 826–831 (1974).
[CrossRef]

Prior, Y.

Rahn, L. A.

R. L. Farrow, P. L. Mattern, L. A. Rahn, “Crossed-beam background-free CARS measurements in a methane diffusion flame,” presented at the VIIth International Conference on Raman Spectroscopy, Ottawa, Canada, August 1980.

Régnier, P. R.

P. R. Régnier, F. Moya, J. P. E. Taran, AIAA J. 12, 826–831 (1974).
[CrossRef]

Rimai, L.

Shirley, J. A

A. C. Eckbreth, R. J. Hall, J. A Shirley, “Investigations of coherent anti-Stokes Raman spectroscopy (CARS) for practical combustion diagnostics,” presented at the AGARD Propulsion and Energetics Panel 55th (A) Specialists Meeting on Testing and Measurement Techniques in Heat Transfer and Combustion, Brussels, Belgium, May 1980.

Shirley, J. A.

A. C. Eckbreth, R. J. Hall, J. A. Shirley, “Investigations of coherent anti-Stokes Raman spectroscopy (CARS) for combustion diagnostics,” presented at 17th Aerospace Sciences Meeting, New Orleans, La., January 1979.

St. John, G. E.

K. S. Jammu, G. E. St. John, H. L. Welsh, Can. J. Phys. 44, 797–814 (1966).
[CrossRef]

Taran, J. P. E.

P. R. Régnier, F. Moya, J. P. E. Taran, AIAA J. 12, 826–831 (1974).
[CrossRef]

Verdieck, J. F.

R. J. Hall, J. F. Verdieck, A. C. Eckbreth, “Pressure-induced narrowing of the CARS spectrum of N2,” Opt. Commun. (to be published).

Welsh, H. L.

K. S. Jammu, G. E. St. John, H. L. Welsh, Can. J. Phys. 44, 797–814 (1966).
[CrossRef]

West, G. A.

AIAA J. (1)

P. R. Régnier, F. Moya, J. P. E. Taran, AIAA J. 12, 826–831 (1974).
[CrossRef]

Appl. Opt. (1)

Appl. Phys. Lett. (2)

R. F. Begley, A. B. Harvey, R. L. Byer, Appl. Phys. Lett. 25, 387–390 (1974).
[CrossRef]

A. C. Eckbreth, Appl. Phys. Lett. 32, 421–423 (1978).
[CrossRef]

Can. J. Phys. (1)

K. S. Jammu, G. E. St. John, H. L. Welsh, Can. J. Phys. 44, 797–814 (1966).
[CrossRef]

Nature (1)

I. R. Beattie, T. R. Gilson, D. A. Greenhalgh, Nature 276, 378–379 (1978).
[CrossRef]

Opt. Commun. (1)

G. Laufer, R. B. Miles, Opt. Commun. 28, 250–254 (1979).
[CrossRef]

Opt. Lett. (4)

Other (5)

A. C. Eckbreth, R. J. Hall, J. A. Shirley, “Investigations of coherent anti-Stokes Raman spectroscopy (CARS) for combustion diagnostics,” presented at 17th Aerospace Sciences Meeting, New Orleans, La., January 1979.

R. J. Hall, J. F. Verdieck, A. C. Eckbreth, “Pressure-induced narrowing of the CARS spectrum of N2,” Opt. Commun. (to be published).

S. Bhagavantam, Scattering of Light and the Raman Effect (Chemical Publishing Co., Brooklyn, N.Y., 1942).

R. L. Farrow, P. L. Mattern, L. A. Rahn, “Crossed-beam background-free CARS measurements in a methane diffusion flame,” presented at the VIIth International Conference on Raman Spectroscopy, Ottawa, Canada, August 1980.

A. C. Eckbreth, R. J. Hall, J. A Shirley, “Investigations of coherent anti-Stokes Raman spectroscopy (CARS) for practical combustion diagnostics,” presented at the AGARD Propulsion and Energetics Panel 55th (A) Specialists Meeting on Testing and Measurement Techniques in Heat Transfer and Combustion, Brussels, Belgium, May 1980.

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Figures (3)

Fig. 1
Fig. 1

CARS crossed-beam phase-matching approaches showing the phase-matching diagram and actual geometry of the optical beams for (a) planar and (b) folded BOXCARS. Subscripts denote beams: 1, pump; 2, Stokes; 3, anti-Stokes.

Fig. 2
Fig. 2

Rotational CARS spectrum of air at normal temperature and pressure. The pump- and Stokes-laser polarizations are parallel. Instrumental resolution is 0.06 nm (2 cm−1).

Fig. 3
Fig. 3

Rotational CARS spectrum of N2 at normal temperature and pressure. The pump- and Stokes-laser polarizations are perpendicular. The solid curve shows the measured spectra, and the dotted curve shows the theoretical prediction. The calculation is arbitrarily truncated so that transitions beyond J = 12 → 14 are not shown.

Equations (2)

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χ ( 3 ) ~ J J 1 m m | α J , m J + 2 , m | 2 Δ ρ J , m J + 2 , m ,
N g J ( 2 J + 1 ) Q R { exp [ J ( J + 1 ) hcB / kT ] exp [ ( J + 2 ) ( J + 3 ) hcB / kT ] } = N J [ 1 exp ( hc Δ ω J J + 2 / kT ) ] ,

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