Abstract

We have controlled the relative phase between two successively generated coherent anti-Stokes Raman-scattering signals with a homemade phase-shifting unit, the thickness of which could be automatically adjusted as the wavelength of Stokes beam scanned in a wide spectral range. With this technique we have recovered the Q-branch spectrum of carbon monoxide distorted by a large nonresonant contribution from propane. Also, we have selectively recorded the spectrum of hydrogen chloride buried in the spectrum of propane.

© 1994 Optical Society of America

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References

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  1. A. C. Eckbreth, “Coherent anti-Stokes Raman spectroscopy,” Laser Diagnostics for Combustion Temperature and Species, A. K. Gupka, D. G. Lilley, eds., Vol. 7 of Energy & Engineering Science Series (Abacus, Tunbridge Wells, England, 1988), Chap. 6, p. 21.
  2. H. W. Schrötter, H. Frunder, H. Berger, J. P. Boquillon, B. Lavorel, G. Millot, “High resolution CARS and inverse Raman spectroscopy,” in Advances in Non-Linear Spectroscopy, R. J. H. Clark, R. E. Hester, eds., Vol. 15 of Advances in Spectroscopy (Wiley, New York, 1988), pp. 97–98.
  3. R. L. Farrow, R. P. Lucht, G. L. Clark, R. E. Palmer, “Species concentration measurements using CARS with non-resonant susceptibility normalization,” Appl. Opt. 24, 2241–2251 (1985).
    [CrossRef] [PubMed]
  4. T. Dreier, B. Lange, J. Wolfrum, M. Zahn, “Determination of temperature and concentration of molecular nitrogen, oxygen and methane with coherent anti-Stokes Raman scattering,” Appl. Phys. B 45, 183–190 (1988).
    [CrossRef]
  5. J. J. Song, G. L. Eesley, M. D. Levenson, “Background suppression in coherent Raman spectroscopy,” Appl. Phys. Lett. 29, 567–569 (1976).
    [CrossRef]
  6. J. L. Oudar, R. W. Smith, Y. R. Shen, “Polarization-sensitive coherent anti-Stokes Raman spectroscopy,” Appl. Phys. Lett. 34, 758–760 (1979).
    [CrossRef]
  7. R. K. Chang, J. Ducuing, N. Bloembergen, “Relative phase measurement between fundamental and second-harmonic light,” Phys. Rev. Lett. 15, 6–8 (1965).
    [CrossRef]
  8. Y. Yacoby, R. Fitzgibbon, B. Lax, “Coherent cancellation of background in four-wave mixing spectroscopy,” J. Appl. Phys. 51, 3072–3077 (1980).
    [CrossRef]
  9. G. Lüpke, G. Marowsky, R. Steinhoff, “Phase-controlled nonlinear interferometry,” Appl. Phys. B 49, 283–289 (1989).
    [CrossRef]
  10. G. Marowsky, G. Lüpke, “CARS-background suppression by phase-controlled nonlinear interferometry,” Appl. Phys. B 51, 49–51 (1990).
    [CrossRef]
  11. E. S. Lee, J. W. Hahn, S. N. Park, C. Rhee, “Study on the interference phenomena of nonlinear optical signals,” J. Opt. Soc. Korea 3, 239–243 (1992).
  12. Hoya Optical Glass Technical Data (Hoya Corp., Tokyo, 1985), pp. 42–175.
  13. G. Herzberg, Molecular Spectra and Molecular Structure: I. Spectra of Diatomic Molecules, 2nd ed. (Van Nostrand, Princeton, 1950), p. 62.
  14. G. Herzberg, Molecular Spectr and Molecular Structure: II. Infrared and Raman Spectra of Polyatomic Molecules (Van Nostrand, Princeton, 1945), p. 361.

1992 (1)

E. S. Lee, J. W. Hahn, S. N. Park, C. Rhee, “Study on the interference phenomena of nonlinear optical signals,” J. Opt. Soc. Korea 3, 239–243 (1992).

1990 (1)

G. Marowsky, G. Lüpke, “CARS-background suppression by phase-controlled nonlinear interferometry,” Appl. Phys. B 51, 49–51 (1990).
[CrossRef]

1989 (1)

G. Lüpke, G. Marowsky, R. Steinhoff, “Phase-controlled nonlinear interferometry,” Appl. Phys. B 49, 283–289 (1989).
[CrossRef]

1988 (1)

T. Dreier, B. Lange, J. Wolfrum, M. Zahn, “Determination of temperature and concentration of molecular nitrogen, oxygen and methane with coherent anti-Stokes Raman scattering,” Appl. Phys. B 45, 183–190 (1988).
[CrossRef]

1985 (1)

1980 (1)

Y. Yacoby, R. Fitzgibbon, B. Lax, “Coherent cancellation of background in four-wave mixing spectroscopy,” J. Appl. Phys. 51, 3072–3077 (1980).
[CrossRef]

1979 (1)

J. L. Oudar, R. W. Smith, Y. R. Shen, “Polarization-sensitive coherent anti-Stokes Raman spectroscopy,” Appl. Phys. Lett. 34, 758–760 (1979).
[CrossRef]

1976 (1)

J. J. Song, G. L. Eesley, M. D. Levenson, “Background suppression in coherent Raman spectroscopy,” Appl. Phys. Lett. 29, 567–569 (1976).
[CrossRef]

1965 (1)

R. K. Chang, J. Ducuing, N. Bloembergen, “Relative phase measurement between fundamental and second-harmonic light,” Phys. Rev. Lett. 15, 6–8 (1965).
[CrossRef]

Berger, H.

H. W. Schrötter, H. Frunder, H. Berger, J. P. Boquillon, B. Lavorel, G. Millot, “High resolution CARS and inverse Raman spectroscopy,” in Advances in Non-Linear Spectroscopy, R. J. H. Clark, R. E. Hester, eds., Vol. 15 of Advances in Spectroscopy (Wiley, New York, 1988), pp. 97–98.

Bloembergen, N.

R. K. Chang, J. Ducuing, N. Bloembergen, “Relative phase measurement between fundamental and second-harmonic light,” Phys. Rev. Lett. 15, 6–8 (1965).
[CrossRef]

Boquillon, J. P.

H. W. Schrötter, H. Frunder, H. Berger, J. P. Boquillon, B. Lavorel, G. Millot, “High resolution CARS and inverse Raman spectroscopy,” in Advances in Non-Linear Spectroscopy, R. J. H. Clark, R. E. Hester, eds., Vol. 15 of Advances in Spectroscopy (Wiley, New York, 1988), pp. 97–98.

Chang, R. K.

R. K. Chang, J. Ducuing, N. Bloembergen, “Relative phase measurement between fundamental and second-harmonic light,” Phys. Rev. Lett. 15, 6–8 (1965).
[CrossRef]

Clark, G. L.

Dreier, T.

T. Dreier, B. Lange, J. Wolfrum, M. Zahn, “Determination of temperature and concentration of molecular nitrogen, oxygen and methane with coherent anti-Stokes Raman scattering,” Appl. Phys. B 45, 183–190 (1988).
[CrossRef]

Ducuing, J.

R. K. Chang, J. Ducuing, N. Bloembergen, “Relative phase measurement between fundamental and second-harmonic light,” Phys. Rev. Lett. 15, 6–8 (1965).
[CrossRef]

Eckbreth, A. C.

A. C. Eckbreth, “Coherent anti-Stokes Raman spectroscopy,” Laser Diagnostics for Combustion Temperature and Species, A. K. Gupka, D. G. Lilley, eds., Vol. 7 of Energy & Engineering Science Series (Abacus, Tunbridge Wells, England, 1988), Chap. 6, p. 21.

Eesley, G. L.

J. J. Song, G. L. Eesley, M. D. Levenson, “Background suppression in coherent Raman spectroscopy,” Appl. Phys. Lett. 29, 567–569 (1976).
[CrossRef]

Farrow, R. L.

Fitzgibbon, R.

Y. Yacoby, R. Fitzgibbon, B. Lax, “Coherent cancellation of background in four-wave mixing spectroscopy,” J. Appl. Phys. 51, 3072–3077 (1980).
[CrossRef]

Frunder, H.

H. W. Schrötter, H. Frunder, H. Berger, J. P. Boquillon, B. Lavorel, G. Millot, “High resolution CARS and inverse Raman spectroscopy,” in Advances in Non-Linear Spectroscopy, R. J. H. Clark, R. E. Hester, eds., Vol. 15 of Advances in Spectroscopy (Wiley, New York, 1988), pp. 97–98.

Hahn, J. W.

E. S. Lee, J. W. Hahn, S. N. Park, C. Rhee, “Study on the interference phenomena of nonlinear optical signals,” J. Opt. Soc. Korea 3, 239–243 (1992).

Herzberg, G.

G. Herzberg, Molecular Spectra and Molecular Structure: I. Spectra of Diatomic Molecules, 2nd ed. (Van Nostrand, Princeton, 1950), p. 62.

G. Herzberg, Molecular Spectr and Molecular Structure: II. Infrared and Raman Spectra of Polyatomic Molecules (Van Nostrand, Princeton, 1945), p. 361.

Lange, B.

T. Dreier, B. Lange, J. Wolfrum, M. Zahn, “Determination of temperature and concentration of molecular nitrogen, oxygen and methane with coherent anti-Stokes Raman scattering,” Appl. Phys. B 45, 183–190 (1988).
[CrossRef]

Lavorel, B.

H. W. Schrötter, H. Frunder, H. Berger, J. P. Boquillon, B. Lavorel, G. Millot, “High resolution CARS and inverse Raman spectroscopy,” in Advances in Non-Linear Spectroscopy, R. J. H. Clark, R. E. Hester, eds., Vol. 15 of Advances in Spectroscopy (Wiley, New York, 1988), pp. 97–98.

Lax, B.

Y. Yacoby, R. Fitzgibbon, B. Lax, “Coherent cancellation of background in four-wave mixing spectroscopy,” J. Appl. Phys. 51, 3072–3077 (1980).
[CrossRef]

Lee, E. S.

E. S. Lee, J. W. Hahn, S. N. Park, C. Rhee, “Study on the interference phenomena of nonlinear optical signals,” J. Opt. Soc. Korea 3, 239–243 (1992).

Levenson, M. D.

J. J. Song, G. L. Eesley, M. D. Levenson, “Background suppression in coherent Raman spectroscopy,” Appl. Phys. Lett. 29, 567–569 (1976).
[CrossRef]

Lucht, R. P.

Lüpke, G.

G. Marowsky, G. Lüpke, “CARS-background suppression by phase-controlled nonlinear interferometry,” Appl. Phys. B 51, 49–51 (1990).
[CrossRef]

G. Lüpke, G. Marowsky, R. Steinhoff, “Phase-controlled nonlinear interferometry,” Appl. Phys. B 49, 283–289 (1989).
[CrossRef]

Marowsky, G.

G. Marowsky, G. Lüpke, “CARS-background suppression by phase-controlled nonlinear interferometry,” Appl. Phys. B 51, 49–51 (1990).
[CrossRef]

G. Lüpke, G. Marowsky, R. Steinhoff, “Phase-controlled nonlinear interferometry,” Appl. Phys. B 49, 283–289 (1989).
[CrossRef]

Millot, G.

H. W. Schrötter, H. Frunder, H. Berger, J. P. Boquillon, B. Lavorel, G. Millot, “High resolution CARS and inverse Raman spectroscopy,” in Advances in Non-Linear Spectroscopy, R. J. H. Clark, R. E. Hester, eds., Vol. 15 of Advances in Spectroscopy (Wiley, New York, 1988), pp. 97–98.

Oudar, J. L.

J. L. Oudar, R. W. Smith, Y. R. Shen, “Polarization-sensitive coherent anti-Stokes Raman spectroscopy,” Appl. Phys. Lett. 34, 758–760 (1979).
[CrossRef]

Palmer, R. E.

Park, S. N.

E. S. Lee, J. W. Hahn, S. N. Park, C. Rhee, “Study on the interference phenomena of nonlinear optical signals,” J. Opt. Soc. Korea 3, 239–243 (1992).

Rhee, C.

E. S. Lee, J. W. Hahn, S. N. Park, C. Rhee, “Study on the interference phenomena of nonlinear optical signals,” J. Opt. Soc. Korea 3, 239–243 (1992).

Schrötter, H. W.

H. W. Schrötter, H. Frunder, H. Berger, J. P. Boquillon, B. Lavorel, G. Millot, “High resolution CARS and inverse Raman spectroscopy,” in Advances in Non-Linear Spectroscopy, R. J. H. Clark, R. E. Hester, eds., Vol. 15 of Advances in Spectroscopy (Wiley, New York, 1988), pp. 97–98.

Shen, Y. R.

J. L. Oudar, R. W. Smith, Y. R. Shen, “Polarization-sensitive coherent anti-Stokes Raman spectroscopy,” Appl. Phys. Lett. 34, 758–760 (1979).
[CrossRef]

Smith, R. W.

J. L. Oudar, R. W. Smith, Y. R. Shen, “Polarization-sensitive coherent anti-Stokes Raman spectroscopy,” Appl. Phys. Lett. 34, 758–760 (1979).
[CrossRef]

Song, J. J.

J. J. Song, G. L. Eesley, M. D. Levenson, “Background suppression in coherent Raman spectroscopy,” Appl. Phys. Lett. 29, 567–569 (1976).
[CrossRef]

Steinhoff, R.

G. Lüpke, G. Marowsky, R. Steinhoff, “Phase-controlled nonlinear interferometry,” Appl. Phys. B 49, 283–289 (1989).
[CrossRef]

Wolfrum, J.

T. Dreier, B. Lange, J. Wolfrum, M. Zahn, “Determination of temperature and concentration of molecular nitrogen, oxygen and methane with coherent anti-Stokes Raman scattering,” Appl. Phys. B 45, 183–190 (1988).
[CrossRef]

Yacoby, Y.

Y. Yacoby, R. Fitzgibbon, B. Lax, “Coherent cancellation of background in four-wave mixing spectroscopy,” J. Appl. Phys. 51, 3072–3077 (1980).
[CrossRef]

Zahn, M.

T. Dreier, B. Lange, J. Wolfrum, M. Zahn, “Determination of temperature and concentration of molecular nitrogen, oxygen and methane with coherent anti-Stokes Raman scattering,” Appl. Phys. B 45, 183–190 (1988).
[CrossRef]

Appl. Opt. (1)

Appl. Phys. B (3)

T. Dreier, B. Lange, J. Wolfrum, M. Zahn, “Determination of temperature and concentration of molecular nitrogen, oxygen and methane with coherent anti-Stokes Raman scattering,” Appl. Phys. B 45, 183–190 (1988).
[CrossRef]

G. Lüpke, G. Marowsky, R. Steinhoff, “Phase-controlled nonlinear interferometry,” Appl. Phys. B 49, 283–289 (1989).
[CrossRef]

G. Marowsky, G. Lüpke, “CARS-background suppression by phase-controlled nonlinear interferometry,” Appl. Phys. B 51, 49–51 (1990).
[CrossRef]

Appl. Phys. Lett. (2)

J. J. Song, G. L. Eesley, M. D. Levenson, “Background suppression in coherent Raman spectroscopy,” Appl. Phys. Lett. 29, 567–569 (1976).
[CrossRef]

J. L. Oudar, R. W. Smith, Y. R. Shen, “Polarization-sensitive coherent anti-Stokes Raman spectroscopy,” Appl. Phys. Lett. 34, 758–760 (1979).
[CrossRef]

J. Appl. Phys. (1)

Y. Yacoby, R. Fitzgibbon, B. Lax, “Coherent cancellation of background in four-wave mixing spectroscopy,” J. Appl. Phys. 51, 3072–3077 (1980).
[CrossRef]

J. Opt. Soc. Korea (1)

E. S. Lee, J. W. Hahn, S. N. Park, C. Rhee, “Study on the interference phenomena of nonlinear optical signals,” J. Opt. Soc. Korea 3, 239–243 (1992).

Phys. Rev. Lett. (1)

R. K. Chang, J. Ducuing, N. Bloembergen, “Relative phase measurement between fundamental and second-harmonic light,” Phys. Rev. Lett. 15, 6–8 (1965).
[CrossRef]

Other (5)

Hoya Optical Glass Technical Data (Hoya Corp., Tokyo, 1985), pp. 42–175.

G. Herzberg, Molecular Spectra and Molecular Structure: I. Spectra of Diatomic Molecules, 2nd ed. (Van Nostrand, Princeton, 1950), p. 62.

G. Herzberg, Molecular Spectr and Molecular Structure: II. Infrared and Raman Spectra of Polyatomic Molecules (Van Nostrand, Princeton, 1945), p. 361.

A. C. Eckbreth, “Coherent anti-Stokes Raman spectroscopy,” Laser Diagnostics for Combustion Temperature and Species, A. K. Gupka, D. G. Lilley, eds., Vol. 7 of Energy & Engineering Science Series (Abacus, Tunbridge Wells, England, 1988), Chap. 6, p. 21.

H. W. Schrötter, H. Frunder, H. Berger, J. P. Boquillon, B. Lavorel, G. Millot, “High resolution CARS and inverse Raman spectroscopy,” in Advances in Non-Linear Spectroscopy, R. J. H. Clark, R. E. Hester, eds., Vol. 15 of Advances in Spectroscopy (Wiley, New York, 1988), pp. 97–98.

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Figures (5)

Fig. 1
Fig. 1

Simplified model of the interference of two nonlinear optical signals in the CARS experiment.

Fig. 2
Fig. 2

Experimental configuration: cross-sectional views of the beam configuration are shown above the collimating lenses.

Fig. 3
Fig. 3

(a) Interference fringe of two CARS signals of propane without phase control, (b) complete cancellation of the CARS signal by the use of phase control.

Fig. 4
Fig. 4

CARS spectra of carbon monoxide (20 Torr) (a) with background and (b) with background suppressed.

Fig. 5
Fig. 5

CARS spectra of (a) 15-Torr HCl, (b) 400-Torr propane, (c) the mixture gas, (d) HCl with the propane signal suppressed.

Tables (1)

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Table 1 Parameters Used for the Calculation of δd BK7/δω s a

Equations (8)

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I CARS = A 2 [ χ CARS 1 ( 3 ) 2 + χ CARS 2 ( 3 ) 2 + 2 χ CARS 1 ( 3 ) * χ CARS 2 ( 3 ) cos ( ϕ + j = 1 N Δ k j d j ) ] ,
A = i 2 π ω c n 0 ( ω c ) c E p 2 E s δ , Δ k j = 2 k j ( ω p ) - k j ( ω s ) - k j ( ω c ) , k j ( ω ) = n j ( ω ) ω / c , χ CARS 1 ( 3 ) * χ CARS 2 = χ CARS 1 ( 3 ) * χ CARS 2 ( 3 ) exp ( i ϕ ) .
χ CARS 1 ( 3 ) = χ des ( 3 ) + χ undes ( 3 ) ,
χ CARS 2 ( 3 ) = χ undes ( 3 ) ,
I CARS = A 2 χ des ( 3 ) 2 .
δ ( Δ k j d j ) = δ ( Δ k j ) d j + Δ k j δ d i = 0.
δ d i = j L c - i L c - j d j L c - j ( d L c - j d ω s ) δ ω s ,
δ d BK 7 = [ L c - BK 7 L c - SF 2 d SF 2 L c - SF 2 ( d L c - SF 2 d ω s ) + d BK 7 L c - BK 7 ( d L c - BK 7 d ω s ) ] δ ω s ,

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