Abstract

A new technique for suppressing the nonresonant contribution to the coherent anti-Stokes Raman scattering (CARS) signal is presented. This involves two-laser three-beam CARS generation using picosecond pulses in which one of the pump beams is delayed with respect to the two others. A reduction of 2 orders of magnitude is obtained for the 656-cm−1 vibrational line of CS2 in a 10% mixture of CS2 in toluene. This reduction is limited by the ratio of the energy in our pulse laser to that in its trailing background, which is about 100:1. Use of alternative laser systems would reduce the background by about 1012:1.

© 1980 Optical Society of America

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  1. W. M. Tolles, J. W. Nibler, J. R. McDonald, A. B. Harvey, Appl. Spectrosc. 31, 253 (1977).
    [CrossRef]
  2. R. T. Lynch, S. D. Kramer, H. Lotem, N. Bloembergen, Opt. Commun. 16, 372 (1976).
    [CrossRef]
  3. J. J. Song, G. L. Eesley, M. D. Levenson, Appl. Phys. Lett. 29, 567 (1976).
    [CrossRef]
  4. A. Owyoung, IEEE J. Quantum Electron. QE-14, 192 (1978).
    [CrossRef]
  5. J. L. Ouder, R. W. Smith, Y. R. Shen, Appl. Phys. Lett. 34, 758 (1979).
    [CrossRef]
  6. M. G. Sceats, reported by A. B. Harvey, J. W. Nibler in Appl. Spectrosc. Rev. 14, 101 (1978).
    [CrossRef]
  7. A. Laubereau, W. Kaiser, Rev. Mod. Phys. 50, 607 (1978).
    [CrossRef]
  8. W. Zinth, A. Laubereau, W. Kaiser, Opt, Commun. 26, 457 (1978).
    [CrossRef]
  9. A. C. Eckbreth, AppI. Phys. Lett. 32, 421 (1978).
    [CrossRef]
  10. J. P. Heritage, Appl. Phys. Lett. 34, 470 (1979).
    [CrossRef]

1979 (2)

J. L. Ouder, R. W. Smith, Y. R. Shen, Appl. Phys. Lett. 34, 758 (1979).
[CrossRef]

J. P. Heritage, Appl. Phys. Lett. 34, 470 (1979).
[CrossRef]

1978 (5)

A. Owyoung, IEEE J. Quantum Electron. QE-14, 192 (1978).
[CrossRef]

M. G. Sceats, reported by A. B. Harvey, J. W. Nibler in Appl. Spectrosc. Rev. 14, 101 (1978).
[CrossRef]

M. G. Sceats, reported by A. B. Harvey, J. W. Nibler in Appl. Spectrosc. Rev. 14, 101 (1978).
[CrossRef]

A. Laubereau, W. Kaiser, Rev. Mod. Phys. 50, 607 (1978).
[CrossRef]

W. Zinth, A. Laubereau, W. Kaiser, Opt, Commun. 26, 457 (1978).
[CrossRef]

A. C. Eckbreth, AppI. Phys. Lett. 32, 421 (1978).
[CrossRef]

1977 (1)

1976 (2)

R. T. Lynch, S. D. Kramer, H. Lotem, N. Bloembergen, Opt. Commun. 16, 372 (1976).
[CrossRef]

J. J. Song, G. L. Eesley, M. D. Levenson, Appl. Phys. Lett. 29, 567 (1976).
[CrossRef]

Bloembergen, N.

R. T. Lynch, S. D. Kramer, H. Lotem, N. Bloembergen, Opt. Commun. 16, 372 (1976).
[CrossRef]

Eckbreth, A. C.

A. C. Eckbreth, AppI. Phys. Lett. 32, 421 (1978).
[CrossRef]

Eesley, G. L.

J. J. Song, G. L. Eesley, M. D. Levenson, Appl. Phys. Lett. 29, 567 (1976).
[CrossRef]

Harvey, A. B.

M. G. Sceats, reported by A. B. Harvey, J. W. Nibler in Appl. Spectrosc. Rev. 14, 101 (1978).
[CrossRef]

W. M. Tolles, J. W. Nibler, J. R. McDonald, A. B. Harvey, Appl. Spectrosc. 31, 253 (1977).
[CrossRef]

Heritage, J. P.

J. P. Heritage, Appl. Phys. Lett. 34, 470 (1979).
[CrossRef]

Kaiser, W.

W. Zinth, A. Laubereau, W. Kaiser, Opt, Commun. 26, 457 (1978).
[CrossRef]

A. Laubereau, W. Kaiser, Rev. Mod. Phys. 50, 607 (1978).
[CrossRef]

Kramer, S. D.

R. T. Lynch, S. D. Kramer, H. Lotem, N. Bloembergen, Opt. Commun. 16, 372 (1976).
[CrossRef]

Laubereau, A.

A. Laubereau, W. Kaiser, Rev. Mod. Phys. 50, 607 (1978).
[CrossRef]

W. Zinth, A. Laubereau, W. Kaiser, Opt, Commun. 26, 457 (1978).
[CrossRef]

Levenson, M. D.

J. J. Song, G. L. Eesley, M. D. Levenson, Appl. Phys. Lett. 29, 567 (1976).
[CrossRef]

Lotem, H.

R. T. Lynch, S. D. Kramer, H. Lotem, N. Bloembergen, Opt. Commun. 16, 372 (1976).
[CrossRef]

Lynch, R. T.

R. T. Lynch, S. D. Kramer, H. Lotem, N. Bloembergen, Opt. Commun. 16, 372 (1976).
[CrossRef]

McDonald, J. R.

Nibler, J. W.

M. G. Sceats, reported by A. B. Harvey, J. W. Nibler in Appl. Spectrosc. Rev. 14, 101 (1978).
[CrossRef]

W. M. Tolles, J. W. Nibler, J. R. McDonald, A. B. Harvey, Appl. Spectrosc. 31, 253 (1977).
[CrossRef]

Ouder, J. L.

J. L. Ouder, R. W. Smith, Y. R. Shen, Appl. Phys. Lett. 34, 758 (1979).
[CrossRef]

Owyoung, A.

A. Owyoung, IEEE J. Quantum Electron. QE-14, 192 (1978).
[CrossRef]

Sceats, M. G.

M. G. Sceats, reported by A. B. Harvey, J. W. Nibler in Appl. Spectrosc. Rev. 14, 101 (1978).
[CrossRef]

Shen, Y. R.

J. L. Ouder, R. W. Smith, Y. R. Shen, Appl. Phys. Lett. 34, 758 (1979).
[CrossRef]

Smith, R. W.

J. L. Ouder, R. W. Smith, Y. R. Shen, Appl. Phys. Lett. 34, 758 (1979).
[CrossRef]

Song, J. J.

J. J. Song, G. L. Eesley, M. D. Levenson, Appl. Phys. Lett. 29, 567 (1976).
[CrossRef]

Tolles, W. M.

Zinth, W.

W. Zinth, A. Laubereau, W. Kaiser, Opt, Commun. 26, 457 (1978).
[CrossRef]

AppI. Phys. Lett. (1)

A. C. Eckbreth, AppI. Phys. Lett. 32, 421 (1978).
[CrossRef]

Appl. Phys. Lett. (3)

J. P. Heritage, Appl. Phys. Lett. 34, 470 (1979).
[CrossRef]

J. L. Ouder, R. W. Smith, Y. R. Shen, Appl. Phys. Lett. 34, 758 (1979).
[CrossRef]

J. J. Song, G. L. Eesley, M. D. Levenson, Appl. Phys. Lett. 29, 567 (1976).
[CrossRef]

Appl. Spectrosc. (1)

Appl. Spectrosc. Rev. (1)

M. G. Sceats, reported by A. B. Harvey, J. W. Nibler in Appl. Spectrosc. Rev. 14, 101 (1978).
[CrossRef]

IEEE J. Quantum Electron. (1)

A. Owyoung, IEEE J. Quantum Electron. QE-14, 192 (1978).
[CrossRef]

Opt, Commun. (1)

W. Zinth, A. Laubereau, W. Kaiser, Opt, Commun. 26, 457 (1978).
[CrossRef]

Opt. Commun. (1)

R. T. Lynch, S. D. Kramer, H. Lotem, N. Bloembergen, Opt. Commun. 16, 372 (1976).
[CrossRef]

Rev. Mod. Phys. (1)

A. Laubereau, W. Kaiser, Rev. Mod. Phys. 50, 607 (1978).
[CrossRef]

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Figures (4)

Fig. 1
Fig. 1

Several contributions to the CARS process are shown as time-ordered sequences of interactions. The horizontal solid lines indicate real states; dashed lines indicate the virtual states. In A, the intermediate state β is a real state; in B, it is a virtual state. The dominant contribution to the nonresonant susceptibility χNR is shown in C.

Fig. 2
Fig. 2

A schematic outline of the PUSCARS experiment using two synchronously pumped dye lasers.

Fig. 3
Fig. 3

PUSCARS signal is plotted as a function of the delay tD for several values of the detuning Δω, namely: A, 20 cm−1; B, 3 cm−1; C, 0 cm−1; D, −3 cm−1; E, −20 cm−1.

Fig. 4
Fig. 4

The PUSCARS spectrum centered at ω0 = 656 cm−1, a vibrational mode of CS2. The detuning is given by Δω = ω0ωL + ωS. Spectrum A corresponds to a delay tD = 0; in Spectrum B, tD = 20 psec. The spectra are normalized at ω0.

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