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Journal of the Optical Society of America B

Journal of the Optical Society of America B


  • Vol. 2, Iss. 4 — Apr. 1, 1985
  • pp: 674–679

Coherent interactions in pump–probe absorption measurements: the effect of phase gratings

S. L. Palfrey and T. F. Heinz  »View Author Affiliations

JOSA B, Vol. 2, Issue 4, pp. 674-679 (1985)

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We show that in order to describe completely the coherent coupling between the pump and probe pulses in a pump– probe measurement of transient absorption, the influence of induced phase gratings must be included. The importance of phase gratings is demonstrated experimentally for the case of a bleachable dye and analyzed in terms of transient four-wave mixing. These results are relevant to the interpretation of pump–probe measurements on all time scales performed with pulses from a single laser, particularly when the pulse duration is comparable with the material response time.

© 1985 Optical Society of America

Original Manuscript: September 28, 1984
Manuscript Accepted: November 13, 1984
Published: April 1, 1985

S. L. Palfrey and T. F. Heinz, "Coherent interactions in pump–probe absorption measurements: the effect of phase gratings," J. Opt. Soc. Am. B 2, 674-679 (1985)

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  1. E. P. Ippen, C. V. Shank, in Ultrashort Light Pulses, S. L. Shapiro, ed., Vol. 18 of Topics in Applied Physics (Springer-Verlag, Berlin, 1977), p. 83. [CrossRef]
  2. Z. Vardeny, J. Tauc, “Picosecond coherence coupling in the pump and probe technique,” Opt. Commun. 39, 396 (1981). [CrossRef]
  3. B. S. Wherrett, A. L. Smirl, T. F. Boggess, “Theory of degenerate four-wave mixing in picosecond excitation-probe experiments,” IEEE J. Quantum Electron. QE-19, 680 (1983), and references therein. [CrossRef]
  4. T. F. Heinz, S. L. Palfrey, K. B. Eisenthal, “Coherent coupling effects in pump–probe measurements with collinear, copropagating beams,” Opt. Lett. 9, 359 (1984). [CrossRef] [PubMed]
  5. Rigorously speaking, as is clear below, phase and amplitude gratings are associated with variations in the real and imaginary parts of the susceptibility.
  6. It should be mentioned that contributions to the coherent signal from a phase grating have been noted previously [C. V. Shank and D. H. Auston, “Parametric coupling in an optically excited plasma in Ge,” Phys. Rev. Lett. 34, 479 (1975)]. The effect that they discuss, however, depends quadratically on the induced nonlinear polarization. This is a higher-order contribution than the interference between the nonlinear polarization and the probe considered here.
  7. We neglect in this discussion the off-resonant contribution to the nonlinear susceptibility. Since this term is real and corresponds to an instantaneous response, it will not affect the signal considered here.
  8. This analysis can be extended in a straightforward fashion to the case of optically thick samples by integrating the wave equation. See, for example, the treatment in Ref. 3.
  9. H. Nakatsuka, D. Grischkowsky, A. C. Balant, “Nonlinear picosecond-pulse propagation through optical fibers with positive group velocity dispersion,” Phys. Rev. Lett. 47, 910 (1981). [CrossRef]
  10. A. J. Taylor, D. J. Erskine, C. L. Tang, “Equal-pulse correlation technique for measuring femtosecond excited state relaxation times,” Appl. Phys. Lett. 43, 989 (1983). [CrossRef]
  11. J-L. Oudar, “Coherent phenomena involved in the time-resolved optical Kerr effect,” IEEE J. Quantum Electron. QE-19, 713 (1983). [CrossRef]

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