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Journal of the Optical Society of America B

Journal of the Optical Society of America B


  • Vol. 17, Iss. 5 — May. 1, 2000
  • pp: 827–832

Coherent coupling in frequency-resolved pump–probe spectroscopy

Sander Woutersen and Huib J. Bakker  »View Author Affiliations

JOSA B, Vol. 17, Issue 5, pp. 827-832 (2000)

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We have studied the influence of coherent coupling on the transient spectra observed in optical pump–probe spectroscopy. If the pump and probe pulses have temporal overlap, a strong increase of the pump–probe signal occurs at probe frequencies close to the pump frequency. This leads to sharp peaks in the transient spectra, which might erroneously be interpreted as spectral holes. We derive an explicit expression for both the delay dependence and the probe-frequency dependence of the pump–probe signal for the case of a homogeneously broadened absorption band. As an illustration, we use this expression to estimate the effect of coherent coupling on vibrational pump–probe spectroscopy on the OH stretch band of hydrogen-bonded systems.

© 2000 Optical Society of America

OCIS Codes
(020.1670) Atomic and molecular physics : Coherent optical effects
(300.0300) Spectroscopy : Spectroscopy
(320.7150) Ultrafast optics : Ultrafast spectroscopy

Sander Woutersen and Huib J. Bakker, "Coherent coupling in frequency-resolved pump–probe spectroscopy," J. Opt. Soc. Am. B 17, 827-832 (2000)

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  1. H. J. Eichler, P. Günter, and D. W. Pohl, Laser-Induced Dynamic Gratings (Springer-Verlag, Berlin, 1986).
  2. A. von Jena and H. E. Lessing, “Coherent coupling effects in picosecond absorption experiments,” Appl. Phys. 19, 131–144 (1979). [CrossRef]
  3. Z. Vardeny and J. Tauc, “Picosecond coherence coupling in the pump and probe technique,” Opt. Commun. 39, 396–400 (1981). [CrossRef]
  4. B. S. Wherrett, A. L. Smirl, and T. F. Boggess, “Theory of degenerate four-wave mixing in picosecond excitation–probe experiments,” IEEE J. Quantum Electron. 19, 680–690 (1983). [CrossRef]
  5. R. W. Boyd and S. Mukamel, “Origin of spectral holes in pump–probe studies of homogeneously broadened lines,” Phys. Rev. A 29, 1973–1983 (1983). [CrossRef]
  6. C. H. Brito Cruz, J. P. Gordon, P. C. Becker, R. L. Fork, and C. V. Shank, “Dynamics of spectral hole burning,” IEEE J. Quantum Electron. 24, 261–266 (1988). [CrossRef]
  7. H. A. Ferwerda, J. Terpstra, and D. A. Wiersma, “Discussion of a ‘coherent artifact’ in four-wave mixing experiments,” J. Chem. Phys. 91, 3296–3305 (1989). [CrossRef]
  8. E. Gaižauskas and L. Valkūnas, “Coherent transients of pump–probe spectroscopy in two-level approximation,” Opt. Commun. 109, 75–80 (1994). [CrossRef]
  9. S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford Univ. Press, Oxford, UK, 1995).
  10. M. Bonn, S. Woutersen, and H. J. Bakker, “Coherent picosecond vibron polaritons as probes of vibrational lifetimes,” Opt. Commun. 147, 138–142 (1998). [CrossRef]
  11. R. Laenen and C. Rauscher, “Numerical study of induced polarization dynamics in ultrafast spectral hole-burning experiments,” Chem. Phys. 230, 223–236 (1998). [CrossRef]
  12. R. Laenen, C. Rauscher, and A. Laubereau, “Transient hole burning in the infrared in an ethanol solution,” J. Phys. Chem. A 101, 3201–3206 (1997). [CrossRef]
  13. S. Woutersen, U. Emmerichs, and H. J. Bakker, “A femtosecond mid-infrared pump–probe study of hydrogen-bonding in ethanol,” J. Chem. Phys. 107, 1483–1490 (1997). [CrossRef]
  14. R. Laenen, C. Rauscher, and A. Laubereau, “Vibrational energy redistribution of ethanol oligomers and dissociation of hydrogen bonds after ultrafast infrared excitation,” Chem. Phys. Lett. 283, 7–14 (1998). [CrossRef]
  15. R. Laenen, C. Rauscher, and A. Laubereau, “Dynamics of local substructures in water observed by ultrafast infrared hole burning,” Phys. Rev. Lett. 80, 2622–2625 (1998). [CrossRef]
  16. S. Woutersen, U. Emmerichs, H.-K. Nienhuys, and H. J. Bakker, “Anomalous temperature dependence of vibrational lifetimes in water and ice,” Phys. Rev. Lett. 81, 1106–1109 (1998). [CrossRef]
  17. G. M. Gale, G. Gallot, F. Hache, N. Lascoux, S. Bratos, and J.-C. Leicknam, “Femtosecond dynamics of hydrogen bonds in liquid water: a real time study,” Phys. Rev. Lett. 82, 1068–1071 (1999). [CrossRef]
  18. H. R. Wyss and M. Falk, “Infrared spectra of HDO in water and in NaCl solution,” Can. J. Chem. 48, 607–614 (1970). [CrossRef]
  19. H. Graener, G. Seifert, and A. Laubereau, “New spectroscopy of water using tunable picosecond pulses in the infrared,” Phys. Rev. Lett. 66, 2092–2095 (1991). [CrossRef] [PubMed]

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