Applied Physics B

, Volume 63, Issue 1, pp 62–68 | Cite as

Ultrabroadband single-pulse CARS of liquids using a spatially dispersive Stokes beam

  • V. H. Astinov
  • G. M. Georgiev


A double-channel spectrometer, which enables to acquire ultrabroadband single-pulse spectra of liquids by Coherent Anti-Stokes Raman Spectroscopy (CARS), is described. The method used to fulfill the phase-matching condition is based on the fact that the CARS efficiency in dispersive media is the largest when the interactive waves cross each other under frequency-determined angles. The dependence of the spatial separation between the pump and Stokes beam, in front of the crossing CARS lens, due to their frequency difference is analysed. It is shown that the different spectral components of an ultrabroadband Stokes source have phase-matched the CARS process when they are laterally shifted by a conjugated prism pair and focused into the sample. The method is tested in the spectral region 2800–3800 cm−1 of a non-resonant medium (CCl4) using an ultrabroadband dye laser (1000 cm−1 FWHM). The influence of the Stokes beam spatial dispersion on the width of CARS generation is demonstrated. By this method, 1060 cm−1 wide single-pulse spectra of the OH stretching vibration of liquid water are obtained for the first time. The ratio between the resonant and non-resonant part of the third-order susceptibility in water and methanol is determined.


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  1. 1.
    J.P. Taran: NATO/ASI Conf. on Applied Laser Spectroscopy, San Miniato (Sept. 1989)Google Scholar
  2. 2.
    A. Tabyaoui, B. Lavorel, R. Saint-Loup, M. Rotger: J Raman Spectrosc.25, 255 (1994)Google Scholar
  3. 3.
    D.V. Murphy, M.B. Long, R.K. Chang, A.C. Eckbreth: Opt. Lett.4, 167 (1979)Google Scholar
  4. 4.
    V. Kornas, A. Roth, H.F. Döbele, G. Proß: Plasma Chem. Plasma Process.15, 71 (1995) V. Kornas, V. Schulz-von der Gathen, T. Bornemann, H.F. Döbele, G. Proß: Plasma Chem. Plasma Process.11, 171 (1991)Google Scholar
  5. 5.
    W.B. Roh, P.W. Schreiber, J.P.E. Taran: Appl. Phys. Lett.29, 174 (1976)Google Scholar
  6. 6.
    R. Bombach, T. Gerber, B. Hemmerling, W. Hubschmid: Appl. Phys. B51, 59 (1990)Google Scholar
  7. 7.
    F.M. Porter, D.A. Greenhalgh, P.J. Stepford, D.R. Williams, C.A. Baker: Appl. Phys. B51, 31 (1990)Google Scholar
  8. 8.
    K. Akihama, T. Asai: Appl. Opt.29, 3143 (1990)Google Scholar
  9. 9.
    M. Péalat, M. Lefebvre: Appl. Phys. B53, 23 (1991)Google Scholar
  10. 10.
    K.A. Marko, L. Rimai: Opt. Lett.4, 211 (1979) D. Klick, K.A. Marko, L. Rimai: Appl. Opt.20, 1178 (1981)Google Scholar
  11. 11.
    Th. Bouché, Th. Treier, B. Lange, J. Wolfrum, E.U. Franck, W. Schilling: Appl. Phys. B50, 527 (1990)Google Scholar
  12. 12.
    T. Dreier, G. Schiff: Appl. Phys. B55, 388 (1992)Google Scholar
  13. 13.
    M.A. Yaratich: Mol. Phys.38, 625 (1979)Google Scholar
  14. 14.
    A.C. Eckbreth, T.J. Anderson: Appl. Opt.24, 2731 (1985) A.C. Eckbreth, T.J. Anderson: Opt. Lett.11, 496 (1986)Google Scholar
  15. 15.
    S. Kröl, P.-E. Bengtsson, M. Aldén, D. Nilsson: Appl. Phys. B51, 25 (1990)Google Scholar
  16. 16.
    F. Grisch, M. Péalat, P. Bouchardy, J.P. Taran, I. Bar, D. Heflinger, S. Rosenwaks: Appl. Phys. Lett.59, 3516 (1991)Google Scholar
  17. 17.
    D.S. Moore, S.C. Schmidt, M.S. Shaw: J. Chem. Phys.101, 3488 (1994) D.S. Moore, S.C. Schmidt, J.W. Shaner: Phys. Rev. Lett.50, 1819 (1983)Google Scholar
  18. 18.
    D.E. Hare, D.D. Dlott: Appl. Phys. Lett.64, 715 (1994) D.E. Hare, J. Franken, D.D. Dlott: J. Appl. Phys.77, 5950 (1995)Google Scholar
  19. 19.
    P. Kukk, A. Lohmus, J. Korppi-Tommola: Appl. Spectrosc.44, 1381 (1990)Google Scholar
  20. 20.
    S.A. Akhmanov, A.A. Ivanov, N.I. Koroteev, S.F. Mironov, A.I. Fishman: J. Mol. Liquids53, 111 (1992)Google Scholar
  21. 21.
    A.I. Fishman, S.F. Mironov: J. Raman Spectrosc.25, 267 (1994)Google Scholar
  22. 22.
    A. Weippert, W. Kiefer: J. Raman Spectrosc.23, 713 (1992)Google Scholar
  23. 23.
    T. Bischof, W. Kiefer: J. Raman Spectrosc.25, 565 (1994)Google Scholar
  24. 24.
    I. Itzkan, D.A. Leonard: Appl. Phys. Lett.26, 106 (1975)Google Scholar
  25. 25.
    J.-L. Oudar, R.W. Smith, Y.R. Shen: Appl. Phys. Lett.34, 758 (1979)Google Scholar
  26. 26.
    W. Li, H.-G. Purucker, A. Laubereau: Opt. Commun.94, 300 (1992)Google Scholar
  27. 27.
    N.I. Koroteev, M. Endemann, R.L. Byer: Phys. Rev. Lett.43, 398 (1979)Google Scholar
  28. 28.
    A.F. Bunkin, D.V. Vlasov, A.S. Galumian, K.O. Surskii: Opt. Spectrosk.58, 481 (1985)Google Scholar
  29. 29.
    A.F. Bunkin, A.S. Galumian, H.A. Zumanov, D.V. Maltzev, K.O. Surskii: Opt. Spectrosk.62, 1249 (1987)Google Scholar
  30. 30.
    A.F. Bunkin, A.S. Galumian, H.A. Zumanov, D.V. Maltzev, K.O. Surskii: Opt. Spectrosk.60, 960 (1986)Google Scholar
  31. 31.
    A. Lau, W. Werncke, J. Klein, M. Pfeiffer: Opt. Commun.21, 399 (1977)Google Scholar
  32. 32.
    M. Pfeiffer, A. Lau, W. Werncke: J. Raman Spectrosc.21, 815 (1990)Google Scholar
  33. 33.
    B.N. Toleutaev, T. Tahara, H. Hamaguchi: Appl. Phys. B59, 369 (1994)Google Scholar
  34. 34.
    V.H. Astinov, G.M. Georgiev: General Conf. of the Balkan Physical Union BPU-2, Izmir, Turkey (Sept. 1994)Google Scholar
  35. 35.
    V.H. Astinov, G.M. Georgiev: Spectrosc. Lett.29, N°1 (1996) (in press)Google Scholar
  36. 36.
    V.H. Astinov: Opt. Commun.118, 297 (1995)Google Scholar
  37. 37.
    S.A. Akhmanov, N.I. Koroteev:Methods of Nonlinear Optics in Light Scattering Spectroscopy (Nauka, Moscow 1981)Google Scholar
  38. 38.
    B.P. Nickolskii (ed.):Handbook of Chemistry, Vol. 1 (Chemistry, Leningrad 1971)Google Scholar
  39. 39.
    M.B. Danailov, I.P. Christov: Appl. Phys. B51, 300 (1990)Google Scholar
  40. 40.
    Optisches Glas, Catalog (Spezial-glas GmbH, Mainz 1985)Google Scholar
  41. 41.
    Optics Guide 5 (Melles Griot 1994) Chap. 3, p. 8Google Scholar
  42. 42.
    G. Laufer, R.B. Miles: Opt. Commun.28, 250 (1979)Google Scholar
  43. 43.
    M. Stoev, J. Maria, V. Astinov, Zh. Nickolov, G. Georgiev: J. Mol. Struct.293, 231 (1993)Google Scholar

Copyright information

© Springer-Verlag 1996

Authors and Affiliations

  • V. H. Astinov
    • 1
  • G. M. Georgiev
    • 1
  1. 1.Quantum Electronics Department, Faculty of PhysicsSofia UniversitySofiaBulgaria

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