Abstract

Intense pulses for two-color pump–probe spectroscopy in the mid-infrared spectral region are generated by optical parametric oscillator (OPO) and optical parametric amplifier (OPA) stages. Synchronous pumping of two OPO’s in parallel delivers tunable pulses in the range 1.2–1.7 μm with a duration of 300 fs. Subsequent frequency conversion in two OPA’s consisting, respectively, of two- and four-crystal setups of AgGaS2 yields pulses in the wavelength interval 2.6–7 μm with a duration of 0.5 ps and single-pulse energy up to 2 μJ. By simple changes of the operating conditions of the two OPO’s, independent adjustments of the resulting mid-infrared pulse duration are achieved that range from 0.5 to 2.6 ps while the pulse duration–bandwidth product of the pulses varies from 0.6 to 1.2.

© 1998 Optical Society of America

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References

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  1. See, for example, Ultrafast Phenomena IX, P. F. Barbara, W. H. Knox, G. A. Mourou, and A. H. Zewail, eds. (Springer-Verlag, Berlin, 1994).
  2. P. Hamm, C. Lauterwasser, and W. Zinth, Opt. Lett. 18, 1943 (1993); F. Seifert, V. Petrov, and M. Woerner, Opt. Lett. 19, 2009 (1994).
    [CrossRef] [PubMed]
  3. C. Ludwig, W. Frey, M. Wörner, and T. Elsässer, Opt. Commun. 102, 447 (1993).
    [CrossRef]
  4. T. P. Dougherty and E. J. Heilweil, Opt. Lett. 19, 129 (1994).
    [CrossRef]
  5. H. Graener, R. Dohlus, and A. Laubereau, Chem. Phys. Lett. 140, 306 (1987).
    [CrossRef]
  6. F. Lindenberger, R. Stöckl, R. Laenen, and A. Laubereau, Opt. Commun. 117, 268 (1995).
    [CrossRef]
  7. K. Wolfrum, R. Laenen, and A. Laubereau, Opt. Commun. 97, 41 (1993).
    [CrossRef]
  8. J. D. V. Khaydarov, J. H. Andrews, and K. D. Singer, Opt. Lett. 19, 831 (1994).
    [CrossRef] [PubMed]
  9. C. Rauscher, T. Roth, R. Laenen, and A. Laubereau, Opt. Lett. 20, 2003 (1995); R. Laenen and T. Roth, J. Opt. Soc. Am. B 14, 454 (1997).
    [CrossRef] [PubMed]
  10. R. Laenen and A. Laubereau, Opt. Lett. 19, 1553 (1994).
    [CrossRef] [PubMed]
  11. D. E. Spence, P. E. Powers, and C. L. Tang, Opt. Commun. 118, 69 (1995).
    [CrossRef]
  12. R. Laenen, K. Wolfrum, A. Seilmeier, and A. Laubereau, J. Opt. Soc. Am. B 10, 2151 (1993).
    [CrossRef]
  13. R. Laenen, H. Graener, and A. Laubereau, in Proceedings of UPS ’91, A. Laubereau and A. Seilmeier, eds. (IOP, Bristol, UK, 1992), p. 63.
  14. R. Laenen, K. Simeonidis, and C. Rauscher, IEEE J. Select. Topics Quantum Electron. 2, 487 (1996).
    [CrossRef]
  15. Schott Inc., Mainz, Germany, data sheet (1984).
  16. J. I. Dadap, G. B. Focht, D. H. Reitze, and M. C. Downer, Opt. Lett. 16, 499 (1991).
    [CrossRef] [PubMed]
  17. A. Reuther, A. Laubereau, and D. N. Nikogosyan, Opt. Commun. 141, 180 (1997).
    [CrossRef]
  18. C. Rauscher and R. Laenen, J. Appl. Phys. 81, 2818 (1997).
    [CrossRef]
  19. A. Leitenstorfer, C. Fürst, and A. Laubereau, Opt. Lett. 20, 916 (1995).
    [CrossRef] [PubMed]

1997 (2)

A. Reuther, A. Laubereau, and D. N. Nikogosyan, Opt. Commun. 141, 180 (1997).
[CrossRef]

C. Rauscher and R. Laenen, J. Appl. Phys. 81, 2818 (1997).
[CrossRef]

1996 (1)

R. Laenen, K. Simeonidis, and C. Rauscher, IEEE J. Select. Topics Quantum Electron. 2, 487 (1996).
[CrossRef]

1995 (3)

A. Leitenstorfer, C. Fürst, and A. Laubereau, Opt. Lett. 20, 916 (1995).
[CrossRef] [PubMed]

F. Lindenberger, R. Stöckl, R. Laenen, and A. Laubereau, Opt. Commun. 117, 268 (1995).
[CrossRef]

D. E. Spence, P. E. Powers, and C. L. Tang, Opt. Commun. 118, 69 (1995).
[CrossRef]

1994 (3)

1993 (3)

K. Wolfrum, R. Laenen, and A. Laubereau, Opt. Commun. 97, 41 (1993).
[CrossRef]

R. Laenen, K. Wolfrum, A. Seilmeier, and A. Laubereau, J. Opt. Soc. Am. B 10, 2151 (1993).
[CrossRef]

C. Ludwig, W. Frey, M. Wörner, and T. Elsässer, Opt. Commun. 102, 447 (1993).
[CrossRef]

1991 (1)

1987 (1)

H. Graener, R. Dohlus, and A. Laubereau, Chem. Phys. Lett. 140, 306 (1987).
[CrossRef]

Andrews, J. H.

Dadap, J. I.

Dohlus, R.

H. Graener, R. Dohlus, and A. Laubereau, Chem. Phys. Lett. 140, 306 (1987).
[CrossRef]

Dougherty, T. P.

Downer, M. C.

Elsässer, T.

C. Ludwig, W. Frey, M. Wörner, and T. Elsässer, Opt. Commun. 102, 447 (1993).
[CrossRef]

Focht, G. B.

Frey, W.

C. Ludwig, W. Frey, M. Wörner, and T. Elsässer, Opt. Commun. 102, 447 (1993).
[CrossRef]

Fürst, C.

Graener, H.

H. Graener, R. Dohlus, and A. Laubereau, Chem. Phys. Lett. 140, 306 (1987).
[CrossRef]

Heilweil, E. J.

Khaydarov, J. D. V.

Laenen, R.

C. Rauscher and R. Laenen, J. Appl. Phys. 81, 2818 (1997).
[CrossRef]

R. Laenen, K. Simeonidis, and C. Rauscher, IEEE J. Select. Topics Quantum Electron. 2, 487 (1996).
[CrossRef]

F. Lindenberger, R. Stöckl, R. Laenen, and A. Laubereau, Opt. Commun. 117, 268 (1995).
[CrossRef]

R. Laenen and A. Laubereau, Opt. Lett. 19, 1553 (1994).
[CrossRef] [PubMed]

R. Laenen, K. Wolfrum, A. Seilmeier, and A. Laubereau, J. Opt. Soc. Am. B 10, 2151 (1993).
[CrossRef]

K. Wolfrum, R. Laenen, and A. Laubereau, Opt. Commun. 97, 41 (1993).
[CrossRef]

Laubereau, A.

A. Reuther, A. Laubereau, and D. N. Nikogosyan, Opt. Commun. 141, 180 (1997).
[CrossRef]

A. Leitenstorfer, C. Fürst, and A. Laubereau, Opt. Lett. 20, 916 (1995).
[CrossRef] [PubMed]

F. Lindenberger, R. Stöckl, R. Laenen, and A. Laubereau, Opt. Commun. 117, 268 (1995).
[CrossRef]

R. Laenen and A. Laubereau, Opt. Lett. 19, 1553 (1994).
[CrossRef] [PubMed]

R. Laenen, K. Wolfrum, A. Seilmeier, and A. Laubereau, J. Opt. Soc. Am. B 10, 2151 (1993).
[CrossRef]

K. Wolfrum, R. Laenen, and A. Laubereau, Opt. Commun. 97, 41 (1993).
[CrossRef]

H. Graener, R. Dohlus, and A. Laubereau, Chem. Phys. Lett. 140, 306 (1987).
[CrossRef]

Leitenstorfer, A.

Lindenberger, F.

F. Lindenberger, R. Stöckl, R. Laenen, and A. Laubereau, Opt. Commun. 117, 268 (1995).
[CrossRef]

Ludwig, C.

C. Ludwig, W. Frey, M. Wörner, and T. Elsässer, Opt. Commun. 102, 447 (1993).
[CrossRef]

Nikogosyan, D. N.

A. Reuther, A. Laubereau, and D. N. Nikogosyan, Opt. Commun. 141, 180 (1997).
[CrossRef]

Powers, P. E.

D. E. Spence, P. E. Powers, and C. L. Tang, Opt. Commun. 118, 69 (1995).
[CrossRef]

Rauscher, C.

C. Rauscher and R. Laenen, J. Appl. Phys. 81, 2818 (1997).
[CrossRef]

R. Laenen, K. Simeonidis, and C. Rauscher, IEEE J. Select. Topics Quantum Electron. 2, 487 (1996).
[CrossRef]

Reitze, D. H.

Reuther, A.

A. Reuther, A. Laubereau, and D. N. Nikogosyan, Opt. Commun. 141, 180 (1997).
[CrossRef]

Seilmeier, A.

Simeonidis, K.

R. Laenen, K. Simeonidis, and C. Rauscher, IEEE J. Select. Topics Quantum Electron. 2, 487 (1996).
[CrossRef]

Singer, K. D.

Spence, D. E.

D. E. Spence, P. E. Powers, and C. L. Tang, Opt. Commun. 118, 69 (1995).
[CrossRef]

Stöckl, R.

F. Lindenberger, R. Stöckl, R. Laenen, and A. Laubereau, Opt. Commun. 117, 268 (1995).
[CrossRef]

Tang, C. L.

D. E. Spence, P. E. Powers, and C. L. Tang, Opt. Commun. 118, 69 (1995).
[CrossRef]

Wolfrum, K.

Wörner, M.

C. Ludwig, W. Frey, M. Wörner, and T. Elsässer, Opt. Commun. 102, 447 (1993).
[CrossRef]

Chem. Phys. Lett. (1)

H. Graener, R. Dohlus, and A. Laubereau, Chem. Phys. Lett. 140, 306 (1987).
[CrossRef]

IEEE J. Select. Topics Quantum Electron. (1)

R. Laenen, K. Simeonidis, and C. Rauscher, IEEE J. Select. Topics Quantum Electron. 2, 487 (1996).
[CrossRef]

J. Appl. Phys. (1)

C. Rauscher and R. Laenen, J. Appl. Phys. 81, 2818 (1997).
[CrossRef]

J. Opt. Soc. Am. B (1)

Opt. Commun. (5)

D. E. Spence, P. E. Powers, and C. L. Tang, Opt. Commun. 118, 69 (1995).
[CrossRef]

A. Reuther, A. Laubereau, and D. N. Nikogosyan, Opt. Commun. 141, 180 (1997).
[CrossRef]

F. Lindenberger, R. Stöckl, R. Laenen, and A. Laubereau, Opt. Commun. 117, 268 (1995).
[CrossRef]

K. Wolfrum, R. Laenen, and A. Laubereau, Opt. Commun. 97, 41 (1993).
[CrossRef]

C. Ludwig, W. Frey, M. Wörner, and T. Elsässer, Opt. Commun. 102, 447 (1993).
[CrossRef]

Opt. Lett. (5)

Other (5)

R. Laenen, H. Graener, and A. Laubereau, in Proceedings of UPS ’91, A. Laubereau and A. Seilmeier, eds. (IOP, Bristol, UK, 1992), p. 63.

Schott Inc., Mainz, Germany, data sheet (1984).

C. Rauscher, T. Roth, R. Laenen, and A. Laubereau, Opt. Lett. 20, 2003 (1995); R. Laenen and T. Roth, J. Opt. Soc. Am. B 14, 454 (1997).
[CrossRef] [PubMed]

See, for example, Ultrafast Phenomena IX, P. F. Barbara, W. H. Knox, G. A. Mourou, and A. H. Zewail, eds. (Springer-Verlag, Berlin, 1994).

P. Hamm, C. Lauterwasser, and W. Zinth, Opt. Lett. 18, 1943 (1993); F. Seifert, V. Petrov, and M. Woerner, Opt. Lett. 19, 2009 (1994).
[CrossRef] [PubMed]

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Figures (4)

Fig. 1
Fig. 1

Schematic of the experimental setup for generation of two independently tunable mid-IR pulses with adjustable duration designed for two-color pump–probe spectroscopy in the mid-IR: SPS, single-pulse selector; SHG, second-harmonic generation; D1–D5, detectors; P1–P5, polarizers; L1–L3, half-wave plates; VD, variable optical delay.

Fig. 2
Fig. 2

(a) Schematic of the noncollinearly pumped, singly resonant OPO. The OPO consists of two mirrors, M1 (R=80%; r=) and M2 (high-reflecting; r=-200 mm), lens L1 (f=200 mm), and a nonlinear crystal (KTP). (b) Schematic of the improved setup of OPA II generating the pump pulse; two pairs of two short nonlinear crystals (3 mm of AgGaS2) with a short-pass filter (WG) between them to absorb the idler component are used to reduce dispersive pulse lengthening. The desired mid-IR idler pulse is generated in the final amplification step. VD1, VD2, variable delays; DM, dichroic mirror with absorption in the mid-infrared.

Fig. 3
Fig. 3

(a) Cross-correlation data for the pump–probe setup taken at νPu=3330 cm-1 and νPr=3700 cm-1; the zero setting of the time delay and the duration of the pulses are deduced from the pump-induced two-photon absorption of the probe in i-Ge. A FWHM of the correlation function of, respectively, 0.9±0.1 ps (filled squares, solid curve) and 3.2±0.4 ps (open circles, dashed curve) is measured for well-defined different operating conditions of the OPO’s; theoretical curves calculated from a three-level model in which two-photon interband excitation of Ge and intraband absorption of generated long-lived free carriers are shown. (b) Sum-frequency spectra of the amplified OPO pulse of the pump branch (signal output of OPA II) mixed with a fundamental laser as a measure of the spectrum of the pump pulse (OPA II idler) for two different OPO I settings: tPu=0.6 ps, measuring a spectral width of 28 cm-1 (filled squares, solid curve), and tPu=2.6 ps, with a spectral width of 23 cm-1 (open circles, dashed curve); experimental points and fitted Gaussian curves. Inset, corresponding experimental data for OPA I taken at the same frequency, resulting in a spectral width of 34 cm-1 (filled squares; tPr=0.5 ps) and 14 cm-1 (open circles; tPr=2.6 ps).

Fig. 4
Fig. 4

Measured mid-IR pump pulse duration (left-hand ordinate scale, filled squares) and spectral width of the corresponding OPA II signal pulse (right-hand ordinate scale, hollow circles) versus frequency setting. The shortest pulse duration of 0.5±0.1 ps refers to an energy of 2 μJ. The data are taken with νPr=3700 cm-1; curves are drawn as a guide for the eye.

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