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Optical Materials Express

Optical Materials Express

  • Editor: David J. Hagan
  • Vol. 1, Iss. 5 — Sep. 1, 2011
  • pp: 953–961

Tin hypothiodiphosphate: nonlinear response in the sub-100 fs time domain

M. Imlau, V. Dieckmann, H. Badorreck, and A. Shumelyuk  »View Author Affiliations

Optical Materials Express, Vol. 1, Issue 5, pp. 953-961 (2011)

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The interaction of sub-100 fs light pulses (τp ≲ 75 fs) with single crystals of nominally undoped tin hypothiodiphosphate, Sn2P2S6, is studied in the near-infrared spectral range (590 – 1630 nm). A predominant contribution of the two-photon absorption (TPA) is verified in the measurements of the sample transmission as a function of pulse intensity and of the time delay between pump and probe pulses. Scans over the photon energy show that the two-photon absorption coefficient β increases in a superlinear way for photon energies h̄ω exceeding Eg/2; for any quantum energy it is nearly independent of propagation direction and polarization of the incident beam. Such a behavior is qualitatively similar to that predicted by perturbation theory within models with allowed-forbidden transitions. The TPA coefficient saturates at a maximum value of β ≈ 8 cm GW−1 at h̄ω ≈ 1.80 eV. It drops when reaching the bandgap Eg. Using pump-probe measurements at 626 nm, a transient absorption is verified that persists for probe pulse delays much longer than the pump pulse duration, up to 2.5 ns. We discuss our results in the framework of the microscopic structure of Sn2P2S6 with emphasis on the optical generation of S small hole polarons.

© 2011 OSA

OCIS Codes
(160.4670) Materials : Optical materials
(190.7110) Nonlinear optics : Ultrafast nonlinear optics
(300.6420) Spectroscopy : Spectroscopy, nonlinear
(300.6530) Spectroscopy : Spectroscopy, ultrafast
(260.7120) Physical optics : Ultrafast phenomena

ToC Category:
Nonlinear Optical Materials

Original Manuscript: July 15, 2011
Revised Manuscript: August 9, 2011
Manuscript Accepted: August 10, 2011
Published: August 16, 2011

M. Imlau, V. Dieckmann, H. Badorreck, and A. Shumelyuk, "Tin hypothiodiphosphate: nonlinear response in the sub-100 fs time domain," Opt. Mater. Express 1, 953-961 (2011)

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