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

Autor(en): Imlau, M. 
Dieckmann, V.
Badorreck, H.
Shumelyuk, A.
Stichwörter: ABSORPTION; CHARGE-TRANSFER; Materials Science; Materials Science, Multidisciplinary; Optics; SMALL POLARONS; SN2P2S6
Erscheinungsdatum: 2011
Volumen: 1
Ausgabe: 5
Startseite: 953
Seitenende: 961
The interaction of sub-100 fs light pulses (tau(p) less than or similar to 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 beta increases in a superlinear way for photon energies (h) over bar omega. exceeding E-g/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 beta approximate to 8 cm GW(-1) at (h) over bar omega approximate to 1.80 eV. It drops when reaching the bandgap E-g. 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. (C) 2011 Optical Society of America
ISSN: 21593930
DOI: 10.1364/OME.1.000953

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