We report on THz emission in single-crystalline SnS2 in response to above bandgap excitation. Symmetry properties of THz generation suggest that its origin is an ultrafast surface shift current, a 2nd order nonlinear effect that can occur as a result of above-gap photoexcitation of a non-centrosymmetric semiconductor. Multilayer SnS2 can exist in several polytypes that differ in the layer stacking. Of those polytypes, 2H and 18R are centrosymmetric while 4H is not. While Raman spectroscopy suggests that the single crystalline SnS2 in our experiments is 2H, its THz emission has symmetry that are fully consistent with the P3m1 phase of 4H polytype. We hypothesize that the stacking disorder, where strain-free stacking faults that interrupt regions of 2H polytype, can break inversion symmetry and result in THz emission. These results lay the foundations for application of SnS2 as an efficient, stable, flexible THz source material, and highlight the use of THz spectroscopy as a sensitive tool for establishing symmetry properties of materials.
Use of nanomaterials for photocatalysis faces challenges such as complex synthesis, high cost, low scalability, and dependance on UV radiation for initiating the photocatalytic activity. We recently demonstrated scalable, one-pot syntheses of one-dimensional (1D) lepidocrocite-based nanofilaments (NFs), 1DL NFs, that have the potential to overcome some of the challenges. 1DL NFs are exceptionally stable in water, have a large surface to volume ratio, and sub-square-nanometer cross sections. Initial reports show the semiconducting nature of this material, with an indirect band gap energy of 4.0 eV, one of the highest ever reported for a titania material. In this work, we present a study of the electronic and optical properties of these newly discovered 1DL NFs using ultrafast transient optical absorption. We show that despite the large band gap of this material, sub-gap states can be accessed with visible light illumination only, and photoexcited species reveal decay times in the nanosecond scale. Long lived photoexcitations in the visible range, without assistance by UV illumination, pave the way for possible application in photocatalysis.
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