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Abstract Above‐band gap optical excitation of non‐centrosymmetric semiconductors can lead to the spatial shift of the center of electron charge in a process known as shift current. Shift current is investigated in single‐crystal SnS₂, a layered semiconductor with the band gap of ≈2.3 eV, by THz emission spectroscopy and first principles density functional theory (DFT). It is observed that normal incidence excitation with above gap (400 nm; 3.1 eV) pulses results in THz emission from 2H SnS₂() polytype, where such emission is nominally forbidden by symmetry. It is argued that the underlying symmetry breaking arises due to the presence of stacking faults that are known to be ubiquitous in SnS₂single crystals and construct a possible structural model of a stacking fault with symmetry properties consistent with the experimental observations. In addition to shift current, it is observed THz emission by optical rectification excited by below band gap (800 nm; 1.55 eV) pulses but it requires excitation fluence more than two orders of magnitude higher to produce same signal amplitude. These results suggest that ultrafast shift current in which can be excited with visible light in blue–green portion of the spectrum makes SnS₂a promising source material for THz photonics. 

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.