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Abstract The presence of in-plane chiral effects, hence spin–orbit coupling, is evident in the changes in the photocurrent produced in a TiS 3 (001) field-effect phototransistor with left versus right circularly polarized light. The direction of the photocurrent is protected by the presence of strong spin–orbit coupling and the anisotropy of the band structure as indicated in NanoARPES measurements. Dark electronic transport measurements indicate that TiS 3 is n-type and has an electron mobility in the range of 1–6 cm 2 V −1 s −1 . I – V measurements under laser illumination indicate the photocurrent exhibits a bias directionality dependence, reminiscent of bipolar spin diode behavior. Because the TiS 3 contains no heavy elements, the presence of spin–orbit coupling must be attributed to the observed loss of inversion symmetry at the TiS 3 (001) surface. 

Theoretical and experimental investigations of various exfoliated samples taken from layered In₄Se₃crystals are performed. In spite of the ionic character of interlayer interactions in In₄Se₃and hence much higher calculated cleavage energies compared to graphite, it is possible to produce few‐nanometer‐thick flakes of In₄Se₃by mechanical exfoliation of its bulk crystals. The In₄Se₃flakes exfoliated on Si/SiO₂have anisotropic electronic properties and exhibit field‐effect electron mobilities of about 50 cm² V⁻¹ s⁻¹at room temperature, which are comparable with other popular transition metal chalcogenide (TMC) electronic materials, such as MoS₂and TiS₃. In₄Se₃devices exhibit a visible range photoresponse on a timescale of less than 30 ms. The photoresponse depends on the polarization of the excitation light consistent with symmetry‐dependent band structure calculations for the most expectedaccleavage plane. These results demonstrate that mechanical exfoliation of layered ionic In₄Se₃crystals is possible, while the fast anisotropic photoresponse makes In₄Se₃a competitive electronic material, in the TMC family, for emerging optoelectronic device applications.