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Highly Polarized Photoelectrical Response in vdW ZrS3 Nanoribbons

2D anisotropic materials, such as black phosphorus, ReS2, and GaTe, have been shown to exhibit exciting direction‐ and polarization‐sensitive material properties. Highly crystalline chemical‐vapor‐transport‐grown ZrS3 crystals exhibit large optical‐absorption‐coefficient anisotropy, which doubles under resonance conditions. The observed optical anisotropy manifests itself in angle‐resolved photocurrent density polar plots with dichroic ratio (Ipb/Ipa) of 1.73 excited by a laser source of λ = 450 nm and 1.14 by λ = 532 nm. The optical absorption and electronic dichroic response are fully explained through detailed band structure and polarization‐sensitive optical‐absorption‐spectrum calculations. Not only is the family of 2D anisotropic semiconductors expanded into Zr‐based trichalcogenides but fundamental insights on how crystalline anisotropy, optical absorption dichroism, and generated photocurrents are interrelated in van der Waals Zr‐based trichalcogenides materials are also provided.