Abstract

Abstract Developing high‐performance polarization‐sensitive ultraviolet photodetectors is crucial for their application in military remote sensing, detection, bio‐inspired navigation, and machine vision. However, the significant absorption in the visible light range severely limits the application of polarization‐sensitive ultraviolet photodetectors, such as high‐quality anti‐interference imaging. Here, based on a wide‐bandgap organic semiconductor single crystal (trans‐1,2‐bis(5‐phenyldithieno[2,3‐b:3′,2′‐d]thiophen‐2‐yl)ethene, BPTTE), high‐performance polarization‐sensitive solar‐blind ultraviolet photodetectors with a dichroic ratio close to 4.26 are demonstrated. The strong anisotropy of 2D grown BPTTE single crystals in molecular vibration and optical absorption is characterized by various techniques. Under voltage modulation, stable and efficient detection of polarized light is demonstrated, attributed to the intrinsic anisotropy of transition dipole moment in the bc crystal plane, rather than other factors. Finally, high‐contrast polarimetric imaging and anti‐interference imaging are successfully demonstrated based on BPTTE single crystal photodetectors, highlighting the potential of organic semiconductors for polarization‐sensitive solar‐blind ultraviolet photodetectors.