Haijuan Wu, Zhicheng Lin, Chao Tan, Guohua Hu, Siyuan Luo, Zegao Wang
Abstract Due to the non‐complementarity of extra‐nuclear electrons, ReS 2 shows anisotropic optical property and deliver polarization‐sensitive photodetection without using complex optical components. However, the low polarization sensitivity does not satisfy to accurate identification. Herein, by employing the symmetry breaking via twisting atomic configuration, the anisotropic optical and photoresponse is improved from both the intralayer and interlayer. By twisting the ReS 2 layers, the dark current decreases by three‐orders to ≈10 pA caused by the interlayer van der Waals gap. Moreover, twisting engineering not only suppress the dark current but also improve the in‐plane optical anisotropy. The optical anisotropic factors of 60°‐twisted ReS 2 and 90°‐twisted ReS 2 are 2.5 and 6.4, respectively, which indicate that the twist angle can alter the relative orientation of the Re‐Re chains and the interface coupling intensity. Furthermore, the device exhibits polarization sensitivity, that the 90°‐twisted ReS 2 exhibited well polarization ratio of 26.8 which is much larger than the value of 5.9 in 60°‐twisted ReS 2 . Moreover, the 90°‐twisted ReS 2 homojunctions as polarization‐sensitive photodetectors in complex visual recognition tasks is validated demonstrating that the captured polarization information significantly enhances image recognition efficiency (98.6%), confirming its practical application potential in artificial intelligence visual perception tasks.