Symmetry Breaking in Twisted Mixed-Dimensional Heterostructure Interfaces for Multifunctional Polarization-Sensitive Photodetection

Moiré superlattices, created by stacking different van der Waals materials at twist angles, have emerged as a versatile platform for exploring intriguing phenomena such as topological properties, superconductivity, the quantum anomalous Hall effect, and the unconventional Stark effect. Additionally, the formation of moiré superlattice potential can generate spontaneous symmetry breaking, leading to an anisotropic optical response and electronic transport behavior. Herein, we propose a two-step chemical vapor deposition (CVD) strategy for synthesizing WS2/Sb2S3 moiré superlattices. Density functional theory calculations show that the moiré potential and interlayer distance at the WS2/Sb2S3 interface can generate anisotropic electronic states. The atomic-resolution HAADF-STEM image clearly reveals angle-dependent complicated moiré periodicity. The polarization-dependent second harmonic generation, Raman, photoluminescence, and absorption spectroscopy of the WS2/Sb2S3 heterostructure confirm optical anisotropic behavior due to symmetry breaking by the moiré superlattice formation. The WS2/Sb2S3 device exhibits high on/off ratios up to 106, a relatively low leakage current of 10–13 A, and a broadband optoelectronic response range from 360 to 914 nm. Notably, the broken symmetry by C2-symmetric Sb2S3 nanowires grown on a C3-symmetric WS2 nanosheet endows the WS2/Sb2S3 photodetector with strong polarization-dependent photocurrent intensity and high-resolution polarization imaging capability. Our study demonstrates the potential for constructing multifunctional moiré materials by incorporating symmetry-breaking engineering.