Alternating BiI3–BiI van der Waals Photodetector with Low Dark Current and High-Performance Photodetection

The emerging two-dimensional (2D) van der Waals (vdW) materials and their heterostructures hold great promise for optoelectronics and photonic applications beyond strictly lattice-matching constraints and grade interfaces. However, previous photodetectors and optoelectronic devices rely on relatively simple vdW heterostructures with one or two blocks. The realization of high-order heterostructures has been exponentially challenging due to conventional layer-by-layer arduous restacking or sequential synthesis. In this study, we present an approach involving the direct exfoliation of high-quality BiI3-BiI heterostructure nanosheets with alternating blocks, derived from solution-grown binary heterocrystals. These heterostructure-based photodetectors offer several notable advantages. Leveraging the "active layer energetics" of BiI layers and the establishment of a significant depletion region, our photodetector demonstrates a significant reduction in dark current compared with pure BiI3 devices. Specifically, the photodetector achieves an extraordinarily low dark current (<9.2 × 10-14 A at 5 V bias voltage), an impressive detectivity of 8.8 × 1012 Jones at 638 nm, and a rapid response time of 3.82 μs. These characteristics surpass the performance of other metal-semiconductor-metal (MSM) photodetectors based on various 2D materials and structures at visible wavelengths. Moreover, our heterostructure exhibits a broad-band photoresponse, covering the visible, near-infrared (NIR)-I, and NIR-II regions. In addition to these promising results, our heterostructure also demonstrated the potential for flexible and imaging applications. Overall, our study highlights the potential of alternating vdW heterostructures for future optoelectronics with low power consumption, fast response, and flexible requirements.