Mixed-dimensional van der Waals (vdW) heterostructures based on two-dimensional (2D) materials exhibit immense potential in infrared optoelectronic applications. However, the weak vdW coupling results in limiting performance of infrared optoelectronic device. Here, we exploit a gapless heterostructure that S dangling bonds of nonlayered PbS are connected to the bonding sites of MoS2 (with factitious S vacancies) via strong orbital hybridization. The strong interface coupling leads to ultrahigh responsivity and photogain (G) exceeding 105, and the detectivity (D*) is greater than 1014 Jones. More importantly, the gapless heterostructure shows fast rise and decay times about 47 and 49 μs, respectively, which is 5 orders of magnitude faster than that of transferred vdW heterostructures. Furthermore, an ultrahigh photon-triggered on/off ratio of 1.6 × 106 is achieved, which is 4 orders of magnitude higher than that of transferred vdW heterostructures. This architecture can offer an effective approach for advanced infrared optoelectronic devices.
Keywords: gapless heterostructure; high performance; infrared optoelectronic device; strong orbital hybridization; two-dimensional.