Abstract

Interlayer excitons (IX), spatially separated electron–hole pair quasiparticles, can form in type-II van der Waals heterostructures (vdWH). To date, the most widely studied IX in hetero- and homobilayer transition metal dichalcogenides feature momentum-indirect and visible interlayer recombinations. However, momentum-direct IX emissions and interlayer absorptions, especially in the infrared, are crucial for excitonic devices but remain underexplored. In this work, we propose and construct a multilayer WSe2/InSe vdWH that hosts momentum-direct IX and manifests near-infrared interlayer absorptions at room temperature, verified by first-principles density functional theory calculations. We conduct power- and temperature-dependent photoluminescence spectroscopies and extract the IX binding energy to be 43 ± 5 meV. Furthermore, we manipulate the IX emission electrically via the Stark effect and tune its energy by 180 meV. Taking advantage of the direct interlayer absorption, we fabricate a near-infrared vdWH photodetector modulated by strong photogating effect, and achieve the optimal photoresponsivity, specific detectivity, and response time of 33 A W–1, 1.8 × 1010 Jones, and 3.7 μs at 1150 nm. In addition, we test the imaging capability of the photodetector by integrating it into a single-pixel imaging system. Our work showcases the possibility for constructing infrared-responsive vdWH that hosts momentum-direct IX for future excitonic devices of optoelectronic applications.