Near-direct bandgap $WS{e}_2$/$Re{S}_2$ type-II pn heterojunction for enhanced ultrafast photodetection and high-performance photovoltaics

Abstract

PN heterojunctions comprising layered van der Waals (vdW) semiconductors have been used to demonstrate current rectifiers, photodetectors, and photovoltaic devices. However, a direct or near-direct bandgap at the heterointerface that can significantly enhance optical generation, for high light absorbing few/multi-layer vdW materials, has not yet been shown. In this work, for the first time, few-layer group-6 transition metal dichalcogenide (TMD) $WS{e}_2$ is shown to form a sizeable (0.7 eV) near-direct bandgap with type-II band alignment at its interface with the group-7 TMD $Re{S}_2$ through density functional theory calculations. Further, the type-II alignment and photogeneration across the interlayer bandgap have been experimentally confirmed through micro-photoluminescence and IR photodetection measurements, respectively. High optical absorption in few-layer flakes, large conduction and valence band offsets for efficient electron-hole separation and stacking of light facing, direct bandgap $Re{S}_2$ on top of gate tunable $WS{e}_2$ are shown to result in excellent and tunable photodetection as well as photovoltaic performance through flake thickness dependent optoelectronic measurements. Few-layer flakes demonstrate ultrafast response time (5 $\mu$s) at high responsivity (3 A/W) and large photocurrent generation and responsivity enhancement at the heterostructure overlap region (10-100X) for 532 nm laser illumination. Large open-circuit voltage of 0.64 V and short-circuit current of 2.6 $\mu$A enables high output electrical power. Finally, long term air-stability and a facile single contact metal fabrication process makes the multi-functional few-layer $WS{e}_2$/$Re{S}_2$ heterostructure diode technologically promising for next-generation optoelectronic applications.

Manuscript- 27 pages, 8 figures. Supporting Information- 17 pages, 17 figures

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