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Abstract Interlayer charge‐transfer (CT) in 2D atomically thin vertical stacks heterostructures offers an unparalleled new approach to regulation of device performance in optoelectronic and photonics applications. Despite the fact that the saturable absorption (SA) in 2D heterostructures involves highly efficient optical modulation in the space and time domain, the lack of explicit SA regulation mechanism at the nanoscale prevents this feature from realizing nanophotonic modulation. Here, the enhancement of SA response via CT in WS2/graphene vertical heterostructure is proposed and the related mechanism is demonstrated through simulations and experiments. Leveraging this mechanism, CT‐induced SA enhancement can be expanded to a wide range of nonlinear optical modulation applications for 2D materials. The results suggest that CT between 2D heterostructures enables efficient nonlinear optical response regulation.

Abstract Two‐dimensional transition metal dichalcogenides (TMDs) are needed in high‐performance piezoresistive sensors due to their strong strain‐induced bandgap modification and thereby large gauge factors. However, integrating a conventional high‐temperature chemical vapor deposition (CVD)‐grown TMD with a flexible substrate necessitates a transfer process that inevitably degrades the sensing properties of the TMDs and increases the overall fabrication complexity. We present a high‐performance piezoresistive strain sensor that employs large‐area PdSe2 films grown directly on polyimide (PI) substrates via plasma‐assisted selenization of a sputtered Pd film. The reliable strain transfer from the substrate to the PdSe2 film ensures an outstanding strain‐sensing capability of the sensor. Specifically, the sensors have a gauge factor of up to −315 ± 2.1, a response time under 25 ms, a detection limit of 8 × 10−6, and an exceptional stability of over 104 loading–unloading cycles. By attaching the sensors to the skin surface, we demonstrate their application for measuring physiological parameters in health care monitoring, including motion, voice, and arterial pulse vibration. Furthermore, using the PdSe2 film sensor combined with deep learning technology, we achieved intelligent recognition of artery temperature from arterial pulse signals with only a 2% difference between predicted and actual temperatures. The excellent sensing performance, together with the advantages of low‐temperature fabrication and simple device structure, make the PdSe2 film sensor promising for wearable electronics and health care sensing systems.