Abstract

Abstract2D materials have been widely applied in flexible electronics but only with limited stretchability, because the metal‐halide bonding is so strong that the materials’ electronic properties will be severely influenced upon tensile strain. Here, a strategy is proposed for the fabrication of ultrastretchable MoS2 photoreceptors based on chemical vapor deposition‐grown or manually stacked multilayer MoS2. Strain‐dependent spectroscopic comparisons of multilayer versus monolayer MoS2 indicate that the strain transfer is suppressed from bottom to top layers owing to interlayer sliding, which is consistent with the density functional theory and molecular dynamics simulations. Thus, the optoelectronic properties of multilayer MoS2 can withstand larger mechanical strain than monolayer MoS2. Leveraging this mechanical feature, ten‐layer MoS2 photodetector is fabricated on polystyrene‐b‐poly (ethylene‐co‐butylene)‐b‐polystyrene elastomer, withstanding ≈50% tensile strain and presenting 32 times higher photoresponsivity than that of monolayer MoS2 under the same stretching condition. Based on large‐area bilayer MoS2 film, 5 × 5 stretchable photodetector array is demonstrated and is capable of working as artificial photoreceptors to control a robotic hand under 16% tensile strain, showing great potential in applications for 2D material‐based electronic skin.

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