Molybdenum disulphide is a layered transition metal dichalcogenide that has recently raised considerable interest due to its unique semiconducting and opto-electronic properties. Although several theoretical studies have suggested an electronic phase transition in molybdenum disulphide, there has been a lack of experimental evidence. Here we report comprehensive studies on the pressure-dependent electronic, vibrational, optical and structural properties of multilayered molybdenum disulphide up to 35 GPa. Our experimental results reveal a structural lattice distortion followed by an electronic transition from a semiconducting to metallic state at B19 GPa, which is confirmed by ab initio calculations. The metallization arises from the overlap of the valance and conduction bands owing to sulphur-sulphur interactions as the interlayer spacing reduces. The electronic transition affords modulation of the opto-electronic gain in molybdenum disulphide. This pressuretuned behaviour can enable the development of novel devices with multiple phenomena involving the strong coupling of the mechanical, electrical and optical properties of layered nanomaterials.

We use micro-Raman and photoluminescence (PL) spectroscopy at 300K to investigate the influence of uniaxial tensile strain on the vibrational and optoelectronic properties of monolayer and bilayer MoS2 on a flexible substrate. The initially degenerate E 1 2g Raman mode is split into a doublet as a direct consequence of the strain applied to MoS2 through Van der Waals coupling at the sample-substrate interface. We observe a strong shift of the direct band gap of 48meV/(% of strain) for the monolayer and 46meV/% for the bilayer, whose indirect gap shifts by 86meV/%. We find a strong decrease of the PL polarization linked to optical valley initialization for both monolayer and bilayer samples, indicating that scattering to the spin-degenerate Γ valley plays a key role.

Electronic skins (e-skins) are devices that can respond to mechanical stimuli and enable robots to perceive their surroundings. A great challenge for existing e-skins is that they may easily fail under extreme mechanical conditions due to their multilayered architecture with mechanical mismatch and weak adhesion between the interlayers. Here we report a flexible pressure sensor with tough interfaces enabled by two strategies: quasi-homogeneous composition that ensures mechanical match of interlayers, and interlinked microconed interface that results in a high interfacial toughness of 390 J·m−2. The tough interface endows the sensor with exceptional signal stability determined by performing 100,000 cycles of rubbing, and fixing the sensor on a car tread and driving 2.6 km on an asphalt road. The topological interlinks can be further extended to soft robot-sensor integration, enabling a seamless interface between the sensor and robot for highly stable sensing performance during manipulation tasks under complicated mechanical conditions.

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