We report that substrate doping-induced charge carrier density modulation leads to the tunable wettability and adhesion of graphene. Graphene's water contact angle changes by as much as 13° as a result of a 300 meV change in doping level. Upon either n- or p-type doping with subsurface polyelectrolytes, graphene exhibits increased hydrophilicity. Adhesion force measurements using a hydrophobic self-assembled monolayer-coated atomic force microscopy probe reveal enhanced attraction toward undoped graphene, consistent with wettability modulation. This doping-induced wettability modulation is also achieved via a lateral metal-graphene heterojunction or subsurface metal doping. Combined first-principles and atomistic calculations show that doping modulates the binding energy between water and graphene and thus increases its hydrophilicity. Our study suggests that the doping-induced modulation of the charge carrier density in graphene influences its wettability and adhesion [corrected]. This opens up unique and new opportunities for the tunable wettability and adhesion of graphene for advanced coating materials and transducers.

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Flexible electrodes that allow electrical conductance to be maintained during mechanical deformation are required for the development of wearable electronics. However, flexible electrodes based on metal thin-films on elastomeric substrates can suffer from complete and unexpected electrical disconnection after the onset of mechanical fracture across the metal. Here we show that the strain-resilient electrical performance of thin-film metal electrodes under multimodal deformation can be enhanced by using a two-dimensional (2D) interlayer. Insertion of atomically-thin interlayers — graphene, molybdenum disulfide, or hexagonal boron nitride — induce continuous in-plane crack deflection in thin-film metal electrodes. This leads to unique electrical characteristics (termed electrical ductility) in which electrical resistance gradually increases with strain, creating extended regions of stable resistance. Our 2D-interlayer electrodes can maintain a low electrical resistance beyond a strain in which conventional metal electrodes would completely disconnect. We use the approach to create a flexible electroluminescent light emitting device with an augmented strain-resilient electrical functionality and an early-damage diagnosis capability.

We report a one-step polymer-free approach to patterning graphene using a stencil mask and oxygen plasma reactive-ion etching, with a subsequent polymer-free direct transfer for flexible graphene devices. Our stencil mask is fabricated via a subtractive, laser cutting manufacturing technique, followed by lamination of stencil mask onto graphene grown on Cu foil for patterning. Subsequently, micro-sized graphene features of various shapes are patterned via reactive-ion etching. The integrity of our graphene after patterning is confirmed by Raman spectroscopy. We further demonstrate the rapid prototyping capability of a stretchable, crumpled graphene strain sensor and patterned graphene condensation channels for potential applications in sensing and heat transfer, respectively. We further demonstrate that the polymer-free approach for both patterning and transfer to flexible substrates allows the realization of cleaner graphene features as confirmed by water contact angle measurements. We believe that our new method promotes rapid, facile fabrication of cleaner graphene devices, and can be extended to other two dimensional materials in the future.

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