Graphene and other two dimensional (2D) materials are currently integrated into nanoscaled devices that may – one day – sequence genomes.

Square millimeters of free-standing graphene do not exist per se because of thermal fluctuations in two-dimensional crystals and their tendency to collapse during the detachment from the substrate. Here we form millimeter-scale freely suspended graphene by injecting an air bubble underneath a graphene monolayer floating at the water–air interface, which allowed us to measure the contact angle on fully free-standing non-contaminated graphene. A captive bubble measurement shows that free-standing clean graphene is hydrophilic with a contact angle of 42° ± 3°. The proposed design provides a simple tool to probe and explore the wettability of two-dimensional materials in free-standing geometries and will expand our perception of two-dimensional materials technologies from microscopic to now millimeter scales.

Establishing contact angles on graphene-on-water has been a long-standing challenge as droplet deposition causes free-floating graphene to rupture. The current work presents ice and hydrogels as substrates mimicking water while offering a stable support for graphene. The lowest water contact angles on graphene ever measured, namely on graphene-on-ice and graphene-on-hydrogel, are recorded. The contact angle measurements of liquids with a range of polarities allow the transparency of graphene toward polar and dispersive interactions to be quantified demonstrating that graphene in water is hydrophilic. These findings are anticipated to shed light on the inconsistencies reported so far on the wetting properties of graphene, and most particularly on their implications toward rationalizing how molecules interact with graphene in water.

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Transfer of large, clean, crack- and fold-free graphene sheets is a critical challenge in the field of graphene-based electronic devices. Polymers, conventionally used for transferring two-dimensional materials, irreversibly adsorb yielding a range of unwanted chemical functions and contaminations on the surface. An oil–water interface represents an ideal support for graphene. Cyclohexane, the oil phase, protects graphene from mechanical deformation and minimizes vibrations of the water surface. Remarkably, cyclohexane solidifies at 7 °C forming a plastic crystal phase molecularly conforming graphene, preventing the use of polymers, and thus drastically limiting contamination. Graphene floating at the cyclohexane/water interface exhibits improved electrical performances allowing for new possibilities of in situ, flexible sensor devices at a water interface.