pH sensitivity of edge-gated graphene field-effect devices with covalent edge-functionalization

We present here a new strategy for a field-effect device, termed graphene edge field-effect transistor (GrEdge-FET), where a micron-wide graphene monolayer is gated exclusively through its edge in an aqueous environment. This is achieved by passivating the basal plane selectively using photolithography. We observe a field-effect behavior in buffer solutions with an ON/OFF ratio of nearly 10 in a small gate-voltage range (+/- 0.5 V) without any need for complex nanofabrication or specialized electrolytes. We attribute this effect to the electrical double layer capacitance at the edge-electrolyte interface, which efficiently gates the entire graphene sheet although it acts only at the edge. We demonstrate that GrEdge-FET devices find applications as pH sensors. Through diazonium electrochemistry, the edges are functionalized persistently with substituted phenyl moieties, which renders the devices with a higher pH sensitivity than classical graphene FETs. Moreover, since only the edge is modified, the favorable field-effect behavior is preserved, despite the covalent nature of attachment of the functional groups.