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Large assemblies of self‐organized aluminum nanoclusters embedded in an oxide layer  are formed on graphene templates and used to build tunnel‐junction devices. Unexpectedly, single‐electron‐transport behavior with well‐defined Coulomb oscillations is observed for a record junction area of up to 100 µm 2  containing millions of metal islands. Such graphene–metal nanocluster hybrid materials offer new prospects for single‐electron electronics.

Conductance Oscillations in a Graphene/Nanocluster Hybrid Material: Toward Large‐Area Single‐Electron Devices