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Three different procedures are used to deposit aluminium onto O‐terminated (100) and (111) boron‐doped diamond, with the aim of producing a thermally stable surface with low work function and negative electron affinity. The methods are 1) deposition of a > 20 nm film of Al by high‐vacuum evaporation followed by HCl acid wash to remove excess metallic Al, 2) deposition of <3 Å of Al by atomic...