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Superconducting properties of thin films can be vastly different from thoseof bulk materials. Seminal work has shown the critical temperature Tc ofelemental superconductors decreases with decreasing film thickness when thenormal-state sheet resistance is lower than the quantum resistance h/(4e2).Sporadic examples on disordered films, however, hinted an enhancement in Tcalthough, structural and strain characterization was not possible since sampleswere prepared on a cold substrate in situ. To clarify the role of reduceddimensionality and disorder on the superconducting properties of thin films weemployed molecular beam epitaxy to grow wafer-scale high-quality aluminum (Al)nanofilms with normal-state sheet resistance at least 20 times lower thanh/(4e2) and investigated their electronic and structural properties ex situ.Defying general expectations, Tc increases with decreasing Al film thickness,reaching 2.4 K for 3.5-nm-thick Al film grown on GaAs: twice that of bulk Al(1.2 K). DFT calculations indicate surface phonon softening impactssuperconductivity in pure ultra-thin films, offering a new route for materialsengineering in two dimensions.

Doubling of the superconducting transition temperature in ultra-clean wafer-scale aluminum nanofilms