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We present a joint experimental and theoretical study of the superconductingphase of the layered binary silicide BaSi2. Compared with the layered AlB2structure of graphite or diboride-like superconductors, in the hexagonalstructure of binary silicides the sp3 arrangement of silicon atoms leads tocorrugated sheets. Through a high-pressure synthesis procedure we are able tomodify the buckling of these sheets, obtaining the enhancement of thesuperconducting transition temperature from 4 K to 8.7 K when the siliconplanes flatten out. By performing ab-initio calculations based on densityfunctional theory we explain how the electronic and phononic properties of thesystem are strongly affected by changes in the buckling. This mechanism islikely present in other intercalated layered superconductors, opening the wayto the tuning of superconductivity through the control of internal structuralparameters.

Enhancing the superconducting transition temperature of BaSi2 by structural tuning