Enhanced Superconductivity and Mixed-dimensional Behaviour in Infinite-layer Samarium Nickelate Thin Films

Abstract

Rare-earth infinite-layer nickelates represent an emerging class of unconventional superconductors, with materials synthesis largely limited to early lanthanide compounds. Here, we report the synthesis and characterization of phase-pure superconducting samarium-based infinite-layer nickelate thin films, including the first demonstration of Sm$_{1-x}$Sr$_x$NiO$_2$, along with co-doped variants incorporating europium and calcium. These films, grown on LSAT (001) substrates, exhibit coherent lattice structures up to $\sim$ 9 nm thickness with minimal stacking faults. The co-doped compounds achieve a record-small $c$-axis parameter of 3.26 {\AA} and display remarkable superconducting transition temperatures up to 32.5 K. These results establish a clear correlation between decreasing $c$-axis parameter and increasing critical temperature across different rare-earth systems. In addition, angle-dependent magnetoresistance investigations reveal the existence of a hybrid mixture of 2D and 3D superconductivity in this novel system with enhanced coupling between the rare-earth 5d and Ni 3d orbitals, confirmed by resonant inelastic X-ray scattering experiments. As the concentration of Eu increases, the system exhibits a clear tendency towards 3D superconductivity. Furthermore, we observe distinctive negative magnetoresistance in the europium-containing samples. These findings advocate clear materials design principles for higher transition temperatures and exotic physics in infinite-layer nickelate superconductors through structural engineering of the rare-earth site.