Electron-like high-temperature superconductivity induced by compressive strain in La2PrNi2O7 thin films

The realization of high-temperature superconductivity in bilayer nickelates under epitaxial compressive strain is widely interpreted as mimicking the effects of high hydrostatic pressure. To test the equivalence of these mechanisms, we investigated a comprehensive strain continuum ranging from compressive (-2.14%) to tensile (+0.91%). Crucially, via ozone-assisted atomic-layer epitaxy, we realized high-temperature superconductivity in as-grown La2PrNi2O7 films on NdAlO3 substrates, which induce the most extreme compressive strain in this material system. Under extreme compression (-2.14%), these films exhibit a Tc_onset of 60 K, zero resistance at 33 K, and a diamagnetic response at 20 K, with magnetotransport measurements confirming a quasi-two-dimensional superconducting nature. Comparing our phase diagram with reported data reveals distinct lattice responses: unlike in pressurized crystals, the superconducting window in epitaxial films diverges significantly in the out-of-plane parameter c (or c/ap ratio) but remains consistent with the bulk regarding the in-plane parameter ap. Crucially, while superconductivity in both systems emerges from the suppression of spin-density waves (SDW), Hall measurements reveal a fundamental electronic dichotomy: optimal superconducting films are intrinsically electron-like (exhibiting a negative Hall coefficient), in stark contrast to the hole-like nature (positive Hall coefficient) of high-pressure bulk crystals and non-superconducting tensile films. Ultimately, both tuning strategies effectively modulate the underlying correlation landscape - the true driver of superconductivity - transcending the constraints of specific Fermi surface topologies. This work establishes a macroscopic platform for probing the multi-orbital physics of nickelates, offering a new dimension for investigating high-temperature superconductivity.