Materials with strongly correlated electrons often exhibit interesting physical properties. An example of these materials is the layered oxide perovskite Sr2RuO4, which has been intensively investigated due to its unusual properties. Whilst the debate on the symmetry of the superconducting state in Sr2RuO4 is still ongoing, a deeper understanding of the Sr2RuO4 normal state appears crucial as this is the background in which electron pairing occurs. Here, by using low-energy muon spin spectroscopy we discover the existence of surface magnetism in Sr2RuO4 in its normal state. We detect static weak dipolar fields yet manifesting at an onset temperature higher than 50 K. We ascribe this unconventional magnetism to orbital loop currents forming at the reconstructed Sr2RuO4 surface. Our observations set a reference for the discovery of the same magnetic phase in other materials and unveil an electronic ordering mechanism that can influence electron pairing with broken time reversal symmetry.

Ruddlesden–Popper (RP) phases (A n+1 B n O3n+1, n = 1, 2,···) have attracted intensive research with diverse functionalities for device applications. However, the realization of a high-quality RP-phase film is hindered by the formation of out-of-phase boundaries (OPBs) that occur at terrace edges, originating from lattice mismatch in the c-axis direction with the A′B′O3 (n = ∞) substrate. Here, using strontium ruthenate RP-phase Sr2RuO4 (n = 1) as a model system, an experimental approach for suppressing OPBs was developed. By tuning the growth parameters, the Sr3Ru2O7 (n = 2) phase was formed in a controlled manner near the film–substrate interface. This higher-order RP-phase then blocked the subsequent formation of OPBs, resulting in nearly defect-free Sr2RuO4 layer at the upper region of the film. Consequently, the Sr2RuO4 thin films exhibited superconductivity up to 1.15 K, which is the highest among Sr2RuO4 films grown by pulsed laser deposition. This work paves the way for synthesizing pristine RP-phase heterostructures and exploring their unique physical properties.

Sr 2 RuO 4 (SRO 214) is a prototypical unconventional superconductor. However, since the discovery of its superconductivity a quarter of a century ago, the symmetry of the bulk and surface superconducting states in single crystal SRO 214 remains controversial. Solving this problem is massively impeded by the fact that superconducting SRO 214 is extremely challenging to achieve in thin-films as structural defects and impurities sensitively annihilate superconductivity. Here we report a protocol for the reliable growth of superconducting SRO 214 thin-films by pulsed laser deposition and identify universal materials properties that are destructive to the superconducting state. We demonstrate that careful control of the starting material is essential in order to achieve superconductivity and use a single crystal target of Sr 3 Ru 2 O 7 (SRO 327). By systematically varying the SRO 214 film thickness, we identify mosaic twist as the key in-plane defect that suppresses superconductivity. The results are central to the development of unconventional superconductivity.

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