Polar Metal Phase Induced by Oxygen Octahedral Network Relaxation in Oxide Thin Films

ABO3 perovskite materials and their derivatives have inherent structural flexibility due to the corner sharing network of the BO6 octahedron, and the large variety of possible structural distortions and strong coupling between lattice and charge/spin degrees of freedom have led to the emergence of intriguing properties, such as high‐temperature superconductivity, colossal magnetoresistance, and improper ferroelectricity. Here, an unprecedented polar ferromagnetic metal phase in SrRuO3 (SRO) thin films is presented, arising from the strain‐controlled oxygen octahedral rotation (OOR) pattern. For compressively strained SRO films grown on SrTiO3 substrate, oxygen octahedral network relaxation is accompanied by structural phase separation into strained tetragonal and bulk‐like orthorhombic phases, and the asymmetric OOR evolution across the phase boundary allows formation of the polar phase, while bulk metallic and ferromagnetic properties are maintained. From the results, it is expected that other oxide perovskite thin films will also yield similar structural environments with variation of OOR patterns, and thereby provide promising opportunities for atomic scale control of material properties through strain engineering. Oxygen octahedral rotation relaxation in compressively strained SrRuO3 thin films stabilizes a polar distortion (triclinic C1 symmetry) between strained tetragonal and relaxed bulk‐like orthorhombic phases. The metallicity and the ferromagnetism can be maintained in the polar structure, which suggests an emergence of the ferromagnetic polar metal phase.