Direct Synthesis of Chromium Perovskite Oxyhydride with a High Magnetic‐Transition Temperature

We report a novel oxyhydride SrCrO 2 H directly synthesized by a high‐pressure high‐temperature method. Powder neutron and synchrotron X‐ray diffraction revealed that this compound adopts the ideal cubic perovskite structure ${\left( {Pm\bar 3m} \right)}$ with O 2− /H − disorder. Surprisingly, despite the non‐bonding nature between Cr 3d t 2g orbitals and the H 1s orbital, it exhibits G‐type spin ordering at T N ≈380 K, which is higher than that of RCrO 3 (R=rare earth) and any chromium oxides. The enhanced T N in SrCrO 2 H with four Cr‐O‐Cr bonds in comparison with RCr 3+ O 3 with six Cr‐O‐Cr bonds is reasonably explained by the tolerance factor. The present result offers an effective strategy to tune octahedral tilting in perovskites and to improve physical and chemical properties through mixed anion chemistry.