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Ca2Co2O5 in the brownmillerite form was synthesized using a high-pressureoptical-image floating zone furnace, and single crystals with dimensions up to1.4x0.8x0.5 mm3 were obtained. At room temperature, Ca2Co2O5 crystallizes as afully ordered brownmillerite variant in the orthorhombic space group Pcmb (No.57) with unit cell parameters a=5.28960(10) {\AA}, b=14.9240(2) {\AA}, andc=10.9547(2) {\AA}. With decreasing temperature, it undergoes a re-entrantsequence of first-order structural phase transitions (Pcmb to P2/c11 to P121/m1to Pcmb) that is unprecedented among brownmillerites, broadening the family ofspace groups available to these materials and challenging current approachesfor sorting the myriad variants of brownmillerite structures. Magneticsusceptibility data indicate antiferromagnetic ordering in Ca2Co2O5 occurs near240 K, corroborated by neutron powder diffraction. Below 140 K, the specimenexhibits a weak ferromagnetic component directed primarily along the b axisthat shows a pronounced thermal and magnetic history dependence.

Brownmillerite Ca2Co2O5: Synthesis, Stability, and Re-entrant Single-Crystal-to-Single-Crystal Structural Transitions