Superconductivity Tuned by the Iron Vacancy Order in KxFe2−ySe2

Combining in-depth neutron diffraction and systematic bulk studies, we discover that the root 5 x root 5 Fe vacancy order, with its associated block antiferromagnetic order, is the ground state with varying occupancy ratios of the iron 16i and vacancy 4d sites across the phase-diagram of KxFe2-ySe2. The orthorhombic order, with one of the four Fe sites vacant, appears only at intermediate temperatures as a competing phase. The material experiences an insulator to metal crossover when the root 5 x root 5 order is highly developed. Superconductivity occurs in such a metallic phase.