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Calcium-for-strontium cation substitution of the a - b 0 c 0 /b 0 a - c 0 -distorted, cation-ordered, n = 2 Ruddlesden-Popper phase, YSr 2 Mn 2 O 7 , leads to separation into two phases, which both retain an a - b 0 c 0 /b 0 a - c 0 -distorted framework and have the same stoichiometry but exhibit different degrees of Y/Sr/Ca cation order. Increasing the calcium concentration to form YSr 0.5 Ca 1.5 Mn 2 O 7 leads to a change in the cooperative tilting on the MnO 6 units to a novel a - b - c - /b - a - c - arrangement described in space group P2 1 /n11. Low-temperature, topochemical fluorination of YSr 2 Mn 2 O 7 yields YSr 2 Mn 2 O 5.5 F 3.5 . In contrast to many other fluorinated n = 2 Ruddlesden-Popper oxide phases, YSr 2 Mn 2 O 5.5 F 3.5 retains the a - b 0 c 0 /b 0 a - c 0 lattice distortion and P4 2 /mnm space group symmetry of the parent oxide phase. The resilience of the a - b 0 c 0 /b 0 a - c 0 -distorted framework of YSr 2 Mn 2 O 7 o resist symmetry-changing deformations upon both cation substitution and anion insertion/exchange is discussed on the basis the A-site cation order of the lattice and the large change in the ionic radius of manganese upon oxidation from Mn 3+ o Mn 4+ . The structure property relations observed in the Y-Sr-Ca-Mn-O-F system provide insight into assisting in the synthesis of n = 2 Ruddlesden-Popper phases, which adopt cooperative structural distortions that break the inversion symmetry of the extended lattice and therefore act as a route for the preparation of ferroelectric and multiferroic materials.

inorganic chemistry

Structural Modification of the Cation-Ordered Ruddlesden–Popper Phase YSr2Mn2O7 by Cation Exchange and Anion Insertion