• Yajima, Takeshi
• Brown, Craig M.
• Yamamoto, Takafumi
• Tanaka, Katsuhisa
• Kageyama, Hiroshi
• Aidzu, Kohei
• Akamatsu, Hirofumi
• Takeiri, Fumitaka
• Lei, Shiming
• Ohkura, Masatoshi
• Gopalan, Venkatraman
• Green, Mark A.
• Yoshimune, Wataru
• Kobayashi, Yoji
• Fujita, Koji

Abstract

Oxynitrides have been explored extensively in the past decade because of their interesting properties, such as visible-light absorption, photocatalytic activity and high dielectric permittivity. Their synthesis typically requires high-temperature NH₃ treatment (800-1,300 °C) of precursors, such as oxides, but the highly reducing conditions and the low mobility of N^3- species in the lattice place significant constraints on the composition and structure-and hence the properties-of the resulting oxynitrides. Here we show a topochemical route that enables the preparation of an oxynitride at low temperatures (<500 °C), using a perovskite oxyhydride as a host. The lability of H^- in BaTiO_3-xH_x (x ≤ 0.6) allows H^-/N^3- exchange to occur, and yields a room-temperature ferroelectric BaTiO_3-xN_2x/3. This anion exchange is accompanied by a metal-to-insulator crossover via mixed O-H-N intermediates. These findings suggest that this 'labile hydride' strategy can be used to explore various oxynitrides, and perhaps other mixed anionic compounds.

Topics

• perovskite
• impedance spectroscopy
• compound
• mobility