Damped soft phonons and diffuse scattering in (BiNa)TiO

(BiNa)TiOにおける過減衰フォノンと散漫散乱

松浦 直人*; 飯田 裕之*; 廣田 和馬*; 大和田 謙二; 野口 祐二*; 宮山 勝*

Matsuura, Masato*; Iida, Hiroyuki*; Hirota, Kazuma*; Owada, Kenji; Noguchi, Yuji*; Miyayama, Masaru*

(BiNa)TiOにおいては600K付近を最大とする誘電率の緩やかな温度変化の他、それに伴う圧電効果の減少が脱分極温度460K-480Kより上で観測される。その起源を中性子散乱を用いて調べた。その結果、点近傍で強く過減衰したwater-fall的ソフトフォノンが脱分極温度付近で観測されたほか、M点においては誘電率の温度依存性に対応する温度依存性を持つ超格子反射が観測された。これらは、正方晶/菱面体晶相が共存するなかでの強誘電クラスターのダイナミックな性質、これらは脱分極やwater-fallを与える、が重要であることを示している。

Neutron-scattering studies of (BiNa)TiO (BNT) have been performed to elucidate the microscopic mechanism of the broad maximum in the temperature dependence of the dielectric constant at Tm 600 K and the reduction in the piezoelectric properties above the depolarization temperature, 460 480 K. We observed diffuse scattering near the point below 700 K, which competes with the superlattice peak at the M point of the tetragonal phase but coexists with the superlattice peak at the R point of the rhombohedral phase. The diffuse scattering shows an anisotropic Q shape extending along the 100 direction transverse to the scattering vector Q, which is explained by atomic shifts bridging the tetragonal and rhombohedral structures. We propose that the broad maximum in the dielectric constant is associated with a diffusive first-order transition between the competing tetragonal and rhombohedral phases. In addition, we found that the diffuse scattering is reduced for single crystals grown under high oxygen pressure, which suggests an analogy with the central peak in hydrogen-reduced SrTiO. Inelastic neutron scattering near the point reveals a heavily overdamped soft mode similar to those reported in lead-based relaxors, the "waterfall" feature. Moreover, a damped soft transverse acoustic mode is observed for the 100 direction as the anisotropic diffuse scattering, indicating phase instabilities with the same origin as that of the diffuse scattering. The recovery of the soft mode is observed near the depolarization temperature, which coincides with the disappearance of the superlattice peak at the M point. These results indicate that the depolarization and the waterfall feature originate in the dynamic nature of ferroelectric clusters in the coexisting tetragonal/rhombohedral phase.