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arXiv 1002.1545cond-mat.mtrl-sci
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多铁性La改性BiFeO3-PbTiO3固溶体大介电常数和大剩余极化的起源及磁电耦合的证据

Origin of Large Dielectric Constant with Large Remnant Polarization and Evidence of Magnetoelectric Coupling in Multiferroic La modified BiFeO3-PbTiO3 Solid Solution

Anupinder Singh, Ratnamala Chatterjee, S. K. Mishra, P. S. R. Krishna, S. L. Chaplot

摘要:

超晶格反射的存在以及粉末中子和X射线衍射数据的详细分析表明,富La(BF $_{0.50}$ -LF $_{0.50}$)$_{0.50}$ -(PT)$_{0.50}$(BF-LF-PT)在环境条件下具有空间群为\textit{$R3c$}的铁电菱形晶体结构。晶格参数、倾斜角、计算的极化$(P_{s})$、体积以及超晶格和磁反射的积分强度的温度依赖性在170 K附近显示出异常。在$473K \leq T \leq 573K$温度范围内进行阻抗谱、介电和交流电导率测量,以探测$T_c^{FE}$附近具有大介电常数的大剩余极化和频率依赖性宽跃迁的起源。阻抗谱测量的结果清楚地显示了在整个频率范围($10^{3}$ Hz $\leq f\leq 10^{7} $ Hz)内晶粒和晶界的贡献。可以得出结论,与晶粒相比,晶界的电阻性和电容性更大,导致样品中的不均匀性,从而引起宽频率依赖的介电异常。介电常数和剩余极化值的增加可能是由于颗粒界面和晶界处电荷堆积引起的空间电荷极化。在$T_c^{FE}(\sim 523$ K)下使用Maxwell-Wagner模型拟合介电常数($ε^{\prime\prime}$)的虚部与频率数据,并且模型与高达$10^{5}$ Hz的数据拟合得非常好。磁介电测量证明样品在$\sim 170$ K开始表现出磁电耦合,这也被中子衍射数据所验证。

英文摘要:

The presence of superlattice reflections and detailed analyses of the powder neutron and x-ray diffraction data reveal that La rich (BF$_{0.50}$-LF$_{0.50}$)$_{0.50}$-(PT)$_{0.50}$ (BF-LF-PT) has ferroelectric rhombohedral crystal structure with space group \textit{$R3c$} at ambient conditions. The temperature dependence of lattice parameters, tilt angle, calculated polarization $(P_{s})$, volume, and integrated intensity of superlattice and magnetic reflections show an anomaly around 170 K. Impedance spectroscopy, dielectric and ac conductivity measurements were performed in temperature range $473K \leq T \leq 573K$ to probe the origin of large remnant polarization and frequency dependent broad transitions with large dielectric constant near $T_c^{FE}$. Results of impedance spectroscopy measurements clearly show contributions of both grain and grain boundaries throughout the frequency range ($10^{3}$ Hz$\leq f\leq 10^{7} $ Hz). It could be concluded that the grain boundaries are more resistive and capacitive as compared to the grains, resulting in inhomogeneities in the sample causing broad frequency dependent dielectric anomalies. Enhancement in dielectric constant and remnant polarization values are possibly due to space charge polarization caused by piling of charges at the interface of grains and grain boundaries. The imaginary parts of dielectric constant ($ε^{\prime\prime}$) Vs frequency data were fitted using Maxwell-Wagner model at $T_c^{FE}(\sim 523$K) and model fits very well with the data up to $10^{5}$ Hz. Magnetodielectric measurements prove that the sample starts exhibiting magnetoelectric coupling at $\sim 170$ K, which is also validated by neutron diffraction data.

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