Tsuji Kosuke, Han HyukSu, Guillemet-Fritsch Sophie, Randall Clive A
Center for Dielectrics and Piezoelectrics, Materials Research Institute, Department of Material Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, USA.
Phys Chem Chem Phys. 2017 Mar 28;19(12):8568-8574. doi: 10.1039/c7cp00042a. Epub 2017 Mar 14.
Dielectric spectroscopy was performed on a Nb and In co-doped rutile TiO nano-crystalline ceramic (n-NITO) synthesized by a low-temperature spark plasma sintering (SPS) technique. The dielectric properties of the n-NITO were not largely affected by the metal electrode contacts. Huge dielectric relaxation was observed at a very low temperature below 35 K. Both the activation energy and relaxation time suggested that the electronic hopping motion is the underlying mechanism responsible for the colossal dielectric permittivity (CP) and its relaxation, instead of the internal barrier layer effect or a dipolar relaxation. With Havriliak-Negami (H-N) fitting, a relaxation time with a large distribution of dielectric relaxations was revealed. The broad distributed relaxation phenomena indicated that Nb and In were involved, controlling the dielectric relaxation by modifying the polarization mechanism and localized states. The associated distribution function is calculated and presented. The frequency-dependent a.c. conductance is successfully explained by a hopping conduction model of the localized electrons with the distribution function. It is demonstrated that the dielectric relaxation is strongly correlated with the hopping electrons in the localized states. The CP in SPS n-NITO is then ascribed to a hopping polarization.
采用低温放电等离子体烧结(SPS)技术合成了Nb和In共掺杂的金红石型TiO纳米晶陶瓷(n-NITO),并对其进行了介电谱测试。n-NITO的介电性能受金属电极接触的影响不大。在低于35 K的极低温度下观察到巨大的介电弛豫。活化能和弛豫时间均表明,电子跳跃运动是导致巨介电常数(CP)及其弛豫的潜在机制,而非内部势垒层效应或偶极弛豫。通过Havriliak-Negami(H-N)拟合,揭示了具有大介电弛豫分布的弛豫时间。宽分布弛豫现象表明Nb和In参与其中,通过改变极化机制和局域态来控制介电弛豫。计算并给出了相关的分布函数。频率相关的交流电导通过具有分布函数的局域电子跳跃传导模型得到了成功解释。结果表明,介电弛豫与局域态中的跳跃电子密切相关。SPS n-NITO中的CP归因于跳跃极化。