Zhang Qingteng, Dufresne Eric M, Chen Pice, Park Joonkyu, Cosgriff Margaret P, Yusuf Mohammed, Dong Yongqi, Fong Dillon D, Zhou Hua, Cai Zhonghou, Harder Ross J, Callori Sara J, Dawber Matthew, Evans Paul G, Sandy Alec R
X-Ray Science Division, Argonne National Laboratory, Lemont, Illinois 60439, USA.
Department of Materials Science and Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706, USA.
Phys Rev Lett. 2017 Mar 3;118(9):097601. doi: 10.1103/PhysRevLett.118.097601. Epub 2017 Feb 27.
Ferroelectric-dielectric superlattices consisting of alternating layers of ferroelectric PbTiO_{3} and dielectric SrTiO_{3} exhibit a disordered striped nanodomain pattern, with characteristic length scales of 6 nm for the domain periodicity and 30 nm for the in-plane coherence of the domain pattern. Spatial disorder in the domain pattern gives rise to coherent hard x-ray scattering patterns exhibiting intensity speckles. We show here using variable-temperature Bragg-geometry x-ray photon correlation spectroscopy that x-ray scattering patterns from the disordered domains exhibit a continuous temporal decorrelation due to spontaneous domain fluctuations. The temporal decorrelation can be described using a compressed exponential function, consistent with what has been observed in other systems with arrested dynamics. The fluctuation speeds up at higher temperatures and the thermal activation energy estimated from the Arrhenius model is 0.35±0.21 eV. The magnitude of the energy barrier implies that the complicated energy landscape of the domain structures is induced by pinning mechanisms and domain patterns fluctuate via the generation and annihilation of topological defects similar to soft materials such as block copolymers.
由铁电体PbTiO₃和电介质SrTiO₃交替层组成的铁电 - 电介质超晶格呈现出无序的条纹状纳米畴图案,畴周期的特征长度尺度为6纳米,畴图案的面内相干长度尺度为30纳米。畴图案中的空间无序导致相干硬X射线散射图案出现强度斑点。我们在此使用变温布拉格几何X射线光子相关光谱表明,来自无序畴的X射线散射图案由于自发畴涨落而呈现出连续的时间去相关。时间去相关可以用压缩指数函数来描述,这与在其他具有动力学阻滞的系统中所观察到的情况一致。涨落在较高温度下加快,根据阿仑尼乌斯模型估计的热激活能为0.35±0.21电子伏特。能垒的大小意味着畴结构复杂的能量景观是由钉扎机制引起的,并且畴图案通过类似于嵌段共聚物等软材料中的拓扑缺陷的产生和湮灭而涨落。