Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
J Phys Condens Matter. 2011 Apr 27;23(16):164214. doi: 10.1088/0953-8984/23/16/164214. Epub 2011 Apr 6.
To understand the origin of the spin-glass state in molybdate pyrochlores, the structure of Tb(2)Mo(2)O(7) is investigated using two techniques: the long-range lattice structure was measured using neutron powder diffraction, and local structure information was obtained from the extended x-ray absorption fine structure technique. While the long-range structure appears generally well ordered, enhanced mean-squared site displacements on the O(1) site and the lack of temperature dependence of the strongly anisotropic displacement parameters for both the Mo and O(1) sites indicate some disorder exists. Likewise, the local structure measurements indicate some Mo-Mo and Tb-O(1) nearest-neighbor disorder exists, similar to that found in the related spin-glass pyrochlore, Y(2)Mo(2)O(7). Although the freezing temperature in Tb(2)Mo(2)O(7), 25 K, is slightly higher than in Y(2)Mo(2)O(7), 22 K, the degree of local pair distance disorder is actually less in Tb(2)Mo(2)O(7). This apparent contradiction is considered in light of the interactions involved in the freezing process.
为了理解钼酸盐尖晶石中自旋玻璃态的起源,使用两种技术研究了 Tb(2)Mo(2)O(7)的结构:使用中子粉末衍射测量长程晶格结构,并用扩展 X 射线吸收精细结构技术获得局部结构信息。尽管远程结构通常表现出良好的有序性,但 O(1)位置上的均方根 site 位移增强以及 Mo 和 O(1)位置上强烈各向异性位移参数缺乏温度依赖性表明存在一些无序。同样,局部结构测量表明存在一些 Mo-Mo 和 Tb-O(1)最近邻无序,类似于在相关的自旋玻璃尖晶石 Y(2)Mo(2)O(7)中发现的无序。尽管 Tb(2)Mo(2)O(7)的冻结温度为 25 K,略高于 Y(2)Mo(2)O(7)的 22 K,但 Tb(2)Mo(2)O(7)中局部对距离无序的程度实际上较小。这种明显的矛盾是根据冻结过程中涉及的相互作用来考虑的。