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Design of crystal-like aperiodic solids with selective disorder–phonon coupling

机译:选择性无序-声子耦合的类晶体非周期性固体的设计

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摘要

Functional materials design normally focuses on structurally ordered systems because disorder is considered detrimental to many functional properties. Here we challenge this paradigm by showing that particular types of strongly correlated disorder can give rise to useful characteristics that are inaccessible to ordered states. A judicious combination of low-symmetry building unit and high-symmetry topological template leads to aperiodic ‘procrystalline’ solids that harbour this type of disorder. We identify key classes of procrystalline states together with their characteristic diffraction behaviour, and establish mappings onto known and target materials. The strongly correlated disorder found in these systems is associated with specific sets of modulation periodicities distributed throughout the Brillouin zone. Lattice dynamical calculations reveal selective disorder-driven phonon broadening that resembles the poorly understood ‘waterfall’ effect observed in relaxor ferroelectrics. This property of procrystalline solids suggests a mechanism by which strongly correlated topological disorder might allow independently optimized thermal and electronic transport behaviour, such as required for high-performance thermoelectrics.
机译:功能材料设计通常集中于结构有序的系统,因为混乱被认为对许多功能特性有害。在这里,我们通过显示特定类型的高度相关的障碍可以产生有序状态无法获得的有用特征,来挑战这种范式。低对称建筑单元和高对称拓扑模板的明智组合会导致非周期性的“前晶体”固体具有这种类型的混乱。我们确定前晶态的关键类别及其特征衍射行为,并建立到已知材料和目标材料的映射。在这些系统中发现的高度相关的疾病与分布在整个布里渊区中的特定调制周期集相关。晶格动力学计算表明,选择性失调驱动的声子变宽,类似于在弛张铁电体中观察到的鲜为人知的“瀑布”效应。原晶固体的这种性质表明了一种机制,通过该机制,高度相关的拓扑异常可能允许独立优化的热和电子传输行为,例如高性能热电学所要求的行为。

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