层状结构1 T '-TaTe2中三聚体超结构的超快光学熔化
Ultrafast optical melting of trimer superstructure in layered 1T'-TaTe2
摘要:
准二维过渡金属二硫属化物是探索复杂相互作用所产生的纳米现象的关键平台。访问其自然时间尺度上的基本自由度激励使用先进的超快探头敏感的自组织原子尺度模式。在这里,我们报告的第一个超快调查的TaTe 2,它具有独特的电荷和晶格三聚体的顺序,其特征在于冷却后从条纹状链过渡到一个$(3 \times 3)$超结构的三聚体簇。利用兆电子伏级的超快电子衍射,我们捕获的光诱导TaTe 2结构动力学-暴露一个快速的$\approx\!1.4$ PS熔化其低温有序状态,然后通过热恢复成一个热的集群超结构。密度泛函计算表明,初始淬火是由内三聚体Ta电荷转移,不稳定的集群,不像其他TaX 2化合物中的电荷密度波熔化触发。我们的工作为进一步探索和最终快速的光学和电子操纵三聚体超结构铺平了道路。
英文摘要:
Quasi-two-dimensional transition-metal dichalcogenides are a key platform for exploring emergent nanoscale phenomena arising from complex interactions. Access to the underlying degrees-of-freedom on their natural time scales motivates the use of advanced ultrafast probes sensitive to self-organised atomic-scale patterns. Here, we report the first ultrafast investigation of TaTe2, which exhibits unique charge and lattice trimer order characterised by a transition upon cooling from stripe-like chains into a $(3 \times 3)$ superstructure of trimer clusters. Utilising MeV-scale ultrafast electron diffraction, we capture the photo-induced TaTe2 structural dynamics -- exposing a rapid $\approx\!1.4$ ps melting of its low-temperature ordered state followed by recovery via thermalisation into a hot cluster superstructure. Density-functional calculations indicate that the initial quench is triggered by intra-trimer Ta charge transfer which destabilises the clusters, unlike melting of charge density waves in other TaX2 compounds. Our work paves the way for further exploration and ultimately rapid optical and electronic manipulation of trimer superstructures.
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