Mantravadi Aishwarya, Weaver Bradyn C, Chen Shiya, Mukta Shahnaz, Abusa Yao, Sarkar Arka, Sun Yang, Mudryk Yaroslav, Gundlach-Graham Alexander, Ho Kai-Ming, Lebedev Oleg I, Zaikina Julia V
Department of Chemistry, Iowa State University, Ames, Iowa 50011, United States.
Department of Physics, Xiamen University, Xiamen 361005, China.
J Am Chem Soc. 2024 Oct 2;146(39):26786-26800. doi: 10.1021/jacs.4c07285. Epub 2024 Sep 21.
2D materials showcase unconventional properties emerging from quantum confinement effects. In this work, a "soft chemical" route allows for the deintercalation of K from the layered antimonide KVSb, resulting in the discovery of a new metastable 2D-Kagome antimonide KVSb with a van der Waals gap of 3.2 Å. The structure of KVSb was determined via the synergistic techniques, including X-ray pair distribution function analysis, advanced transmission electron microscopy, and density functional theory calculations. The KVSb compound crystallizes in the monoclinic space group 2/ ( = 9.57(2) Å, = 5.502(8) Å, = 10.23(2) Å, β = 97.6(2)°, = 2). The [VSb] layers in KVSb are retained upon deintercalation and closely resemble the layers in the parent compound, yet deintercalation results in a relative shift of the adjacent [VSb] layers. The magnetic properties of the KVSb phase in the 2-300 K range are comparable to those of KVSb and another Kagome antimonide KVSb, consistent with nearly temperature-independent paramagnetism. Electronic band structure calculation suggests a nontrivial band topology with flat bands and opening of band crossing afforded by deintercalation. Transport property measurements reveal a metallic nature for KVSb and a low thermal conductivity of 0.6 W K m at 300 K. Additionally, ion exchange in KVSb via a solvothermal route leads to a successful partial exchange of K with ( = Na, Rb, and Cs). This study highlights the tunability of the layered structure of the KVSb compound, providing a rich playground for the realization of new 2D materials.
二维材料展现出源于量子限域效应的非常规特性。在这项工作中,一种“软化学”途径实现了从层状锑化物KVSb中脱嵌钾,从而发现了一种新的亚稳二维 Kagome 锑化物KVSb,其范德华间隙为3.2 Å。KVSb的结构通过包括X射线对分布函数分析、先进透射电子显微镜和密度泛函理论计算在内的协同技术得以确定。KVSb化合物结晶于单斜空间群2/ ( = 9.57(2) Å, = 5.502(8) Å, = 10.23(2) Å,β = 97.6(2)°, = 2)。脱嵌后KVSb中的[VSb]层得以保留,且与母体化合物中的层非常相似,但脱嵌导致相邻[VSb]层发生相对位移。KVSb相在2 - 300 K范围内的磁性与KVSb以及另一种Kagome锑化物KVSb的磁性相当,符合几乎与温度无关的顺磁性。电子能带结构计算表明其具有非平凡的能带拓扑结构,存在平带且脱嵌导致能带交叉打开。输运性质测量揭示KVSb具有金属特性,在300 K时热导率低至0.6 W K m 。此外,通过溶剂热途径在KVSb中进行离子交换成功实现了K与 ( = Na、Rb和Cs)的部分交换。这项研究突出了KVSb化合物层状结构的可调控性,为新型二维材料的实现提供了丰富的研究空间。