Cheng Jingwen, Bai Jianli, Ruan Binbin, Liu Pinyu, Huang Yu, Dong Qingxin, Huang Yifei, Sun Yingrui, Li Cundong, Zhang Libo, Liu Qiaoyu, Zhu Wenliang, Ren Zhian, Chen Genfu
Institute of Physics and Beijing National Laboratory for Condensed Matter Physics, Chinese Academy of Sciences, Beijing 100190, China.
School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.
J Am Chem Soc. 2024 Mar 6;146(9):5908-5915. doi: 10.1021/jacs.3c11968. Epub 2024 Feb 23.
Unconventional superconductivity in bulk materials under ambient pressure is extremely rare among the 3d transition metal compounds outside the layered cuprates and iron-based family. It is predominantly linked to highly anisotropic electronic properties and quasi-two-dimensional (2D) Fermi surfaces. To date, the only known example of a Co-based exotic superconductor is the hydrated layered cobaltate, NaCoO·HO, and its superconductivity is realized in the vicinity of a spin-1/2 Mott state. However, the nature of the superconductivity in these materials is still a subject of intense debate, and therefore, finding a new class of superconductors will help unravel the mysteries of their unconventional superconductivity. Here, we report the discovery of superconductivity at ∼6.3 K in our newly synthesized layered compound NaCoSeO, in which the edge-shared CoSe octahedra form [CoSe] layers with a perfect triangular lattice of Co ions. It is the first 3d transition metal oxychalcogenide superconductor with distinct structural and chemical characteristics. Despite its relatively low , this material exhibits very high superconducting upper critical fields, μ(0), which far exceeds the Pauli paramagnetic limit by a factor of 3-4. First-principles calculations show that NaCoSeO is a rare example of a negative charge transfer superconductor. This cobalt oxychalcogenide with a geometrical frustration among Co spins shows great potential as a highly appealing candidate for the realization of unconventional and/or high- superconductivity beyond the well-established Cu- and Fe-based superconductor families and opens a new field in the physics and chemistry of low-dimensional superconductors.
在常压下,除层状铜酸盐和铁基家族外的3d过渡金属化合物中,块状材料中的非常规超导极为罕见。它主要与高度各向异性的电子特性和准二维(2D)费米面有关。迄今为止,已知的钴基奇异超导体的唯一例子是水合层状钴酸盐NaCoO₂·H₂O,其超导性在自旋1/2莫特态附近实现。然而,这些材料中超导性的本质仍是激烈争论的主题,因此,发现一类新的超导体将有助于揭开其非常规超导性的奥秘。在此,我们报告在新合成的层状化合物NaCoSeO₃中发现了约6.3K的超导性,其中边缘共享的CoSe₄八面体形成了具有完美Co离子三角形晶格的[CoSe₄]层。它是首个具有独特结构和化学特征的3d过渡金属氧硫族化合物超导体。尽管其转变温度相对较低,但该材料表现出非常高的超导上临界场μ₀(Hc2),比泡利顺磁极限高出3 - 4倍。第一性原理计算表明,NaCoSeO₃是负电荷转移超导体的罕见例子。这种在Co自旋间具有几何阻挫的钴氧硫族化合物作为实现超越成熟的铜基和铁基超导家族的非常规和/或高温超导的极具吸引力的候选材料,具有巨大潜力,并为低维超导体的物理和化学开辟了新领域。