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中国物理学会期刊

铁基超导衍生体系CaCo2As2的磁结构

Magnetic Structure of the Iron-Based Superconductor Derived System CaCo2As2

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  • CCaCo2As2是铁基超导“122”体系的钴基衍生物,其低温磁基态与塌缩四方结构、费米能级附近的Co 3d电子态以及Co缺位密切相关。本文以CaCo2As2单晶为研究对象,结合电输运、磁性测量和单晶中子衍射实验,系统研究其晶体结构和低温磁基态。实验结果表明,该样品表现出金属性输运特征,并在低温下发生反铁磁相变;磁化率和等温磁化曲线显示出明显的磁各向异性,说明其磁有序具有显著的单轴特征。单晶中子衍射结果进一步表明,样品保持ThCr2Si2型塌缩四方结构,并存在一定程度的Co缺位。低温磁衍射结果直接确认了CCaCo2As2的A型反铁磁结构,即Co磁矩在层内铁磁排列、相邻层间反铁磁排列,且磁矩主要沿c轴方向取向。进一步的变温中子衍射结果表明,该磁有序的相变奈尔温度为TN ≈ 36 K。与已有报道相比,本文样品具有更高的Co缺位浓度、较低的TN和类似的有序磁矩大小,支持了先前对CCaCo2As2体系中较低的磁相变温度可能与Co缺位对磁相互作用的削弱有关的认识。本研究为理解CCaCo2As2中塌缩四方结构、Co缺位与巡游磁性之间的耦合关系提供了实验依据。

     

    CaCo2As2, an isostructural cobalt analogue of the “122” iron arsenides, provides a useful platform for investigating the interplay among a collapsed-tetragonal lattice, itinerant Co 3d electrons, and transitionmetal-site vacancies. Although its low-temperature magnetic ground state is known to be sensitive to the Co 3d states near the Fermi level and to Co deficiency, the connection between the actual Co occupancy and the magnetic ordering temperature remains to be clarified. Here we investigate the crystal structure and low-temperature magnetic order of a self-flux-grown CaCo2As2 single crystal using electrical transport, magnetization, and single-crystal neutron diffraction measurements. The resistance decreases monotonically on cooling, confirming metallic transport. No pronounced resistive anomaly is observed at the magnetic transition, suggesting that the onset of long-range antiferromagnetic order only weakly affects carrier scattering in this itinerant system. Magnetic susceptibility and isothermal magnetization measured for H || ab and H || c reveal pronounced uniaxial anisotropy. In particular, the low-temperature M(H) curve for H || c exhibits a field-induced spin-flop transition, identifying the c axis as the magnetic easy axis. Single-crystal neutron diffraction at 45 K, in the paramagnetic state, confirms the ThCr2Si2-type collapsed-tetragonal structure, with a = b = 3.989 Å, c = 10.330 Å, and an interlayer As-As distance of 2.7577 Å. Refinement of the nuclear structure gives a Co occupancy of 88.8(1.6)%, corresponding to CaCo1.78(3)As2, indicating a relatively high concentration of Co vacancies. Upon cooling to 4 K, eight additional Bragg reflections, (111), (113), (115), (-111), (-113), (-115), (201), and (203), appear at positions forbidden by the body-centered nuclear structure. These reflections are magnetic in origin and can be indexed with the propagation vector k = (0, 0, 1). This magnetic propagation vector identifies an Atype antiferromagnetic structure, with ferromagnetic alignment of Co moments within each Co layer and antiferromagnetic stacking between adjacent layers. The absence of a resolvable (001) magnetic reflection further indicates that the ordered moments are oriented predominantly along the c axis. Symmetry analysis yields two candidate magnetic space groups compatible with c-axis moments. The PI42/mnm model is ruled out by the observed extinction conditions, whereas the PI4/nnc model accounts for the measured magnetic intensities and gives an ordered moment of 0.311(15)μB/Co at 4 K. Temperature-dependent neutron diffraction of the (111) magnetic reflection gives a Néel temperature of TN ≈ 36 K. Compared with previous reports, the present crystal has a higher Co-vacancy concentration, a substantially lower TN, and a similarly small ordered moment. These results indicate that Co vacancies primarily weaken the Co-Co exchange network and suppress the ordering temperature of the itinerant A-type antiferromagnetic state, rather than substantially altering the ordered moment. Our results provide microscopic evidence for the coupled roles of collapsed-tetragonal bonding, transition-metal-site vacancies, and itinerant magnetism in CaCo2As2.

     

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