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From magnetic order to quantum disorder in the Zn-barlowite series of S  = 1/2 kagomé antiferromagnets
npj Quantum Materials ( IF 5.4 ) Pub Date : 2020-10-23 , DOI: 10.1038/s41535-020-00276-4
Katherine Tustain , Brendan Ward-O’Brien , Fabrice Bert , Tianheng Han , Hubertus Luetkens , Tom Lancaster , Benjamin M. Huddart , Peter J. Baker , Lucy Clark

We report a comprehensive muon spectroscopy study of the Zn-barlowite series of \(S=\frac{1}{2}\) kagomé antiferromagnets, ZnxCu4−x(OH)6FBr, for x = 0.00 to 0.99(1). By combining muon spin relaxation and rotation measurements with state-of-the-art density-functional theory muon-site calculations, we observe the formation of both μ–F and μ–OH complexes in Zn-barlowite. From these stopping sites, implanted muon spins reveal the suppression of long-range magnetic order into a possible quantum spin liquid state upon the increasing concentration of Zn-substitution. In the parent compound (x = 0), static long-range magnetic order below TN = 15 K manifests itself in the form of spontaneous oscillations in the time-dependent muon asymmetry signal consistent with the dipolar fields expected from the calculated muon stopping sites and the previously determined magnetic structure of barlowite. Meanwhile, in the x = 1.0 end-member of the series—in which antiferromagnetic kagomé layers of Cu2+\(S=\frac{1}{2}\) moments are decoupled by diamagnetic Zn2+ ions—we observe that dynamic magnetic moment fluctuations persist down to at least 50 mK, indicative of a quantum disordered ground state. We demonstrate that this crossover from a static to dynamic magnetic ground state occurs for compositions of Zn-barlowite with x > 0.5, which bears resemblance to the dynamical behaviour of the widely studied Zn-paratacamite series that contains the quantum spin liquid candidate herbertsmithite.



中文翻译:

从S = 1/2kagomé反铁磁体的Zn-重晶石系列中的磁阶到量子无序

我们报告了\(S = \ frac {1} {2} \) kagomé反铁磁体Zn x Cu 4− x(OH)6 FBr的Zn-重晶石系列的全面muon光谱研究,x  = 0.00至0.99( 1)。由μ介子自旋松弛和旋转测量与国家的最先进的密度泛函理论μ介子现场计算相结合,我们观察二者的形成μ -F和μ -OH络合物的Zn-barlowite。从这些停止位点开始,注入的介子自旋揭示了随着Zn取代浓度的增加,远距离磁阶被抑制为可能的量子自旋液态。在母体化合物(x = 0)时,低于T N  = 15 K的静态远程磁阶以与时间相关的μon不对称信号中的自发振荡的形式表现出来,该信号与从计算出的muon停止位点和先前确定的磁结构所预期的偶极场一致的重晶石。同时,在该 序列的x = 1.0端部成员中,Cu 2+的反铁磁kagomé层(S = \ frac {1} {2} \)矩被反磁性Zn 2+解耦离子—我们观察到,动态磁矩波动至少会降低到50 mK,这表明量子无序基态。我们证明,这种从静态到动态磁基态的转换发生在x  > 0.5的锌-巴洛石的成分上,这与广泛研究的包含量子自旋液体候选铁矾的Zn-paracamelite系列的动力学行为相似。

更新日期:2020-10-28
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