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Register a new userUltralow-temperature heat transport in the quantum spin liquid candidate Ca10Cr7O28 with bilayer kagome lattice
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Recently, a novel material with bilayer kagome lattice Ca$_{10}$Cr$_7$O$_{28}$ was proposed to be a gapless quantum spin liquid, due to the lack of long-range magnetic order and the observation of broad diffuse excitations. Here, we present the ultralow-temperature thermal conductivity measurements on single crystals of Ca$_{10}$Cr$_7$O$_{28}$ to detect its low-lying magnetic excitations. At finite temperatures, with increasing the magnetic fields, the thermal conductivity exhibits a clear dip around 6 T, which may correspond to a crossover in the magnetic ground state. At the zero-temperature limit, no residual linear term is found at any fields, indicating the absence of gapless itinerant fermionic excitations. Therefore, if the spinons do exist, they are either localized or gapped. In the gapped case, the fitting of our data gives a small gap $Delta sim$ 0.27(2) K. These results put strong constraints on the theoretical description of the ground state in this quantum spin liquid candidate.
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Arguably the most favorable situation for spins to enter the long-sought quantum spin liquid (QSL) state is when they sit on a kagome lattice. No consensus has been reached in theory regarding the true ground state of this promising platform. The experimental efforts, relying mostly on one archetypal material ZnCu$_3$(OH)$_6$Cl$_2$, have also led to diverse possibilities. Apart from subtle interactions in the Hamiltonian, there is the additional degree of complexity associated with disorder in the real material ZnCu$_3$(OH)$_6$Cl$_2$ that haunts most experimental probes. Here we resort to heat transport measurement, a cleaner probe in which instead of contributing directly, the disorder only impacts the signal from the kagome spins. For ZnCu$_3$(OH)$_6$Cl$_2$ and a related QSL candidate Cu$_3$Zn(OH)$_6$FBr, we observed no contribution by any spin excitation nor any field-induced change to the thermal conductivity. These results impose different constraints on various scenarios about the ground state of these two kagome compounds: while a gapped QSL, or certain quantum paramagnetic state other than a QSL, is compatible with our results, a gapless QSL must be dramatically modified by the disorder so that gapless spin excitations are localized.
Frustrated quantum magnets are expected to host many exotic quantum spin states like quantum spin liquid (QSL), and have attracted numerous interest in modern condensed matter physics. The discovery of the triangular lattice spin liquid candidate YbMgGaO$_4$ stimulated an increasing attention on the rare-earth-based frustrated magnets with strong spin-orbit coupling. Here we report the synthesis and characterization of a large family of rare-earth chalcogenides AReCh$_2$ (A = alkali or monovalent ions, Re = rare earth, Ch = O, S, Se). The family compounds share the same structure (R$bar{3}$m) as YbMgGaO$_4$, and antiferromagnetically coupled rare-earth ions form perfect triangular layers that are well separated along the $c$-axis. Specific heat and magnetic susceptibility measurements on NaYbO$_2$, NaYbS$_2$ and NaYbSe$_2$ single crystals and polycrystals, reveal no structural or magnetic transition down to 50mK. The family, having the simplest structure and chemical formula among the known QSL candidates, removes the issue on possible exchange disorders in YbMgGaO$_4$. More excitingly, the rich diversity of the family members allows tunable charge gaps, variable exchange coupling, and many other advantages. This makes the family an ideal platform for fundamental research of QSLs and its promising applications.
In this paper, we performed thermodynamic and electron spin resonance (ESR) measurements to study low-energy magnetic excitations, which were significantly affected by crystalline electric field (CEF) excitations due to relatively small gaps between the CEF ground state and the excited states. Based on the CEF and mean-field (MF) theories, we analyzed systematically and consistently the ESR experiments and thermodynamic measurements including susceptibility, magnetization, and heat capacity. The CEF parameters were successfully extracted by fitting high-temperature (> 20 K) susceptibilities in the ab-plane and along the c-axis, allowing to determine the Lande factors ($g_{ab,calc}$ = 5.98(7) and $g_{c,calc}$ = 2.73(3)). These values were consistent with the values of Lande factors determined by ESR experiments ($g_{ab,exp}$ = 5.69 and $g_{c,exp}$ = 2.75). By applying the CEF and MF theories to the susceptibility and magnetization results, we estimated the anisotropic spin-exchange energies and found that the CEF excitations in ce{KErTe2} played a decisive role in the magnetism above 3 K, while the low-temperature magnetism below 10 K was gradually correlated with the anisotropic spin-exchange interactions. The CEF excitations were demonstrated in the low-temperature heat capacity, where both the positions of two broad peaks and their magnetic field dependence well corroborated our calculations. The present study provides a basis to explore the enriched magnetic and electronic properties of the QSL family.
The $S$ = $frac{1}{2}$ kagome Heisenberg antiferromagnet (KHA) is a leading model hosting a quantum spin liquid (QSL), but the exact nature of its ground state remains a key issue under debate. In the previously well-studied candidate materials, magnetic defects always dominate the low-energy spectrum and hinder the detection of the intrinsic nature. We demonstrate that the new single crystal of YCu$_3$[OH(D)]$_{6.5}$Br$_{2.5}$ is a perfect KHA without evident magnetic defects ($ll$ 0.8%). Through fitting the magnetic susceptibilities of the orientated single crystals, we find the spin system with weak anisotropic interactions and with first-, second-, and third-neighbor couplings, $J_1$ $sim$ 56 K and $J_2$ $sim$ $J_3$ $sim$ 0.1$J_1$, belongs to the continuous family of fully frustrated KHAs. No conventional freezing is observed down to 0.36 K $sim$ 0.006$J_1$, and the raw specific heat exhibits a nearly quadratic temperature dependence below 1 K $sim$ 0.02$J_1$, well consistent with a gapless (spin gap $leq$ 0.025$J_1$) Dirac QSL.
We present the ultralow-temperature specific heat and thermal conductivity measurements on single crystals of triangular-lattice organic compound EtMe$_3$Sb[Pd(dmit)$_2$]$_2$, which has long been considered as a gapless quantum spin liquid candidate. In specific heat measurements, a finite linear term is observed, consistent with the previous work [S. Yamashita $et$ $al.$, Nat. Commun. {bf 2}, 275 (2011)]. However, we do not observe a finite residual linear term in the thermal conductivity measurements, and the thermal conductivity does not change in a magnetic field of 6 Tesla. These results are in sharp contrast to previous thermal conductivity measurements on EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ [M. Yamashita $et$ $al.$ Science {bf 328}, 1246 (2010)], in which a huge residual linear term was observed and attributed to highly mobile gapless excitations, likely the spinons of a quantum spin liquid. In this context, the true ground state of EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ has to be reconsidered.
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