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Register a new userSite-Specific Structure at Multiple Length Scales in Kagome Quantum Spin Liquid Candidates
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Realizing a quantum spin liquid (QSL) ground state in a real material is a leading issue in condensed matter physics research. In this pursuit, it is crucial to fully characterize the structure and influence of defects, as these can significantly affect the fragile QSL physics. Here, we perform a variety of cutting-edge synchrotron X-ray scattering and spectroscopy techniques, and we advance new methodologies for site-specific diffraction and L-edge Zn absorption spectroscopy. The experimental results along with our first-principles calculations address outstanding questions about the local and long-range structures of the two leading kagome QSL candidates, Zn-substituted barlowite Cu$_3$Zn$_{x}$Cu$_{1-x}$(OH)$_6$FBr and herbertsmithite Cu$_3$Zn(OH)$_6$Cl$_2$. On all length scales probed, there is no evidence that Zn substitutes onto the kagome layers, thereby preserving the QSL physics of the kagome lattice. Our calculations show that antisite disorder is not energetically favorable and is even less favorable in Zn-barlowite compared to herbertsmithite. Site-specific X-ray diffraction measurements of Zn-barlowite reveal that Cu$^{2+}$ and Zn$^{2+}$ selectively occupy distinct interlayer sites, in contrast to herbertsmithite. Using the first measured Zn L-edge inelastic X-ray absorption spectra combined with calculations, we discover a systematic correlation between the loss of inversion symmetry from pseudo-octahedral (herbertsmithite) to trigonal prismatic coordination (Zn-barlowite) with the emergence of a new peak. Overall, our measurements suggest that Zn-barlowite has structural advantages over herbertsmithite that make its magnetic properties closer to an ideal QSL candidate: its kagome layers are highly resistant to nonmagnetic defects while the interlayers can accommodate a higher amount of Zn substitution.
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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.
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.
Magnetic susceptibility, NMR, muSR, and inelastic neutron scattering measurements show that kapellasite, Cu3Zn(OH)6Cl2, a geometrically frustrated spin-1/2 kagome antiferromagnet polymorphous with the herbertsmithite mineral, is a gapless spin liquid with frustrated interactions showing unusual dynamic short-range correlations of non-coplanar cuboc2 type which persist down to 20 mK. The Hamiltonian is determined from a fit of a high-temperature series expansion to thermodynamical data. The experimental data are compared to theoretical calculations using the Schwinger-boson approach.
A promising route to realize entangled magnetic states combines geometrical frustration with quantum-tunneling effects. Spin-ice materials are canonical examples of frustration, and Ising spins in a transverse magnetic field are the simplest many-body model of quantum tunneling. Here, we show that the tripod kagome lattice material Ho${_3}$Mg${_2}$Sb${_3}$O${_{14}}$ unites an ice-like magnetic degeneracy with quantum-tunneling terms generated by an intrinsic splitting of the Ho$^{3+}$ ground-state doublet, which is further coupled to a nuclear spin bath. Using neutron scattering and thermodynamic experiments, we observe a symmetry-breaking transition at $T^{ast}approx0.32$ K to a remarkable state with three peculiarities: a concurrent recovery of magnetic entropy associated with the strongly coupled electronic and nuclear degrees of freedom; a fragmentation of the spin into periodic and ice-like components; and persistent inelastic magnetic excitations down to $Tapprox0.12$ K. These observations deviate from expectations of classical spin fragmentation on a kagome lattice, but can be understood within a model of dipolar kagome ice under a homogeneous transverse magnetic field, which we survey with exact diagonalization on small clusters and mean-field calculations. In Ho${_3}$Mg${_2}$Sb${_3}$O${_{14}}$, hyperfine interactions dramatically alter the single-ion and collective properties, and suppress possible quantum correlations, rendering the fragmentation with predominantly single-ion quantum fluctuations. Our results highlight the crucial role played by hyperfine interactions in frustrated quantum magnets, and motivate further investigations of the role of quantum fluctuations on partially-ordered magnetic states.
The theory of deconfined quantum critical points describes phase transitions at temperature T = 0 outside the standard paradigm, predicting continuous transformations between certain ordered states where conventional theory requires discontinuities. Numerous computer simulations have offered no proof of such transitions, however, instead finding deviations from expected scaling relations that were neither predicted by the DQC theory nor conform to standard scenarios. Here we show that this enigma can be resolved by introducing a critical scaling form with two divergent length scales. Simulations of a quantum magnet with antiferromagnetic and dimerized ground states confirm the form, proving a continuous transition with deconfined excitations and also explaining anomalous scaling at T > 0. Our findings revise prevailing paradigms for quantum criticality, with potentially far-reaching implications for many strongly-correlated materials.
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