The search for the resonating valence bond (RVB) state continues to underpin many areas of condensed matter research. The RVB is made from the dimerisation of spins on different sites into fluctuating singlets, and was proposed by Anderson to be the reference state from which the transition to BCS superconductivity occurs. Little is known about the state experimentally, due to the scarcity of model materials. Theoretical work has put forward the S = 1/2 kagome antiferromagnet (KAFM) as a good candidate for the realization of the RVB state. In this paper we introduce a new model system, the S = 1/2 KAFM Kapellasite, Cu3Zn(OH)6Cl2. We show that its crystal structure is a good approximation to a 2-dimensional kagome antiferromagnet and that susceptibility data indicate a collapse of the magnetic moment below T = 25 K that is compatible with the spins condensing into the non-magnetic RVB state.
The recently discovered natural minerals Cu3Zn(OH)6Cl2 and Cu3Mg(OH)6Cl2 are spin 1/2 systems with an ideal kagome geometry. Based on electronic structure calculations, we develop a realistic model which includes couplings across the kagome hexagons beyond the original kagome model that are intrinsic in real kagome materials. Exact diagonalization studies for the derived model reveal a strong impact of these couplings on the magnetic ground state. Our predictions could be compared to and supplied with neutron scattering, thermodynamic and NMR data.
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.
We investigate the magnetism of a previously unexplored distorted spin-1/2 kagome model consisting of three symmetry-inequivalent nearest-neighbor antiferromagnetic Heisenberg couplings Jhexagon, J and J', and uncover a rich ground state phase diagram even at the classical level. Using analytical arguments and numerical techniques we identify a collinear Q = 0 magnetic phase, two unusual non-collinear coplanar Q = (1/3,1/3) phases and a classical spin liquid phase with a degenerate manifold of non-coplanar ground states, resembling the jammed spin liquid phase found in the context of a bond-di…
We present a method to build magnetic models for insulators based on high-temperature expansions by fitting both the magnetic susceptibility and the low temperature specific heat data. It is applied to the frustrated magnet kapellasite (Cu3Zn(OH)6Cl2) with the J1-J2-Jd-Heisenberg model on the kagome lattice. Experimental data are reproduced with a set of "competing" exchange energies closed to J1 = -12K, J2= -4K and Jd=15.6K, where Jd is the third neighbor exchange energy across the hexagon. Strong constrains between these exchange energies are established. These values confirm the results of …
We present a $^{35}$Cl NMR study for spin $S=1/2$ perfect kagome antiferromagnet Ca-kapellasite (CaCu$_{3}$(OH)$_{6}$Cl$_{2}\cdot$0.6H$_{2}$O) with a magnetic transition at $T^{\ast}=7.2$ K. The static magnetic structure in the ground state has been determined to be a chirality-ordered $Q=0$ state, which is selected by a finite Dzyaloshinskii-Moriya interaction. The low-energy magnetic excitations in the ordered state are investigated by the nuclear spin-lattice relaxation rate measurement. We detect a weakly temperature dependent contribution in the magnetic fluctuations perpendicular to the …
We report $^{35}$Cl NMR, ESR, $μ$SR and specific heat measurements on the $S=1/2$ frustrated kagomé magnet kapellasite, $α-$Cu$_3$Zn(OH)$_6$Cl$_2$, where a gapless spin liquid phase is stabilized by a set of competing exchange interactions. Our measurements confirm the ferromagnetic character of the nearest-neighbour exchange interaction $J_1$ and give an energy scale for the competing interactions $|J| \sim 10$ K. The study of the temperature-dependent ESR lineshift reveals a moderate symmetric exchange anisotropy term $D$, with $|D/J|\sim 3$%. These findings validate a posteriori the use of …
Gapped 1/9 Magnetization Plateau in the Anisotropic Kagome Antiferromagnet Y-kapellasite
Université Paris-Saclay（巴黎萨克雷大学）；CNRS（法国国家科学研究中心）；Laboratoire de Physique des Solides（固体物理实验室）；Clarendon Laboratory, Department of Physics, University of Oxford（牛津大学克拉伦登实验室物理系）；Department of Physics, University of Warwick（华威大学物理系）；Physikalisches Institut, Goethe-Universität Frankfurt（法兰克福歌德大学物理研究所）；Laboratoire National des Champs Magnétiques Intenses, LNCMI-CNRS (UPR3228), EMFL, Univ. Grenoble Alpes, Univ. Toulouse, INSA-T（强磁场国家实验室，LNCMI-CNRS (UPR3228)，欧洲强磁场联合实验室，格勒诺布尔阿尔卑斯大学，图卢兹大学，INSA-T）；Max-Planck-Institute for So（马克斯·普朗克研究所）
Frustrated magnetism on the kagome lattice has been a fertile ground for rich and fascinating physics, ranging from experimental evidence of a spin liquid to theoretical predictions of exotic superconductivity. Among experimentally realized spin-$\frac{1}{2}$ kagome magnets, herbertsmithite, kapellasite, and haydeeite [(Zn,Mg)Cu$_{3}$(OH)$_{6}$Cl$_{2}$] are all well described by a three-parameter Heisenberg model, but they exhibit distinctly different physics. We address the problem using a pseudofermion functional renormalization-group approach and analyze the low-energy physics in the experi…
A clear thermal Hall signal ($κ_{xy}$) was observed in the spin liquid phase of the $S=1/2$ kagomé antiferromagnet Ca kapellasite (CaCu$_3$(OH)$_6$Cl$_2\cdot 0.6$H$_2$O). We found that $κ_{xy}$ is well reproduced, both qualitatively and quantitatively, using the Schwinger-boson mean-field theory with the Dzyaloshinskii--Moriya interaction of $D/J \sim 0.1$. In particular, $κ_{xy}$ values of Ca kapellasite and those of another kagomé antiferromagnet, volborthite, converge to one single curve in simulations modeled using Schwinger bosons, indicating a common temperature dependence of $κ_{xy}$ fo…
We have investigated the thermal-transport properties of the kagome antiferromagnet Cd-kapellasite (Cd-K). We find that a field suppression effect on the longitudinal thermal conductivity k_xx sets in below ~25 K, suggesting a large spin contribution k_xx^sp in k_xx. We also find clear thermal Hall signals in the spin liquid phase in all Cd-K samples. The magnitude of the thermal Hall conductivity k_xy shows a significant dependence on the sample's scattering time. On the other hand, the temperature dependence of k_xy is similar in all Cd-K samples; k_xy shows a peak at almost the same tempera…
Motivated by recent experiments on the Heisenberg S=1/2 quantum spin liquid candidate material kapellasite, we classify all possible chiral (time-reversal symmetry breaking) spin liquids with fermionic spinons on the kagome lattice. We obtain the phase diagram for the physically relevant extended Heisenberg model, comparing the energies of a wide range of microscopic variational wave functions. We propose that, at low temperature, kapellasite exhibits a gapless chiral spin liquid phase with spinon Fermi surfaces. This two-dimensional state inherits many properties of the nearby one-dimensional…
Recent discoveries in neutron scattering experiments for Kapellasite and Herbertsmithite as well as theoretical calculations of possible spin liquid phases have revived interest in magnetic phenomena on the kagome lattice. We study the quantum phase diagram of the S=1/2 Heisenberg kagome model as a function of nearest neighbor coupling J1 and second neighbor coupling J2. Employing the pseudofermion functional renormalization group, we find four types of magnetic quantum order (q=0 order, cuboc order, ferromagnetic order, and Sqrt{3}x\Sqrt{3} order) as well as extended magnetically disordered r…
Ab Initio Investigation of Pressure Effects in the Spin-Liquid Candidate Y-Kapellasite
European Synchrotron Radiation Facility（欧洲同步辐射装置）；Institute for Quantum Materials and Technologies, Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院量子材料与技术研究所）；Institut für Theoretische Physik, Goethe-Universitat Frankfurt（法兰克福歌德大学理论物理研究所）；Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）
Herbertsmithite (ZnCu3(OH)6Cl2) is often discussed as the best realization of the highly frustrated antiferromagnetic kagome lattice known so far. We employ density functional theory calculations to determine eight exchange coupling constants of the underlying Heisenberg Hamiltonian. We find the nearest neighbour coupling J1 to exceed all other couplings by far. However, next-nearest neighbour kagome layer couplings of 0.019 J1 and interlayer couplings of up to -0.035 J1 slightly modify the perfect antiferromagnetic kagome Hamiltonian. Interestingly, the largest interlayer coupling is ferromag…
Using a perturbative renormalization group approach, we show that the extended ($J_1$-$J_2$-$J_d$) Heisenberg model on the kagome lattice with a staggered chiral interaction ($J_χ$) can exhibit a gapless chiral quantum spin liquid phase. Within a coupled-chains construction, this phase can be understood as a chiral sliding Luttinger liquid with algebraic decay of spin correlations along the chain directions. We calculate the low-energy properties of this gapless chiral spin liquid using the effective field theory and show that they are compatible with the predictions from parton mean-field the…
Spin-1/2 magnets with kagome geometry, being for years a generic object of theoretical investigations, have few real material realizations. Recently, a DFT-based microscopic model for two such materials, kapellasite Cu3Zn(OH)6Cl2 and haydeeite Cu3Mg(OH)6Cl2, was presented [O. Janson, J. Richter and H. Rosner, arXiv:0806.1592]. Here, we focus on the intrinsic properties of real spin-1/2 kagome materials having influence on the magnetic ground state and the low-temperature excitations. We find that the values of exchange integrals are strongly dependent on O--H distance inside the hydroxyl group…
Search for a new quantum state of matter emerging in a crystal is one of recent trends in condensed matter physics. For magnetic materials, geometrical frustration and high magnetic field are two key ingredients to realize it: a conventional magnetic order is possibly destroyed by competing interactions (frustration) and is replaced by an exotic state that is characterized in terms of quasiparticles, that are magnons, and the magnetic field can control the density and chemical potential of the magnons. Here we show that a synthetic copper mineral, Cd-kapellasite, comprising a kagome lattice ma…
We report on the low-energy dynamics in the kagome antiferromagnet CaCu$_3$(OD)$_6$Cl$_2\cdot0.6$D$_2$O (Ca-kapellasite) as studied by use of $^2$D-NMR measurements. Previous $^{35}$Cl-NMR measurements revealed that the nuclear spin-lattice relaxation rate ($1/T_1$) shows two peaks at temperatures, $T^{\ast} = 7.2$ K and $T_s \simeq 25$ K. While the low-temperature peak at $T^{\ast}$ is ascribed to the critical fluctuations near the long-range magnetic ordering, the origin of the high-temperature peak has not been fully understood. From the $1/T_1$ measurements on the D sites at the OD groups …
