No Arabic abstract
Recently, several putative quantum spin liquid (QSL) states were discovered in ${tilde S} = 1/2$ rare-earth based triangular-lattice antiferromagnets (TLAF) with the delafossite structure. A way to clarify the origin of the QSL state in these systems is to identify ways to tune them from the putative QSL state towards long-range magnetic order. Here, we introduce the Ce-based TLAF KCeS$_2$ and show via low-temperature specific heat and $mu$SR investigations that it yields magnetic order below $T_{mathrm N} = 0.38$ K despite the same delafossite structure. We identify a well separated ${tilde S} = 1/2$ ground state for KCeS$_2$ from inelastic neutron scattering and embedded-cluster quantum chemical calculations. Magnetization and electron spin resonance measurements on single crystals indicate a strong easy-plane $g$~factor anisotropy, in agreement with the ab initio calculations. Finally, our specific-heat studies reveal an in-plane anisotropy of the magnetic field-temperature phase diagram which may indicate anisotropic magnetic interactions in KCeS$_2$.
We report on high-field electron spin resonance (ESR) studies of magnetic excitations in the spin-1/2 triangular-lattice antiferromagnet Cs$_2$CuBr$_4$. Frequency-field diagrams of ESR excitations are measured for different orientations of magnetic fields up to 25 T. We show that the substantial zero-field energy gap, $Deltaapprox9.5$ K, observed in the low-temperature excitation spectrum of Cs$_2$CuBr$_4$ [Zvyagin $et~al.$, Phys. Rev. Lett. 112, 077206 (2014)], is present well above $T_N$. Noticeably, the transition into the long-range magnetically ordered phase does not significantly affect the size of the gap, suggesting that even below $T_N$ the high-energy spin dynamics in Cs$_2$CuBr$_4$ is determined by short-range-order spin correlations. The experimental data are compared with results of model spin-wave-theory calculations for spin-1/2 triangle-lattice antiferromagnet.
Oxide double perovskites wherein octahedra formed by both 3d elements and sp-based heavy elements give rise to unconventional magnetic ordering and correlated quantum phenomena crucial for futuristic applications. Here, by carrying out experimental and first principles investigations, we present the electronic structure and magnetic phases of Ba2MnTeO6, where Mn^2+ ions with S = 5/2 spins constitute a perfect triangular lattice. The magnetic susceptibility reveals a large Curie- Weiss temperature -152 K suggesting the presence of strong antiferromagnetic interactions between Mn^2+ moments in the spin lattice. A phase transition at 20 K is revealed by magnetic susceptibility and specific heat which is attributed to the presence of a sizeable inter-plane interactions. Below the transition temperature, the specific heat data show antiferromagnetic magnon excitations with a gap of 1.4 K. Furthermore, muon spin-relaxation reveals the presence of static internal fields in the ordered state and provides strong evidence of short-range spin correlations for T > TN. The DFT+U calculations and spin-dimer analysis infer that Heisenberg interactions govern the inter and intra-layer spin-frustrations in this perovskite. The inter and intra-layer exchange interactions are of comparable strengths (J1 = 4.6 K, J2 = 0.92 J1). However, a weak third nearest-neighbor ferromagnetic inter-layer interaction exists (J3=-0.04 J1) due to double-exchange interaction via the linear path Mn-O-Te-O-Mn. The combined effect of J2 and J3 interactions stabilizes a three dimensional long-range magnetic ordering in this frustrated magnet.
We report on the low-energy dynamics in the kagome antiferromagnet CaCu$_3$(OD)$_6$Cl$_2cdot0.6$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 (D$_{rm OD}$), we find no peak at $T_s$, evidencing that the high-temperature peak is not related to the molecular dynamics of the OD groups. We discuss the possibility of a frustration-induced short-range ordered state below $T_s$ before the long-range order is stabilized by the Dzyaloshinskii-Moriya interaction. We also observed static internal fields at the D$_{rm OD}$ site in the long-range ordered state below $T^{ast}$, and confirm the previously proposed negative-chirality $q=0$ magnetic structure.
We study effects of nonmagnetic impurities in a spin-1/2 frustrated triangular antiferromagnet with the aim of understanding the observed broadening of $^{13}$C NMR lines in the organic spin liquid material $kappa$-(ET)$_2$Cu$_2$(CN)$_3$. For high temperatures down to $J/3$, we calculate local susceptibility near a nonmagnetic impurity and near a grain boundary for the nearest neighbor Heisenberg model in high temperature series expansion. We find that the local susceptibility decays to the uniform one in few lattice spacings, and for a low density of impurities we would not be able to explain the line broadening present in the experiments already at elevated temperatures. At low temperatures, we assume a gapless spin liquid with a Fermi surface of spinons. We calculate the local susceptibility in the mean field and also go beyond the mean field by Gutzwiller projection. The zero temperature local susceptibility decays as a power law and oscillates at $2 k_F$. As in the high temperature analysis we find that a low density of impurities is not able to explain the observed broadening of the lines. We are thus led to conclude that there is more disorder in the system. We find that a large density of point-like disorder gives broadening that is consistent with the experiment down to about 5K, but that below this temperature additional mechanism is likely needed.
The crystal structure and magnetic correlations in triangular antiferromagnet FeGa$_2$S$_4$ are studied by x-ray diffraction, magnetic susceptibility, neutron diffraction and neutron inelastic scattering. We report significant mixing at the cation sites and disentangle magnetic properties dominated by major and minor magnetic sites. The magnetic short-range correlations at 0.77 AA$^{-1}$ correspond to the major sites and being static at base temperature they evolve into dynamic correlations around 30 - 50 K. The minor sites contribute to the magnetic peak at 0.6 AA$^{-1}$, which vanishes at 5.5 K. Our analytical studies of triangular lattice models with bilinear and biquadratic terms provide the ratios between exchanges for the proposed ordering vectors. The modelling of the inelastic neutron spectrum within linear spin wave theory results in the set of exchange couplings $J_1=1.7$,meV, $J_2=0.9$,meV, $J_3=0.8$,meV for the bilinear Heisenberg Hamiltonian. However, not all features of the excitation spectrum are explained with this model.