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Register a new userUnconventional magnetism in the 4d$^{4}$ based ($S=1$) honeycomb system Ag$_{3}$LiRu$_{2}$O$_{6}$
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We have investigated the thermodynamic and local magnetic properties of the Mott insulating system Ag$_{3}$LiRu$_{2}$O$_{6}$ containing Ru$^{4+}$ (4$d$$^{4}$) for novel magnetism. The material crystallizes in a monoclinic $C2/m$ structure with RuO$_{6}$ octahedra forming an edge-shared two-dimensional honeycomb lattice with limited stacking order along the $c$-direction. The large negative Curie-Weiss temperature ($theta_{CW}$ = -57 K) suggests antiferromagnetic interactions among Ru$^{4+}$ ions though magnetic susceptibility and heat capacity show no indication of magnetic long-range order down to 1.8 K and 0.4 K, respectively. $^{7}$Li nuclear magnetic resonance (NMR) shift follows the bulk susceptibility between 120-300 K and levels off below 120 K. Together with a power-law behavior in the temperature dependent spin-lattice relaxation rate between 0.2 and 2 K, it suggest dynamic spin correlations with gapless excitations. Electronic structure calculations suggest an $S = 1$ description of the Ru-moments and the possible importance of further neighbour interactions as also bi-quadratic and ring-exchange terms in determining the magnetic properties. Analysis of our $mu$SR data indicates spin freezing below 5 K but the spins remain on the borderline between static and dynamic magnetism even at 20 mK.
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The system Ag[Li$_{1/3}$Mn$_{2/3}$]O$_{2}$ belongs to a quaternary 3R-delafossite family and crystallizes in a monoclinic symmetry with space group $C,2/m$ and the magnetic Mn$^{4+}$($S=3/2$) ions form a honeycomb network in the $ab$-plane. An anomaly around 50 K and the presence of antiferromagnetic (AFM) coupling (Curie-Weiss temperature $theta_{CW}sim-51$ K) were inferred from our magnetic susceptibility data. The magnetic specific heat clearly manifests the onset of magnetic ordering in the vicinity of 48,K and the recovered magnetic entropy, above the ordering temperature, falls short of the expected value, implying the presence of short-range magnetic correlations. The (ESR) line broadening on approaching the ordering temperature $T_{{rm N}}$ could be described in terms of a Berezinski-Kosterlitz-Thouless (BKT) scenario with $T_{{rm KT}}=40(1)$ K. $^{7}$Li NMR line-shift probed as a function of temperature tracks the static susceptibility (K$_{iso}$) of magnetically coupled Mn$^{4+}$ ions. The $^{7}$Li spin-lattice relaxation rate (1/$T$$_{1}$) exhibits a sharp decrease below about 50 K. Combining our bulk and local probe measurements, we establish the presence of an ordered ground state for the honeycomb system Ag$_{3}$LiMn$_{2}$O$_{6}$.Our ab-initio electronic structure calculations suggest that in the $ab$-plane, the nearest neighbor (NN) exchange interaction is strong and AFM, while the next NN and the third NN exchange interactions are FM and AFM respectively. In the absence of any frustration the system is expected to exhibit long-range, AFM order, in agreement with experiment.
We report a combined $^{115}$In NQR, $^{51}$V NMR and $mu$SR spectroscopic study of the low-temperature magnetic properties of InCu$_{2/3}$V$_{1/3}$O$_3$, a quasi-two dimensional (2D) compound comprising in the spin sector a honeycomb lattice of antiferromagnetically coupled spins $S=1/2$ associated with Cu$^{2+}$ ions. Despite substantial experimental and theoretical efforts, the ground state of this material was has not been ultimately identified. In particular, two characteristic temperatures of about $sim 40$ K and $sim 20$ K manifesting themselves as anomalies in different magnetic measurements are discussed controversially. A combined analysis of the experimental data complemented with theoretical calculations of exchange constants enabled us to identify below 39 K an ``intermediate quasi-2D static spin state. This spin state is characterized by a staggered magnetization with a temperature evolution that agrees with the predictions for the 2D XY model. We observe that this state gradually transforms at 15 K into a fully developed 3D antiferromagnetic Neel state. We ascribe such an extended quasi-2D static regime to an effective magnetic decoupling of the honeycomb planes due to a strong frustration of the interlayer exchange interactions which inhibits long-range spin-spin correlations across the planes. Interestingly, we find indications of the topological Berezinsky-Kosterlitz-Thouless transition in the quasi-2D static state of the honeycomb spin-1/2 planes of InCu$_{2/3}$V$_{1/3}$O$_3$.
High field electron spin resonance, nuclear magnetic resonance and magnetization studies addressing the ground state of the quasi two-dimensional spin-1/2 honeycomb lattice compound InCu{2/3}V{1/3}O{3} are reported. Uncorrelated finite size structural domains occurring in the honeycomb planes are expected to inhibit long range magnetic order. Surprisingly, ESR data reveal the development of two collinear antiferromagnetic (AFM) sublattices below ~ 20 K whereas NMR results show the presence of the staggered internal field. Magnetization data evidence a spin reorientation transition at ~ 5.7 T. Quantum Monte-Carlo calculations show that switching on the coupling between the honeycomb spin planes in a finite size cluster yields a Neel-like AFM spin structure with a substantial staggered magnetization at finite temperatures. This may explain the occurrence of a robust AFM state in InCu{2/3}V{1/3}O{3} despite an unfavorable effect of structural disorder.
Recently, there have been contrary claims of Kitaev spin-liquid behaviour and ordered behavior in the honeycomb compound Ag$_3$LiIr$_2$O$_6$ based on various experimental signatures. Our investigations on this system reveal a low-temperature ordered state with persistent dynamics down to the lowest temperatures. Magnetic order is confirmed by clear oscillations in the muon spin relaxation ($mu$SR) time spectrum below 9 K till 52 mK. Coincidentally in $^7$Li nuclear magnetic resonance, a wipe-out of the signal is observed below $sim$ 10 K which again strongly indicates magnetic order in the low temperature regime. This is supported by our density functional theory calculations which show an appreciable Heisenberg exchange term in the spin Hamiltonian that favors magnetic ordering. The $^7$Li shift and spin-lattice relaxation rate also show anomalies at $sim$ 50 K. They are likely related to the onset of dynamic magnetic correlations, but their origin is not completely clear. Detailed analysis of our $mu$SR data is consistent with a co-existence of incommensurate Neel and striped environments. A significant and undiminished dynamical relaxation rate ($sim 5$ MHz) as seen in $mu$SR deep into the ordered phase indicates enhanced quantum fluctuations in the ordered state.
The S=3/2 Kitaev honeycomb model (KHM) has defied an analytical as well as numerical understanding because it is not exactly soluble like its S=1/2 brethren and in contrast to other spin-S Kitaev models numerical methods are plagued by a massive pile up of low energy states. Here, we uncover the phase diagram of the S=3/2 KHM and find gapped and gapless quantum spin liquids (QSLs) generally coexisting with spin quadrupolar orders. Employing an SO(6) Majorana fermion representation of spin-3/2s, we find an exact representation of the conserved plaquette fluxes in terms of static Z$_2$ gauge fields akin to the S=1/2 KHM which enables us to treat the remaining interacting matter fermion sector in a parton mean-field theory. The latter provides an explanation for the extensive near degeneracy of low energy states in the gapless phase via the appearance of almost flat Majorana bands close to zero energy. Our parton description is in remarkable quantitative agreement with numerical simulations using the density matrix renormalization group method, and is furthermore corroborated by the addition of a single ion anisotropy which continuously connects the gapless Dirac QSL of our model with that of the S=1/2 KHM. We discuss the implications of our findings for materials realization of higher S=3/2 KHMs and the stability of the QSL phase with respect to additional interactions.
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