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Register a new userA Class of Compounds Featuring Frustrated Triangular Magnetic Lattice CsRESe$_2$ (RE=La-Lu): Quantum Spin-Liquid Candidates
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A triangular lattice selenide series of rare earth (RE), CsRESe2, were synthesized as large single crystals using a flux growth method. This series stabilized in either trigonal (R-3m) or hexagonal (P63/mmc) crystal systems. Physical properties of CsRESe2 were explored by magnetic susceptibility and heat capacity measurements down to 0.4 K. Antiferromagnetic interaction was observed in all magnetic compounds, while no long-range magnetic order was found, indicating the frustrated magnetism. CsDySe2 presents spin freezing at 0.7 K, revealing a spin-glass state. CsCeSe2 and CsYbSe2 present broad peaks at 0.7 K and 1.5 K in the magnetization, respectively, suggesting the short-range interactions between magnetic rare earth ions. The lack of signature for long-range magnetic order and spin freezing down to 0.4 K in these compounds (RE = Ce, Yb) implies their candidacy for quantum spin liquid state.
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The layered {beta}-NaMnO2, a promising Na-ion energy-storage material has been investigated for its triangular lattice capability to promote complex magnetic configurations that may release symmetry restrictions for the coexistence of ferroelectric and magnetic orders. The complexity of the neutron powder diffraction patterns underlines that the routinely adopted commensurate structural models are inadequate. Instead, a single-phase superspace symmetry description is necessary, demonstrating that the material crystallizes in a compositionally modulated q= (0.077(1), 0, 0) structure. Here, Mn3+ Jahn-Teller distorted MnO6 octahedra form corrugated layer stacking sequences of the {beta}-NaMnO2 type, which are interrupted by flat sheets of the {alpha}-like oxygen topology. Spontaneous long-range collinear antiferromagnetic order, defined by the propagation vector k= (1/2, 1/2, 1/2), appears below TN1= 200 K. Moreover, a second transition into a spatially modulated proper-screw magnetic state (k+-q) is established at TN2= 95 K, with an antiferromagnetic order parameter resembling that of a two-dimensional (2D) system. The evolution of 23Na NMR spin-lattice relaxation identifies a magnetically inhomogene-ous state in the intermediate T-region (TN2 <T< TN1), while its strong suppression below TN2 indicates that a spin-gap opens in the excitation spectrum. High-resolution neutron inelastic scattering confirms that the magnetic dynamics are indeed gapped ({Delta}~5 meV) in the low-temperature magnetic phase, while simulations on the basis of the single-mode approximation suggest that Mn-spins residing on ad-jacent antiferromagnetic chains, establish sizable 2D correlations. Our analysis points that novel struc-tural degrees of freedom promote, cooperative magnetism and emerging dielectric properties in this non-perovskite-type of manganite.
The triangular lattice compound TlYbS$_2$ was prepared as large single crystals via a molten flux growth technique using sodium chloride. Anisotropic magnetic susceptibility measurements down to 0.4 K indicate a complete absence of long-range magnetic order. Despite this lack of long-range order, short-range antiferromagnetic interactions are evidenced through broad transitions, suggesting frustrated behavior. Variable magnetic field measurements reveal metamagnetic behavior at temperatures less than 2 K. Complex low temperature field-tunable magnetic behavior, in addition to no observable long-range order down to 0.4 K, suggest that TlYbS$_2$ is a frustrated magnet and a possible quantum spin liquid candidate.
Birnessite compounds are stable across a wide range of compositions that produces a remarkable diversity in their physical, electrochemical and functional properties. These are hydrated analogues of the magnetically frustrated, mixed-valent manganese oxide structures, with general formula, NaxMnO2. Here we demonstrate that the direct hydration of layered rock-salt type a-NaMnO2, with the geometrically frustrated triangular lattice topology, yields the birnessite type oxide, Na0.36MnO2 0.2H2O, transforming its magnetic properties. This compound has a much-expanded interlayer spacing compared to its parent a-NaMnO2 compound. We show that while the parent a-NaMnO2 possesses a Neel temperature of 45 K as a result of broken symmetry in the Mn3+ sub-lattice, the hydrated derivative undergoes collective spin-freezing at 29 K within the Mn3+/Mn4+ sub-lattice. Scaling-law analysis of the frequency dispersion of the AC susceptibility, as well as the temperature-dependent, low-field DC magnetization confirm a cooperative spin-glass state of strongly interacting spins. This is supported by complementary spectroscopic analysis (HAADF-STEM, EDS, EELS) as well as by a structural investigation (high-resolution TEM, X-ray and neutron powder diffraction) that yield insights into the chemical and atomic structure modifications. We conclude that the spin-glass state in birnessite is driven by the spin-frustration imposed by the underlying triangular lattice topology that is further enhanced by the in-plane bond-disorder generated by the mixed-valent character of manganese in the layers.
We have grown single crystals of Na$_2$BaNi(PO$_4$)$_2$, a new spin-1 equilateral triangular lattice antiferromagnet (ETLAF), and performed magnetic susceptibility, specific heat and thermal conductivity measurements at ultralow temperatures. The main results are (i) at zero magnetic field, Na$_2$BaNi(PO$_4$)$_2$ exhibits a magnetic ordering at 430 mK with a weak ferromagnetic moment along the $c$ axis. This suggests a canted 120$^circ$ spin structure, which is in a plane including the crystallographic $c$ axis due to the existence of an easy-axis anisotropy and ferromagnetically stacked along the $c$ axis; (ii) with increasing field along the $c$ axis, a 1/3 magnetization plateau is observed which means the canted 120$^circ$ spin structure is transformed to a up up down (UUD) spin structure. With even higher fields, the UUD phase further evolves to possible V and V phases; (iii) with increasing field along the $a$ axis, the canted 120$^circ$ spin structure is possibly transformed to a umbrella phase and a V phase. Therefore, Na$_2$BaNi(PO$_4$)$_2$ is a rare example of spin-1 ETLAF with single crystalline form to exhibit easy-axis spin anisotropy and series of quantum spin state transitions.
We found new two-dimensional (2D) quantum (S=1/2) antiferromagnetic systems: CuRE2Ge2O8 (RE=Y and La). According to our analysis of high-resolution X-ray and neutron diffraction experiments, the Cu-network of CuRE2Ge2O8 (RE=Y and La) exhibits a 2D triangular lattice linked via weak bonds along the perpendicular b-axis. Our bulk characterizations from 0.08 to 400 K show that they undergo a long-range order at 0.51(1) and 1.09(4) K for the Y and La systems, respectively. Interestingly, they also exhibit field induced phase transitions. For theoretical understanding, we carried out the density functional theory (DFT) band calculations to find that they are typical charge-transfer-type insulators with a gap of Eg = 2 eV. Taken together, our observations make CuRE2Ge2O8 (RE=Y and La) additional examples of low-dimensional quantum spin triangular antiferromagnets with the low-temperature magnetic ordering.
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