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Register a new userIncommensurate atomic and magnetic modulations in the spin-frustrated {beta}-NaMnO2 triangular lattice
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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.
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We report thermodynamic properties, magnetic ground state, and microscopic magnetic model of the spin-1 frustrated antiferromaget Li$_{2}$NiW$_{2}$O$_{8}$ showing successive transitions at $T_{rm N1}simeq 18$ K and $T_{rm N2}simeq 12.5$ K in zero field. Nuclear magnetic resonance and neutron diffraction reveal collinear and commensurate magnetic order with the propagation vector $mathbf k=(frac12,0,frac12)$ below $T_{rm N2}$. The ordered moment of 1.8 $mu_B$ at 1.5 K is directed along $[0.89(9),-0.10(5),-0.49(6)]$ and matches the magnetic easy axis of spin-1 Ni$^{2+}$ ions, which is determined by the scissor-like distortion of the NiO$_6$ octahedra. Incommensurate magnetic order, presumably of spin-density-wave type, is observed in the region between $T_{rm N2}$ and $T_{rm N1}$. Density-functional band-structure calculations put forward a three-dimensional spin lattice with spin-1 chains running along the $[01bar 1]$ direction and stacked on a spatially anisotropic triangular lattice in the $ab$ plane. We show that the collinear magnetic order in Li$_2$NiW$_2$O$_8$ is incompatible with the triangular lattice geometry and thus driven by a pronounced easy-axis single-ion anisotropy of Ni$^{2+}$.
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.
The S=2 anisotropic triangular lattice alpha-NaMnO2 is studied by neutron inelastic scattering. Antiferromagnetic order occurs at T ~ 45 K with opening of a spin gap. The spectral weight of the magnetic dynamics above the gap (Delta ~ 7.5 meV) has been analysed by the single-mode approximation. Excellent agreement with the experiment is achieved when a dominant exchange interaction (|J|/k_B ~ 73 K), along the monoclinic b-axis and a sizeable easy-axis magnetic anisotropy (|D|/k_B ~ 3 K) are considered. Despite earlier suggestions for two-dimensional spin interactions, the dynamics illustrate strongly coupled antiferromagnetic S=2 chains and cancellation of the interchain exchange due to the lattice topology. alpha-NaMnO2 therefore represents a model system where the geometric frustration is resolved through the lowering of the dimensionality of the spin interactions.
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.
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.
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