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N. Matsubara

Publications and source records attributed to N. Matsubara.

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The Duel of Magnetic Interactions & Structural Instabilities: Itinerant Frustration in the Triangular Lattice Compound LiCrSe$_2$

The recent synthesis of the chromium selenide compound LiCrSe$_2$ constitutes a valuable addition to the ensemble of two-dimensional triangular lattice antiferromagnets (2D-TLA). In this work we present the very first comprehensive study of the combined low temperature nuclear and magnetic structure established in this material. Details on the connection between Li-ion dynamics and structural changes are also presented along with a direct link between atomic structure and spin order via a strong magnetoelastic coupling. LiCrSe$_2$ was found to undergo a first order structural transition from a trigonal crystal system with space group $P\bar{3}m1$ to a monoclinic one with space group $C2/m$ at $T_{\rm s}=30$~K. Such restructuring of the lattice is accompanied by a magnetic transition at $T_{\rm N}=30$~K, with the formation of a complex spin arrangement for the Cr$^{3+}$ moments. Refinement of the magnetic structure with neutron diffraction data and complementary muon spin rotation analysis reveal the presence of two incommensurate magnetic domains with a up-up-down-down arrangement of the spins with ferromagnetic (FM) double chains coupled antiferromagnetically (AFM). In addition to this unusual arrangement, the spin axial vector is modulated both in direction and modulus, resulting in a spin density wave-like order with periodic suppression of the Cr moment along the chains. This behavior is believed to appear as a result of strong competition between direct exchange AFM and superexchange FM couplings established between both nearest neighbor and next nearest neighbor Cr$^{3+}$ ions. We finally conjecture that the resulting magnetic order is stabilized via subtle vacancy/charge order within the Li layers, potentially causing a mix of two different magnetic phases within the sample.

cond-mat.str-el

Nuclear and magnetic spin structure of the antiferromagnetic triangular lattice compound LiCrTe$_2$ investigated by $μ^+$SR as well as neutron and X-ray diffraction

Two$-$dimensional (2D) triangular lattices antiferromagnets (2D$-$TLA) often manifest intriguing physical and technological properties, due to the strong interplay between lattice geometry and electronic properties. The recently synthesized 2$-$dimensional transition metal dichalcogenide LiCrTe$_2$, being a 2D$-$TLA, enriched the range of materials which can present such properties. In this work, muon spin rotation ($μ^+$SR) and neutron powder diffraction (NPD) have been utilized to reveal the true magnetic nature and ground state of LiCrTe$_2$. From high$-$resolution NPD the magnetic spin order at base$-$temperature is not, as previously suggested, helical, but rather collinear antiferromagnetic (AFM) with ferromagnetic (FM) spin coupling within the $ab-$plane and AFM coupling along the $c-$axis. The ordered magnetic Cr moment is established as $μ_{\rm Cr}=$ 2.36 $μ_{\rm B}$. From detailed $μ^+$SR measurements we observe an AFM ordering temperature $T_{\rm N}\approx$ 125 K. This value is remarkably higher than the one previously reported by magnetic bulk measurements. From $μ^+$SR we are able to extract the magnetic order parameter, whose critical exponent allows us to categorize LiCrTe$_2$ in the 3D Heisenberg AFM universality class. Finally, by combining our magnetic studies with high$-$resolution synchrotron X$-$ray diffraction (XRD), we find a clear coupling between the nuclear and magnetic spin lattices. This suggests the possibility for a strong magnon$-$phonon coupling, similar to what has been previously observed in the closely related compound LiCrO$_2$.

cond-mat.str-el

Neutron powder diffraction study of NaMn$_2$O$_4$ and Li$_{0.92}$Mn$_2$O$_4$: New insights on spin-charge-orbital ordering

The high-pressure synthesized quasi-one-dimensional compounds NaMn$_2$O$_4$ and Li$_{0.92}$Mn$_2$O$_4$ are both antiferromagnetic insulators, and here their atomic and magnetic structures were investigated using neutron powder diffraction. The present crystal structural analyses of NaMn2O4 reveal that Mn3+/Mn4+ charge-ordering state exist even at low temperature (down to 1.5 K). It is evident from one of the Mn sites shows a strongly distorted Mn3+ octahedra due to the Jahn-Teller effect. Above TN = 39 K, a two-dimensional short-range correlation is observed, as indicated by an asymmetric diffuse scattering. Below TN, two antiferromagnetic transitions are observed (i) a commensurate long-range Mn3+ spin ordering below 39 K, and (ii) an incommensurate Mn4+ spin ordering below 10 K. The commensurate magnetic structure (kC = 0.5, -0.5, 0.5) follows the magnetic anisotropy of the local easy axes of Mn3+, while the incommensurate one shows a spin-density-wave order with kIC = (0,0,0.216). For Li$_{0.92}$Mn$_2$O$_4$, on the other hand, absence of a long-range spin ordered state down to 1.5 K is confirmed.

cond-mat.mtrl-sci

Magnetism and Ion Diffusion in Honeycomb Layered Oxide K$_2$Ni$_2$TeO$_6$: First Time Study by Muon Spin Rotation & Neutron Scattering

In the quest of finding novel and efficient batteries, a great interest has raised in K-based honeycomb layer oxide materials both for their fundamental properties and potential applications. A key issue in the realization of efficient batteries based on such compounds, is to understand the K-ion diffusion mechanism. However, investigation of potassium-ion (K$^+$) dynamics in materials using magneto-spin properties has so far been challenging, due to its inherently weak nuclear magnetic moment, in contrast to other alkali ions such as lithium and sodium. Spin-polarised muons, having a high gyromagnetic ratio, make the muon spin rotation and relaxation ($μ$+SR) technique ideal for probing ions dynamics in weak magneto-spin moment materials. Here we report the magnetic properties and K+ dynamics in honeycomb layered oxide material of the K$_2$Ni$_2$TeO$_6$ using $μ$+SR measurements. Our low-temperature $μ$+SR results together with, with complementary magnetic susceptibility, find an antiferromagnetic transition at 26 K. Further $μ$+SR studies performed at higher temperatures reveal that potassium ions (K$^+$) become mobile above 250 K and the activation energy for the diffusion process is Ea = 121(13) meV. This is the first time that K+ dynamics in potassium-based battery materials has been measured using $μ$+SR. Finally our results also indicate an interesting possibility that K-ion self diffusion occurs predominantly at the surface of the powder particles. This opens future possibilities for improving ion diffusion and device performance using nano-structuring.

cond-mat.mtrl-sci