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106 - H. Guo , L. Zhao , M. Baenitz 2021
Despite the absence of an apparent triangular pattern in the crystal structure, we observe unusually well pronounced 1/3 magnetization plateaus in the quasi one-dimensional Ising spin chain compound CoGeO$_3$ which belongs to the class of pyroxene mi nerals. We succeeded in uncovering the detailed microscopic spin structure of the 1/3 magnetization plateau phase by means of neutron diffraction. We observed changes of the initial antiferromagnetic zero-field spin structure that are resembling a regular formation of antiferromagnetic domain wall boundaries, resulting in a kind of modulated magnetic structure with 1/3-integer propagation vector. The net ferromagnetic moment emerges at these domain walls whereas two third of all antiferromagnetic chain alignments can be still preserved. We propose a microscopic model on the basis of an anisotropic frustrated square lattice to explain the observations.
Our studies evidence an anisotropic magnetic order below $T_N = 32$~K. Susceptibility data in small fields of about 1~T reveal an antiferromagnetic (AFM) order for $H perp c$, whereas for $H parallel c$ the data are reminiscent of a field-induced fer romagnetic (FM) structure. At low temperatures and for $H perp c$, the field-dependent magnetization and AC susceptibility data evidence a metamagnetic transition at $H^+ = 5$~T, which is absent for $H parallel c$. We assign this to a transition from a planar cycloidal spin structure at low fields to a planar fan-like arrangement above $H^+$. A fully FM polarized state is obtained above the saturation field of $H_{perp S} = 23.7$~T at 2~K with a magnetization of $M_s = 2.8$~$mu_{rm B}{rm /Cr}$. For $H parallel c$, $M(H)$ monotonously increases and saturates at the same $M_s$ value at $H_{parallel S} = 25.1$~T at 4.2~K. Above $T_N $, the magnetic susceptibility and specific heat indicate signatures of two dimensional (2D) frustration related to the presence of planar ferromagnetic and antiferromagnetic exchange interactions. We found a pronounced nearly isotropic maximum in both properties at about $T^* = 45$~K, which is a clear fingerprint of short-range correlations and emergent spin fluctuations. Calculations based on a planar 2D Heisenberg model support our experimental findings and suggest a predominant FM exchange among nearest and AFM exchange among third-nearest neighbors. Only a minor contribution might be assigned to the antisymmetric Dzyaloshinskii-Moriya interaction possible related to the non-centrosymmetric polar space group $R3m$. Due to these competing interactions, the magnetism in AgCrSe$_{2}$, in contrast to the oxygen based delafossites, can be tuned by relatively small, experimentally accessible, magnetic fields, allowing us to establish the complete anisotropic magnetic $H-T$ phase diagram in detail.
Thermodynamic properties, $^{31}$P nuclear magnetic resonance (NMR) measurements, and density-functional band-structure calculations for $varepsilon$-LiVOPO$_4$ are reported. This quantum magnet features a singlet ground state and comprises two types of alternating spin-$frac12$ chains that manifest themselves by the double maxima in the susceptibility and magnetic specific heat, and by the two-step magnetization process with an intermediate $frac12$-plateau. From thermodynamic data and band-structure calculations, we estimate the leading couplings of $J_1simeq 20$ K and $J_2simeq 60$ K and the alternation ratios of $alpha_1=J_1/J_1simeq 0.6$ and $alpha_2=J_2/J_2simeq 0.3$ within the two chains, respectively. The zero-field spin gap $Delta_0/k_{rm B}simeq 7.3$ K probed by thermodynamic and NMR measurements is caused by the $J_1$-$J_1$ spin chains and can be closed in the applied field of $mu_{0}H_{rm c1}simeq 5.6$ T, giving rise to a field-induced long-range order. The NMR data reveal predominant three-dimensional spin-spin correlations at low temperatures. Field-induced magnetic ordering transition observed above $H_{c1}$ is attributed to the Bose-Einstein condensation of triplons in the sublattice formed by the $J_1$-$J_1$ chains with weaker exchange couplings.
Platelike high-quality NaYbS$_{2}$ rhombohedral single crystals with lateral dimensions of a few mm have been grown and investigated in great detail by bulk methods like magnetization and specific heat, but also by local probes like nuclear magnetic resonance (NMR), electron-spin resonance (ESR), muon-spin relaxation ($mu$SR), and inelastic neutron scattering (INS) over a wide field and temperature range. Our single-crystal studies clearly evidence a strongly anisotropic quasi-2D magnetism and an emerging spin-orbit entangled $S=1/2$ state of Yb towards low temperatures together with an absence of long-range magnetic order down to 260~mK. In particular, the clear and narrow Yb ESR lines together with narrow $^{23}$Na NMR lines evidence an absence of inherent structural distortions in the system, which is in strong contrast to the related spin-liquid candidate YbMgGaO$_{4}$ falling within the same space group $Roverline{3}m$. This identifies NaYbS$_{2}$ as a rather pure spin-1/2 triangular lattice magnet and a new putative quantum spin liquid.
We report on magnetic susceptibility and specific heat measurements of the cubic helimagnet FeGe in external magnetic fields and temperatures near the onset of long-range magnetic order at T_C=278.2(3)K. Pronounced anomalies in the field-dependent ch i_ac(H) data as well as in the corresponding imaginary part chi_ac(H) reveal a precursor region around T_C in the magnetic phase diagram. The occurrence of a maximum at T_0=279.6K in the zero-field specific heat data indicates a second order transition into a magnetically ordered state. A shoulder evolves above this maximum as a magnetic field is applied. The field dependence of both features coincides with crossover lines from the field-polarized to the paramagnetic state deduced from chi_ac(T) at constant magnetic fields. The experimental findings are analyzed within the standard Dzyaloshinskii theory for cubic helimagnets. The remarkable multiplicity of modulated precursor states and the complexity of the magnetic phase diagram near the magnetic ordering are explained by the change of the character of solitonic inter-core interactions and the onset of specific confined chiral modulations in this area.
The ground state properties of CeFePO, a homologue of the new high temperature superconductors RFePnO(1-x)Fx, were studied by means of susceptibility, specific heat, resistivity, and NMR measurements on polycrystals. All the results demonstrate that this compound is a magnetically non-ordered heavy Fermion metal with a Kondo temperature TK~10K, a Sommerfeld coefficient gamma=700mJ/molK2 and a mass enhancement factor of the order of 200. The absence of a Fe-contribution to the effective moment at high temperatures indicates that the magnetism in CeFePO is completely dominated by the effect of Ce. Thus the strong electronic correlation effects originate from the Ce-4f electrons rather than from the Fe-3d electrons. An enhanced Sommerfeld-Wilson ratio R=5.5 as well as a Korringa product S0/T1TK2~0.065 well below 1 indicate the presence of ferromagnetic correlations. Therefore, CeFePO appears to be on the non-magnetic side of a ferromagnetic instability.
CuSiO_3, isotypic to the spin - Peierls compound CuGeO_3, was discovered recently as a metastable decomposition product of the silicate mineral dioptase, Cu_6Si_6O_{18}cdot6H_2O. We investigated the physical properties of CuSiO_3 using susceptibility , magnetization and specific heat measurements on powder samples. The magnetic susceptibility chi(T) is reproduced very well above T = 8 K by theoretical calculations for an S=1/2 antiferromagnetic Heisenberg linear chain without frustration (alpha = 0) and a nearest - neighbor exchange coupling constant of J/k_{B} = 21 K, much weaker than in CuGeO_3. Below 8 K the susceptibility exhibits a substantial drop. This feature is identified as a second - order phase transition at T_{0} = 7.9 K by specific heat measurements. The influence of magnetic fields on T_{0} is weak, and ac - magnetization measurements give strong evidence for a spin - flop - phase at mu_0H_{SF} ~ 3 T. The origin of the magnetic phase transition at T_{0} = 7.9 K is discussed in the context of long - range antiferromagnetic order (AF) versus spin - Peierls(SP)order. Susceptibility and specific heat results support the AF ordered ground state. Additional temperature dependent ^{63,65}Cu nuclear quadrupole resonance experiments have been carried out to probe the Cu^{2+} electronic state and the spin dynamics in CuSiO_3.
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