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Register a new userMagneto-structural properties of the layered quasi-2D triangular-lattice antiferromagnets Cs$_2$CuCl$_{4-x}$Br$_x$ for ${x}$ = 0,1,2 and 4
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We present a study of the magnetic susceptibility $chi_{mol}$ under variable hydrostatic pressure on single crystals of Cs$_2$CuCl$_{4-x}$Br$_x$. This includes the border compounds textit{x} = 0 and 4, known as good realizations of the distorted triangular-lattice spin-1/2 Heisenberg antiferromagnet, as well as the isostructural stoichiometric systems Cs$_2$CuCl$_{3}$Br$_1$ and Cs$_2$CuCl$_{2}$Br$_2$. For the determination of the exchange coupling constants $J$ and $J^{prime}$, $chi_{mol}$ data were fitted by a $J-J^{prime}$ model cite{Schmidt2015}. Its application, validated for the border compounds, yields a degree of frustration $J^{prime}$/$J$ = 0.47 for Cs$_2$CuCl$_3$Br$_1$ and $J^{prime}$/$J$ $simeq$ 0.63 - 0.78 for Cs$_2$CuCl$_2$Br$_2$, making these systems particular interesting representatives of this family. From the evolution of the magnetic susceptibility under pressure up to about 0.4,GPa, the maximum pressure applied, two observations were made for all the compounds investigated here. First, we find that the overall energy scale, given by $J_c = (J^2$ + $J^{prime 2}$)$^{1/2}$, increases under pressure, whereas the ratio $J^{prime}$/$J$ remains unchanged in this pressure range. These experimental observations are in accordance with the results of DFT calculations performed for these materials. Secondly, for the magnetoelastic coupling constants, extraordinarily small values are obtained. We assign these observations to a structural peculiarity of this class of materials.
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The quantum-spin S = 1=2 chain system Cs$_2$CuCl$_4$ is of high interest due to competing anti-ferromagnetic intra-chain J and inter-chain exchange J interactions and represents a paramount example for Bose-Einstein condensation of magnons [R. Coldea et al., Phys. Rev. Lett. 88, 137202 (2002)]. Substitution of chlorine by bromine allows tuning the competing exchange interactions and corresponding magnetic frustration. Here we report on electron spin resonance (ESR) in single crystals of Cs$_2$CuCl$_{4-x}$Br$_x$ with the aim to analyze the evolution of anisotropic exchange contributions. The main source of the ESR linewidth is attributed to the uniform Dzyaloshinskii-Moriya interaction. The vector components of the Dzyaloshinskii-Moriya interaction are determined from the angular dependence of the ESR spectra using a high-temperature approximation. The obtained results support the site selectivity of the Br substitution suggested from the evolution of lattice parameters and magnetic susceptibility dependent on the Br concentration.
We report an experimental and theoretical study of the low-temperature specific heat $C$ and magnetic susceptibility $chi$ of the layered anisotropic triangular-lattice spin-1/2 Heisenberg antiferromagnets Cs$_2$CuCl$_{4-x}$Br$_x$ with $x$ = 0, 1, 2, and 4. We find that the ratio $J/J$ of the exchange couplings ranges from 0.32 to $approx 0.78$, implying a change (crossover or quantum phase transition) in the materials magnetic properties from one-dimensional (1D) behavior for $J/J < 0.6$ to two-dimensional (2D) behavior for $J/J approx 0.78$ behavior. For $J/J < 0.6$, realized for $x$ = 0, 1, and 4, we find a magnetic contribution to the low-temperature specific heat, $C_{rm m} propto T$, consistent with spinon excitations in 1D spin-1/2 Heisenberg antiferromagnets. Remarkably, for $x$ = 2, where $J/J approx 0.78$ implies a 2D magnatic character, we also observe $C_{rm m} propto T$. This finding, which contrasts the prediction of $C_{rm m} propto T^2$ made by standard spin-wave theories, shows that Fermi-like statistics also plays a significant role for the magnetic excitations in frustrated spin-1/2 2D antiferromagnets.
We report on a systematic study of the magnetic properties on single crystals of the solid solution Cs$_2$CuCl$_{4-x}$Br$_x$ (0 $leq$ x $leq$ 4), which include the two known end-member compounds Cs$_2$CuCl$_4$ and Cs$_2$CuBr$_4$, classified as quasi-two-dimensional quantum antiferromagnets with different degrees of magnetic frustration. By comparative measurements of the magnetic susceptibility $chi$($T$) on as many as eighteen different Br concentrations, we found that the inplane and out-of-plane magnetic correlations, probed by the position and height of a maximum in the magnetic susceptibility, respectively, do not show a smooth variation with x. Instead three distinct concentration regimes can be identified, which are separated by critical concentrations x$_{c1}$ = 1 and x$_{c2}$ = 2. This unusual magnetic behavior can be explained by considering the structural peculiarities of the materials, especially the distorted Cu-halide tetrahedra, which support a site-selective replacement of Cl- by Br- ions. Consequently, the critical concentrations x$_{c1}$ (x$_{c2}$) mark particularly interesting systems, where one (two) halidesublattice positions are fully occupied.
Powder X-ray diffraction (PXRD) and single-crystal neutron scattering were used to study in detail the structural properties of the Cs2CuCl(4-x)Br(x) series, good realizations of layered triangular antiferromagnets. Detailed temperature-dependent PXRD reveal a pronounced anisotropy of the thermal expansion for the three different crystal directions of the orthorhombic structure without any structural phase transition down to 20 K. Remarkably, the anisotropy of the thermal expansion varies for different $x$, leading to distinct changes of the geometry of the local Cu environment as a function of temperature and composition. The refinement of the atomic positions confirms that for x=1 and 2, the Br atoms occupy distinct halogen sites in the [CuX4]-tetrahedra (X = Cl, Br). The precise structure data are used to calculate the magnetic exchange couplings using density functional methods for x=0. We observe a pronounced temperature dependence of the calculated magnetic exchange couplings, reflected in the strong sensitivity of the magnetic exchange couplings on structural details. These calculations are in good agreement with the experimentally established values for Cs2CuCl4 if one takes the low-temperature structure data as a starting point.
The magnetism in the saw-tooth lattice of Mn in the olivine chalcogenides, Mn$_2$SiS$_{4-x}$Se$_x$ ($x$ = 1$textendash$4) is studied in detail by analyzing their magnetization, specific heat and thermal conductivity properties and complemented with density functional theory calculations. The air-stable chalcogenides are antiferromagnets and show a linear trend in the transition temperature, $T_N$ as a function of Se-content ($x$) which shows a decrease from $T_N approx$ 86~K for {mss} to 66~K for {msse}. Additional new magnetic anomalies are revealed at low temperatures for all the compositions. Magnetization irreversibilities are also observed as a function of $x$. The specific heat and the magnetic entropy indicate the presence of short-range spin fluctuations in Mn$_2$SiS$_{4-x}$Se$_x$. A spin-flop antiferromagnetic phase transition in the presence of applied magnetic field is present in Mn$_2$SiS$_{4-x}$Se$_x$, where the critical field for the spin flop increases from $x$ = 0 towards 4 in a non-linear fashion. Density functional theory calculations show that an overall antiferromagnetic structure with ferromagnetic coupling of the spins in the $ab$-plane minimizes the total energy. The band structures calculated for mss and msse reveal features near the band edges similar to those reported for Fe-based olivines suggested as thermoelectrics; however the experimentally determined thermal transport data do not support superior thermoelectric features. The transition from long-range magnetic order in mss to short-range order and spin fluctuations in msse is explained using the variation of the Mn-Mn distances in the triangle units that constitutes the saw-tooth lattice upon progressive replacement of sulphur with selenium.
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