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Register a new user$^{133}$Cs NMR investigation of 2D frustrated Heisenberg antiferromagnet, Cs$_2$CuCl$_4$
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We report $^{133}$Cs nuclear magnetic resonance (NMR) measurements on the 2D frustrated Heisenberg antiferromagnet Cs$_2$CuCl$_4$ down to 2 K and up to 15 T. We show that $^{133}$Cs NMR is a good probe of the magnetic degrees of freedom in this material. Cu spin degrees of freedom are sensed through a strong anisotropic hyperfine coupling. The spin excitation gap opens above the critical saturation field. The gap value was determined from the activation energy of the nuclear spin-lattice relaxation rate in a magnetic field applied parallel to the Cu chains (b axis). The values of the g-factor and the saturation field are consistent with the neutron-scattering and magnetization results. The measurements of the spin-spin relaxation time are exploited to show that no structural changes occur down to the lowest temperatures investigated.
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We report nuclear magnetic resonance measurements of the spin-1/2 anisotropic triangular lattice antiferromagnet Cs$_2$CuCl$_4$ as a function of temperature and applied magnetic field. The observed temperature and magnetic field dependence of the NMR relaxation rate suggests that low energy excitations in the short-range ordered region stabilized over a wide range of intermediate fields and temperatures of the phase diagram are gapless or nearly gapless fermionic excitations. An upper bound on the size of the gap of 0.037 meV $approx J/10$ is established. The magnetization and NMR relaxation rate can be qualitatively described either by a quasi-1D picture of weakly coupled chains, or by mean-field theories of specific 2D spin liquids; however, quantitative differences exist between data and theory in both cases. This comparison indicates that 2D interactions are quantitatively important in describing the low-energy physics.
We investigate the electronic and magnetic properties of the frustrated triangular-lattice antiferromagnets Cs$_2$CuCl$_4$ and Cs$_2$CuBr$_4$ in the framework of density functional theory. Analysis of the exchange couplings J and J using the available X-ray structural data corroborates the values obtained from experimental results for Cs$_2$CuBr$_4$ but not for Cs$_2$CuCl$_4$. In order to understand this discrepancy, we perform a detailed study of the effect of structural optimization on the exchange couplings of Cs$_2$CuCl$_4$ employing different exchange-correlation functionals. We find that the exchange couplings depend on rather subtle details of the structural optimization and that only when the insulating state (mediated through spin polarization) is present in the structural optimization, we do have good agreement between the calculated and the experimentally determined exchange couplings. Finally, we discuss the effect of interlayer couplings as well as longer-ranged couplings in both systems.
We have found an unusual competition of two frustration mechanisms in the 2D quantum antiferromagnet Cs$_2$CoBr$_4$. The key actors are the alternation of single-ion planar anisotropy direction of the individual magnetic Co$^{2+}$ ions, and their arrangement in a distorted triangular lattice structure. In particular, the uniquely oriented Ising-type anisotropy emerges from the competition of easy-plane ones, and for a magnetic field applied along this axis one finds a cascade of five ordered phases at low temperatures. Two of these phases feature magnetization plateaux. The low-field one is supposed to be a consequence of a collinear ground state stabilized by the anisotropy, while the other plateau bears characteristics of an up-up-down state exclusive for lattices with triangular exchange patterns. Such coexistence of the magnetization plateaux is a fingerprint of competition between the anisotropy and the geometric frustration in Cs$_2$CoBr$_4$.
Quantum triangular-lattice antiferromagnets are important prototype systems to investigate phenomena of the geometrical frustration in condensed matter. Apart from highly unusual magnetic properties, they possess a rich phase diagram (ranging from an unfrustrated square lattice to a quantum spin liquid), yet to be confirmed experimentally. One major obstacle in this area of research is the lack of materials with appropriate (ideally tuned) magnetic parameters. Using Cs$_2$CuCl$_4$ as a model system, we demonstrate an alternative approach, where, instead of the chemical composition, the spin Hamiltonian is altered by hydrostatic pressure. The approach combines high-pressure electron spin resonance and magnetization measurements, allowing us not only to quasi-continuously tune the exchange parameters, but also to accurately monitor them. Our experiments indicate a substantial increase of the exchange coupling ratio from 0.3 to 0.42 at a pressure of 1.8 GPa, revealing a number of emergent field-induced phases.
We report on low-temperature heat-transport properties of the spin-1/2 triangular-lattice antiferromagnet Cs$_2$CuCl$_4$. Broad maxima in the thermal conductivity along the three principal axes, observed at about 5 K, are interpreted in terms of the Debye model, including the phonon Umklapp scattering. For thermal transport along the $b$ axis, we observed a pronounced field-dependent anomaly, close to the transition into the three-dimensional long-range-ordered state. No such anomalies were found for the transport along the $a$ and $c$ directions. We argue that this anisotropic behavior is related to an additional heat-transport channel through magnetic excitations, that can best propagate along the direction of the largest exchange interaction. Besides, peculiarities of the heat transport of Cs$_2$CuCl$_4$ in magnetic fields up to the saturation field and above are discussed.
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