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Register a new userPressure-tuning the quantum spin Hamiltonian of the triangular lattice antiferromagnet Cs$_2$CuCl$_4$
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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.
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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.
We report on high-field electron spin resonance (ESR) studies of magnetic excitations in the spin-1/2 triangular-lattice antiferromagnet Cs$_2$CuBr$_4$. Frequency-field diagrams of ESR excitations are measured for different orientations of magnetic fields up to 25 T. We show that the substantial zero-field energy gap, $Deltaapprox9.5$ K, observed in the low-temperature excitation spectrum of Cs$_2$CuBr$_4$ [Zvyagin $et~al.$, Phys. Rev. Lett. 112, 077206 (2014)], is present well above $T_N$. Noticeably, the transition into the long-range magnetically ordered phase does not significantly affect the size of the gap, suggesting that even below $T_N$ the high-energy spin dynamics in Cs$_2$CuBr$_4$ is determined by short-range-order spin correlations. The experimental data are compared with results of model spin-wave-theory calculations for spin-1/2 triangle-lattice antiferromagnet.
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.
We study the high magnetic field regime of the antiferromagnetic insulator Cs$_2$CuCl$_4$ by expressing the spin-1/2 operators in the relevant Heisenberg model in terms of hard-core bosons and implementing the hard-core constraint via an infinite on-site interaction. We focus on the case where the external magnetic field exceeds the saturation field $B_{c}approx8.5;mathrm{T}$ and is oriented along the crystallographic $a$ axis perpendicular to the lattice plane. Because in this case the excited states are separated by an energy gap from the ground state, we may use the self-consistent ladder approximation to take the strong correlations due to the hard-core constraint into account. In Cs$_2$CuCl$_4$ there are additional interactions besides the hard-core interaction which we treat in self-consistent Hartree-Fock approximation. We calculate the spectral function of the hard-core bosons from which we obtain the in-plane components of the dynamic structure factor, the magnetic susceptibility, and the specific heat. Our results for the specific heat are in good agreement with the available experimental data. We conclude that the self-consistent ladder approximation in combination with a self-consistent Hartree-Fock decoupling of the non-hard-core interactions gives an accurate description of the physical properties of gapped hard-core bosons in two dimensions at finite temperatures.
A layered triangular lattice with spin-1/2 ions is an ideal platform to explore highly entangled exotic states like quantum spin liquid (QSL). Here, we report a systematic in-field neutron scattering study on a perfect two-dimensional triangular-lattice antiferromagnet, CsYbSe$_2$, a member of the large QSL candidate family rare-earth chalcogenides. The elastic neutron scattering measured down to 70 mK shows that there is a short-range 120$^{circ}$ magnetic order at zero field. In the field-induced ordered states, the spin-spin correlation lengths along the $c$ axis are relatively short, although the heat capacity results indicate long-range magnetic orders at 3 T $-$ 5 T. The inelastic neutron scattering spectra evolve from highly damped continuum-like excitations at zero field to relatively sharp spin wave modes at the plateau phase. Our extensive large-cluster density-matrix renormalization group calculations with a Heisenberg triangular-lattice nearest-neighbor antiferromagnetic model reproduce the essential features of the experimental spectra, including continuum-like excitations at zero field, series of sharp magnons at the plateau phase as well as two-magnon excitations at high energy. This work presents comprehensive experimental and theoretical overview of the unconventional field-induced spin dynamics in triangular-lattice Heisenberg antiferromagnet and thus provides valuable insight into quantum many-body phenomena.
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