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Register a new userImpact of the lattice on magnetic properties and possible spin nematicity in the S=1 triangular antiferromagnet NiGa$_2$S$_4$
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NiGa$_2$S$_4$ is a triangular lattice S=1 system with strong two-dimensionality of the lattice, actively discussed as a candidate to host spin-nematic order brought about by strong quadrupole coupling. Using Raman scattering spectroscopy we identify a phonon of E$_g$ symmetry which can modulate magnetic exchange $J_1$ and produce quadrupole coupling. Additionally, our Raman scattering results demonstrate a loss of local inversion symmetry on cooling, which we associate with sulfur vacancies. This will lead to disordered Dzyaloshinskii-Moriya interactions, which can prevent long range magnetic order. Using magnetic Raman scattering response we identify 160~K as a temperature of an upturn of magnetic correlations. The temperature below 160~K, but above 50~K where antiferromagnetic magnetic start to increase, is a candidate for spin-nematic regime.
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The crystal structure and magnetic correlations in triangular antiferromagnet FeGa$_2$S$_4$ are studied by x-ray diffraction, magnetic susceptibility, neutron diffraction and neutron inelastic scattering. We report significant mixing at the cation sites and disentangle magnetic properties dominated by major and minor magnetic sites. The magnetic short-range correlations at 0.77 AA$^{-1}$ correspond to the major sites and being static at base temperature they evolve into dynamic correlations around 30 - 50 K. The minor sites contribute to the magnetic peak at 0.6 AA$^{-1}$, which vanishes at 5.5 K. Our analytical studies of triangular lattice models with bilinear and biquadratic terms provide the ratios between exchanges for the proposed ordering vectors. The modelling of the inelastic neutron spectrum within linear spin wave theory results in the set of exchange couplings $J_1=1.7$,meV, $J_2=0.9$,meV, $J_3=0.8$,meV for the bilinear Heisenberg Hamiltonian. However, not all features of the excitation spectrum are explained with this model.
Nonmagnetic impurity effects of the spin disordered state in the triangular antiferromagnet NiGa$_2$S$_4$ was studied through magnetic and thermal measurements for Ni$_{1-x}$Zn$_x$Ga$_2$S$_4$ (0.0le xle 0.3). Only 1 % substitution is enough to strongly suppress the coherence observed in the spin disordered state. However, the suppression is not complete and the robust feature of the T^2 dependent specific heat and its scaling behavior with the Weiss temperature indicate the existence of a coherent Nambu-Goldstone mode. Absence of either conventional magnetic order or bulk spin freezing suggests a novel symmetry breaking of the ground state.
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.
Recently, several putative quantum spin liquid (QSL) states were discovered in ${tilde S} = 1/2$ rare-earth based triangular-lattice antiferromagnets (TLAF) with the delafossite structure. A way to clarify the origin of the QSL state in these systems is to identify ways to tune them from the putative QSL state towards long-range magnetic order. Here, we introduce the Ce-based TLAF KCeS$_2$ and show via low-temperature specific heat and $mu$SR investigations that it yields magnetic order below $T_{mathrm N} = 0.38$ K despite the same delafossite structure. We identify a well separated ${tilde S} = 1/2$ ground state for KCeS$_2$ from inelastic neutron scattering and embedded-cluster quantum chemical calculations. Magnetization and electron spin resonance measurements on single crystals indicate a strong easy-plane $g$~factor anisotropy, in agreement with the ab initio calculations. Finally, our specific-heat studies reveal an in-plane anisotropy of the magnetic field-temperature phase diagram which may indicate anisotropic magnetic interactions in KCeS$_2$.
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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