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We report magnetization, heat capacity, thermal expansion, and magnetostriction measurements down to millikelvin temperatures on the triangular antiferromagnet YbMgGaO$_4$. Our data exclude the formation of the distinct $frac13$ plateau phase observe d in other triangular antiferromagnets, but reveal plateaulike features in second derivatives of the free energy, magnetic susceptibility and specific heat, at $mu_0H$ = 1.0 - 2.5 T for $Hparallel{}c$ and 2 - 5 T for $Hperp{}c$. Using Monte-Carlo simulations of a realistic spin Hamiltonian, we ascribe these features to nonmonotonic changes in the magnetization and the $frac12$ plateau that is smeared out by the random distribution of exchange couplings in YbMgGaO$_4$.
Frustrated quasidoublets without time-reversal symmetry can host highly unconventional magnetic structures with continuously distributed order parameters even in a single-phase crystal. Here, we report the comprehensive thermodynamic and neutron diff raction investigation on the single crystal of TmMgGaO$_4$, which entails non-Kramers Tm$^{3+}$ ions arranged on a geometrically perfect triangular lattice. The crystal electric field (CEF) randomness caused by the site-mixing disorder of the nonmagnetic Mg$^{2+}$ and Ga$^{3+}$ ions, merges two lowest-lying CEF singlets of Tm$^{3+}$ into a ground-state (GS) quasidoublet. Well below $T_c$ $sim$ 0.7 K, a small fraction of the antiferromagnetically coupled Tm$^{3+}$ Ising quasidoublets with small inner gaps condense into two-dimensional (2D) up-up-down magnetic structures with continuously distributed order parameters, and give rise to the emph{columnar} magnetic neutron reflections below $mu_0H_c$ $sim$ 2.6 T, with highly anisotropic correlation lengths, $xi_{ab}$ $geq$ 250$a$ in the triangular plane and $xi_c$ $<$ $c$/12 between the planes. The remaining fraction of the Tm$^{3+}$ ions remain nonmagnetic at 0 T and become uniformly polarized by the applied longitudinal field at low temperatures. We argue that the similar model can be generally applied to other compounds of non-Kramers rare-earth ions with correlated GS quasidoublets.
DC-magnetization data measured down to 40 mK speak against conventional freezing and reinstate YbMgGaO$_4$ as a triangular spin-liquid candidate. Magnetic susceptibility measured parallel and perpendicular to the $c$-axis reaches constant values belo w 0.1 and 0.2 K, respectively, thus indicating the presence of gapless low-energy spin excitations. We elucidate their nature in the triple-axis inelastic neutron scattering experiment that pinpoints the low-energy ($E$ $leq$ $J_0$ $sim$ 0.2 meV) part of the excitation continuum present at low temperatures ($T$ $<$ $J_0$/$k_B$), but emph{completely} disappearing upon warming the system above $T$ $gg$ $J_0$/$k_B$. In contrast to the high-energy part at $E$ $>$ $J_0$ that is rooted in the breaking of nearest-neighbor valence bonds and persists to temperatures well above $J_0$/$k_B$, the low-energy one originates from the rearrangement of the valence bonds and thus from the propagation of unpaired spins. We further extend this picture to herbertsmithite, the spin-liquid candidate on the kagome lattice, and argue that such a hierarchy of magnetic excitations may be a universal feature of quantum spin liquids.
We present the structural characterization and low-temperature magnetism of the triangular-lattice delafossite NaYbO$_2$. Synchrotron x-ray diffraction and neutron scattering exclude both structural disorder and crystal-electric-field randomness, whe reas heat-capacity measurements and muon spectroscopy reveal the absence of magnetic order and persistent spin dynamics down to at least 70,mK. Continuous magnetic excitations with the low-energy spectral weight accumulating at the $K$-point of the Brillouin zone indicate the formation of a novel spin-liquid phase in a triangular antiferromagnet. This phase is gapless and shows a non-trivial evolution of the low-temperature specific heat. Our work demonstrates that NaYbO$_2$ practically gives the most direct experimental access to the spin-liquid physics of triangular antiferromagnets.
Frustrated Ising magnets host exotic excitations, such as magnetic monopoles in spin ice. The ground state (GS) in this case is characterized by an extensive degeneracy and associated residual entropy going back to the pioneering work by G. Wannier w ho established large residual entropy of nearly 50%Rln2 per mole spins in a triangular Ising antiferromagnet (TIAF) already in 1950. Here, we endeavor to verify this result experimentally using TmMgGaO4, a novel rare-earth-based frustrated antiferromagnet with Ising spins arranged on a perfect triangular lattice. Contrary to theoretical expectations, we find almost no residual entropy and ascribe this result to the presence of a weak second-neighbor coupling J2zz ~ 0.09J1zz that lifts the GS degeneracy and gives rise to several ordered states, the stripe order, 1/3-plateau, and 1/2-plateau. TmMgGaO4 gives experimental access to these novel phases of Ising spins on the triangular lattice.
We report a single-crystal study on the magnetism of the rare-earth compound PrTiNbO$_6$ that experimentally realizes the zigzag pseudospin-$frac{1}{2}$ quantum antiferromagnetic chain model. Random crystal electric field caused by the site mixing be tween non-magnetic Ti$^{4+}$ and Nb$^{5+}$, results in the non-Kramers ground state quasi-doublet of Pr$^{3+}$ with the effective pseudospin-$frac{1}{2}$ Ising moment. Despite the antiferromagnetic intersite coupling of about 4 K, no magnetic freezing is detected down to 0.1 K, whilst the system approaches its ground state with almost zero residual spin entropy. At low temperatures, a sizable gap of about 1 K is observed in zero field. We ascribe this gap to off-diagonal anisotropy terms in the pseudospin Hamiltonian, and argue that rare-earth oxides open an interesting venue for studying magnetism of quantum spin chains.
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