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Register a new userRare-earth chalcogenides: A large family of triangular lattice spin liquid candidate
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Frustrated quantum magnets are expected to host many exotic quantum spin states like quantum spin liquid (QSL), and have attracted numerous interest in modern condensed matter physics. The discovery of the triangular lattice spin liquid candidate YbMgGaO$_4$ stimulated an increasing attention on the rare-earth-based frustrated magnets with strong spin-orbit coupling. Here we report the synthesis and characterization of a large family of rare-earth chalcogenides AReCh$_2$ (A = alkali or monovalent ions, Re = rare earth, Ch = O, S, Se). The family compounds share the same structure (R$bar{3}$m) as YbMgGaO$_4$, and antiferromagnetically coupled rare-earth ions form perfect triangular layers that are well separated along the $c$-axis. Specific heat and magnetic susceptibility measurements on NaYbO$_2$, NaYbS$_2$ and NaYbSe$_2$ single crystals and polycrystals, reveal no structural or magnetic transition down to 50mK. The family, having the simplest structure and chemical formula among the known QSL candidates, removes the issue on possible exchange disorders in YbMgGaO$_4$. More excitingly, the rich diversity of the family members allows tunable charge gaps, variable exchange coupling, and many other advantages. This makes the family an ideal platform for fundamental research of QSLs and its promising applications.
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YbMgGaO$_{4}$, a structurally perfect two-dimensional triangular lattice with odd number of electrons per unit cell and spin-orbit entangled effective spin-1/2 local moments of Yb$^{3+}$ ions, is likely to experimentally realize the quantum spin liquid ground state. We report the first experimental characterization of single crystal YbMgGaO$_{4}$ samples. Due to the spin-orbit entanglement, the interaction between the neighboring Yb$^{3+}$ moments depends on the bond orientations and is highly anisotropic in the spin space. We carry out the thermodynamic and the electron spin resonance measurements to confirm the anisotropic nature of the spin interaction as well as to quantitatively determine the couplings. Our result is a first step towards the theoretical understanding of the possible quantum spin liquid ground state in this system and sheds new lights on the search of quantum spin liquids in strong spin-orbit coupled insulators.
Spin-orbit coupling is an important ingredient in many spin liquid candidate materials, especially among the rare-earth magnets and Kitaev materials. We explore the rare-earth chalcogenides NaYbS$_2$ where the Yb$^{3+}$ ions form a perfect triangular lattice. Unlike its isostructural counterpart YbMgGaO$_4$ and the kagom{e} lattice herbertsmithite, this material does not have any site disorders both in magnetic and non-magnetic sites. We carried out the thermodynamic and inelastic neutron scattering measurements. The magnetic dynamics could be observed with a broad gapless excitation band up to 1.0 meV at 50 mK and 0 T, no static long-range magnetic ordering is detected down to 50 mK. We discuss the possibility of Dirac spin liquid for NaYbS$_2$. We identify the experimental signatures of field-induced transitions from the disordered spin liquid to an ordered antiferromagnet with an excitation gap at finite magnetic fields and discuss this result with our Monte Carlo calculation of the proposed spin model. Our findings could inspire further interests in the spin-orbit-coupled spin liquids and the magnetic ordering transition from them.
Kitaev spin liquid (KSL) system has attracted tremendous attention in past years because of its fundamental significance in condensed matter physics and promising applications in fault-tolerant topological quantum computation. Material realization of such a system remains a major challenge in the field due to the unusual configuration of anisotropic spin interactions, though great effort has been made before. Here we reveal that rare-earth chalcohalides REChX (RE=rare earth, Ch=O, S, Se, Te, X=F, Cl, Br, I) can serve as a family of KSL candidates. Most family members have the typical SmSI-type structure with a high symmetry of R-3m and rare-earth magnetic ions form an undistorted honeycomb lattice. The strong spin-orbit coupling of 4f electrons intrinsically offers anisotropic spin interactions as required by Kitaev model. We have grown the crystals of YbOCl and synthesized the polycrystals of SmSI, ErOF, HoOF and DyOF, and made careful structural characterizations. We carry out magnetic and heat capacity measurements down to 1.8 K and find no obvious magnetic transition in all the samples but DyOF. The van der Waals interlayer coupling highlights the true two-dimensionality of the family which is vital for the exact realization of Abelian/non-Abelian anyons, and the graphene-like feature will be a prominent advantage for developing miniaturized devices. The family is expected to act as an inspiring material platform for the exploration of KSL physics.
Alkali metal rare-earth chalcogenide $ARECh2$ (A=alkali or monovalent metal, RE=rare earth, Ch=O, S, Se, Te), is a large family of quantum spin liquid (QSL) candidates we discovered recently. Unlike $YbMgGaO4$, most members in the family except for the oxide ones, have relatively small crystalline electric-field (CEF) excitation levels, particularly the first ones. This makes the conventional Curie-Weiss analysis at finite temperatures inapplicable and CEF excitations may play an essential role in understanding the low-energy spin physics. Here we considered an effective magnetic Hamiltonian incorporating CEF excitations and spin-spin interactions, to accurately describe thermodynamics in such a system. By taking $NaYbSe2$ as an example, we were able to analyze magnetic susceptibility, magnetization under pulsed high fields and heat capacity in a systematic and comprehensive way. The analysis allows us to produce accurate anisotropic exchange coupling energies and unambiguously determine a crossover temperature ($sim$25 K in the case of $NaYbSe2$), below which CEF effects fade away and pure spin-spin interactions stand out. We further validated the effective picture by successfully explaining the anomalous temperature dependence of electron spin resonance (ESR) spectral width. The effective scenario in principle can be generalized to other rare-earth spin systems with small CEF excitations.
We report a comprehensive investigation of the magnetism of the $S$ = 3/2 triangular-lattice antiferromagnet, $alpha$-CrOOH(D) (delafossites green-grey powder). The nearly Heisenberg antiferromagnetic Hamiltonian ($J_1$ $sim$ 23.5 K) with a weak single-ion anisotropy of $|D|$/$J_1$ $sim$ 4.6% is quantitatively determined by fitting to the electron spin resonance (ESR) linewidth and susceptibility measured at high temperatures. The weak single-ion anisotropy interactions, possibly along with other perturbations, e.g. next-nearest-neighbor interactions, suppress the long-range magnetic order and render the system disordered, as evidenced by both the absence of any clear magnetic reflections in neutron diffraction and the presence of the dominant paramagnetic ESR signal down to 2 K ($sim$ 0.04$J_1$$S^2$), where the magnetic entropy is almost zero. The power-law behavior of specific heat ($C_m$ $sim$ $T^{2.2}$) observed below the freezing temperature of $T_f$ = 25 K in $alpha$-CrOOH or below $T_f$ = 22 K in $alpha$-CrOOD is insensitive to the external magnetic field, and thus is consistent with the theoretical prediction of a gapless U(1) Dirac quantum spin liquid (QSL) ground state. At low temperatures, the spectral weight of the low-energy continuous spin excitations accumulates at the K points of the Brillouin zone, e.g. $|mathbf{Q}|$ = 4$pi$/(3$a$), and the putative Dirac cones are clearly visible. Our work is a first step towards the understanding of the possible Dirac QSL ground state in this triangular-lattice magnet with $S$ = 3/2.
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