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.
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 i…
We develop a quantum spin liquid theory for quantum magnets with easy-plane ferromagnetic exchange. These strongly entangled quantum states are obtained by dimer coverings of 2D lattices with triplet $S = 1, m_z = 0$ bonds, forming a triplet resonating valence bond (tRVB) state. We discuss the conditions and the procedure to transfer well-known results from conventional singlet resonating valence bond theory to tRVB. Additionally, we present mean field theories of Abrikosov fermions on 2D triangular and square lattices, which can be controlled in an appropriate large $N$ limit. We also incorpo…
We present scanning tunneling microscopy and spectroscopy studies around an individual excess Fe atom, working as a local perturbation, in the parent material of the iron-chalcogenide superconductor Fe$_{1+δ}$Te. Spectroscopic imaging reveals a novel isosceles triangular electronic structure around the excess Fe atoms. Its spatial symmetry reects the underlying bicollinear antiferromagnetic spin state and the structural monoclinic symmetry. These findings provide important clues to understand the role of the excess Fe atoms, which complicate the understanding of the phenomena occurring in iron…
The rare-earth triangular-lattice chalcogenide is a great platform for exploring both spin liquids and novel magnetic orders with anisotropic spin interactions and magnetic frustrations. Here, we report the thermodynamic and neutron scattering measurements of rare-earth triangular-lattice chalcogenide KErSe$_{2}$, using single-crystal samples. Our experiments revealed a long-range stripe order below 0.2 K. Although the magnetic order was three-dimensional, magnetic excitations exhibited negligible modulation along the z direction, indicating very weak interlayer coupling. Furthermore, magnetic…
We have characterized the magnetic and structural properties of the CdLn2Se4 (Ln = Dy, Ho), and CdLn2S4 (Ln = Ho, Er, Tm, Yb) spinels. We observe all compounds to be normal spinels, possessing a geometrically frustrated sublattice of lanthanide atoms with no observable structural disorder. Fits to the high temperature magnetic susceptibilities indicate these materials to have effective antiferromagnetic interactions, with Curie-Weiss temperatures theta ~ -10 K, except CdYb2S4 for which theta ~ -40 K. The absence of magnetic long range order or glassiness above T = 1.8 K strongly suggests that …
The anisotropic-exchange spin-1/2 model on a triangular lattice has been used to describe the rare-earth chalcogenides, which may have exotic ground states. We investigate the quantum phase diagram of the model by using the projected entangled pair state (PEPS) method, and compare it to the classical phase diagram. Besides two stripe-ordered phase, and the 120$^\circ$ state, there is also a multi-\textbf{Q} phase. We identify the multi-\textbf{Q} phase as a $Z_{2}$ vortex state. No quantum spin liquid state is found in the phase diagram, contrary to the previous DMRG calculations.
The electronic structure of some europium chalcogenides and pnictides is calculated using the {\it ab-initio} self-interaction corrected local-spin-density approximation (SIC-LSD). This approach allows both a localised description of the rare earth $f-$electrons and an itinerant description of $s$, $p$ and $d$-electrons. Localising different numbers of $f$-electrons on the rare earth atom corresponds to different nominal valencies, and the total energies can be compared, providing a first-principles description of valency. All the chalcogenides are found to be insulators in the ferromagnetic s…
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 measure…
We report the magnetic properties of compounds in the KBaRE(BO3)2 family (RE= Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb), materials with a planar triangular lattice composed of rare earth ions. The samples were analyzed by x-ray diffraction and crystallize in the space group R-3m. Physical property measurements indicate the compounds display predominantly antiferromagnetic interactions between spins without any signs of magnetic ordering above 1.8 K. The ideal 2D rare earth triangular layers in this structure type make it a potential model system for investigating magnetic frustration in rare-earth-b…
Pyrochlore lattices, which are found in two important classes of materials -- the $A_2B_2X_7$ pyrochlore family and the $AB_2X_4$ spinel family -- are the quintessential 3-dimensional frustrated lattice architecture. While historically oxides ($X =$~O) have played the starring role in this field, the past decade has seen materials synthesis breakthroughs that have lead to the emergence of fluoride ($X =$~F) and chalcogenide ($X =$~S, Se) pyrochlore lattice materials. In this Research Update, we summarize recent progress in understanding the magnetically frustrated ground states in three famili…
Motivated by the rapid experimental progress on the spin-orbit-coupled Mott insulators, we propose and study a generic spin model that describes the interaction between the non-Kramers doublets on a triangular lattice and is relevant for triangular lattice rare-earth magnets. We predict that the system supports both pure quadrupolar orders and intertwined multipolar orders in the phase diagram. Besides the multipolar orders, we explore the magnetic excitations to reveal the dynamic properties of the systems. Due to the peculiar properties of the non-Kramers doublets and the selective coupling …
We report the single-crystal growth and the fundamental magnetic and thermodynamic properties of a rare-earth triangular lattice antiferromagnet CeCd$_3$As$_3$. In this rare-earth antiferromagnet, the Ce local moments form a perfect triangular lattice. Due to the spin-orbital-entangled nature of the Ce local moments, the compound exhibits extremely anisotropic antiferromagnetic couplings along the c direction and in the ab plane respectively. We show that CeCd$_3$As$_3$ represents a {\it rare} experimental realization of an antiferromagnetic Ising model on a two dimensional triangular lattice …
We report the properties of a triangular lattice iron-chalcogenide antiferromagnet FeAl$_{2}$Se$_{4}$. The spin susceptibility reveals a significant antiferromagnetic interaction with a Curie-Weiss temperature Θ$_{CW}$ ~ -200K and a spin-2 local moment. Despite a large spin and a large |Θ$_{CW}$|, the low-temperature behaviors are incompatible with conventional classical magnets. No long-range order is detected down to 0.4K. Similar to the well-known spin-1 magnet NiGa$_{2}$S$_{4}$, the specific heat of FeAl$_{2}$Se$_{4}$ exhibits an unusual double-peak structure and a T$^{2}$ power law at low…
Magnetic frustration in metallic rare earth lanthanides ($Ln$) with $4f$-electrons is crucial for producing interesting magnetic phases with high magnetic anisotropy where intertwined charge and spin degrees of freedom lead to novel phenomena. Here we report on the magnetic, thermodynamic, and electrical transport properties of TbAuAl$_4$Ge$_2$. Tb ions form 2-dimensional triangular lattice layers which stack along the crystalline $c$-axis. The magnetic phase diagram reveals multiple nearly degenerate ordered states upon applying field along the magnetically easy $ab$-plane before saturation. …
A primary goal at the interface of theoretical and experimental quantum magnetism is the investigation of exotic spin states, most notably quantum spin liquids (QSLs). Magnetic rare-earth ions go beyond the straightforward paradigm of geometrical frustration in Heisenberg antiferromagnets by introducing competing energy scales, and in particular their strong spin-orbit coupling creates multiple split crystal electric-field (CEF) levels, leading to anisotropic effective spin models with intrinsic frustration. While rare-earth delafossites have a triangular-lattice geometry, and thus have gained…
A triangular lattice selenide series of rare earth (RE), CsRESe2, were synthesized as large single crystals using a flux growth method. This series stabilized in either trigonal (R-3m) or hexagonal (P63/mmc) crystal systems. Physical properties of CsRESe2 were explored by magnetic susceptibility and heat capacity measurements down to 0.4 K. Antiferromagnetic interaction was observed in all magnetic compounds, while no long-range magnetic order was found, indicating the frustrated magnetism. CsDySe2 presents spin freezing at 0.7 K, revealing a spin-glass state. CsCeSe2 and CsYbSe2 present broad…
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 who 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 expectation…
CeCd$_3$As$_3$ is a rare-earth triangular-lattice antiferromagnet with large inter-layer separation. Our field-dependent heat capacity measurements at dilution fridge temperatures allow us to trace the field-evolution of the spin-excitation gaps throughout the antiferromagnetic and paramagnetic regions. The distinct gap evolution places strong constraints on the microscopic pseudo-spin model, which, in return, yields a close {\it quantitative} description of the gap behavior. This analysis provides crucial insights into the nature of the magnetic state of CeCd$_3$As$_3$, with a certainty regar…
The breakdown of magnons, the quasiparticles of magnetic systems, has rarely been seen. By using an inelastic neutron scattering technique we report the observation of spontaneous magnon decay in multiferroic LuMnO$_3$, a simple two-dimensional Heisenberg triangular lattice antiferromagnet, with large spin, S = 2. The origin of this rare phenomenon lies in the non-vanishing cubic interaction between magnons in the spin Hamiltonian arising from the noncollinear 120$^o$ spin structure. We observed all three key features of the nonlinear effects as theoretically predicted: a roton-like minimum, a…
We report the de Haas-van Alphen (dHvA) oscillations and first-principle calculations for triangular antiferromagnet PdCrO2 showing unconventional anomalous Hall effect (AHE). The dHvA oscillations in PdCrO2 reveal presence of several 2 dimensional Fermi surfaces of smaller size than found in nonmagnetic PdCoO2. This evidences Fermi surface reconstruction due to the non-collinear 120 antiferromagnetic ordering of the localized Cr, consistent with the first principle calculations. The temperature dependence of dHvA oscillations shows no signature of additional modification of Cr spin structure …
Spin-1/2 antiferromagnetic triangular lattice models are paradigms of geometrical frustration, revealing very different ground states and quantum effects depending on the nature of anisotropies in the model. Due to strong spin orbit coupling and crystal field effects, rare-earth ions can form pseudo-spin-1/2 magnetic moments with anisotropic single-ion and exchange properties. Thus, rare-earth based triangular lattices enable the exploration of this interplay between frustration and anisotropy. Here we study one such case, the rare-earth double vanadate glaserite material K$_3$Er(VO$_4$)$_2$, …
Exotic magnetism and persistent spin dynamics in a frustrated Jeff = 1/2 triangular lattice antiferromagnet
Indian Institute of Technology Madras（印度马德拉斯理工学院）；Jožef Stefan Institute（约瑟夫·斯特凡研究所）；Faculty of Mathematics and Physics, University of Ljubljana（卢布尔雅那大学数学物理学院）；ISIS facility, Rutherford Appleton Laboratory（鲁瑟福阿普尔顿实验室ISIS设施）
A phase transition is often accompanied by the appearance of an order parameter and symmetry breaking. Certain magnetic materials exhibit exotic hidden-order phases, in which the order parameters are not directly accessible to conventional magnetic measurements. Thus, experimental identification and theoretical understanding of a hidden order are difficult. Here we combine neutron scattering and thermodynamic probes to study the newly discovered rare-earth triangular-lattice magnet TmMgGaO$_4$. Clear magnetic Bragg peaks at K points are observed in the elastic neutron diffraction measurements.…
Frustrated magnets host the promises of material realizations of new paradigm of quantum matter, while direct comparison of unbiased model calculations with experimental measurements is still very challenging. Here, we design and implement a protocol of employing many-body computation methodologies for accurate model calculation -- both equilibrium and dynamical properties -- of a frustrated rare-earth magnet TmMgGaO$_4$ (TMGO), which perfectly explains the corresponding experimental findings. Our results confirm TMGO is an ideal realization of triangular-lattice Ising model with an intrinsic …
Residual entropy is a key feature associated with emergence in many-body systems. From a variety of frustrated magnets to the onset of spin-charge separation in Hubbard models and fermion-$Z_2$-flux variables in Kitaev models, the freezing of one set of degrees of freedom and establishment of local constraints are marked by a plateau in entropy as a function of temperature. Yet, with the exception of rare-earth pyrochlore family of spin-ice materials, evidence for such plateaus is rarely seen in real materials, raising questions about their robustness. Following recent experimental findings of…
Frustration, spin correlations and interplay between competing degrees of freedom are some of the key ingredients that underlie exotic states with fractional excitations in quantum materials. Rare-earth based two dimensional magnetic lattice wherein crystal electric field, spin-orbit coupling, anisotropy and electron correlation between rare-earth moments offer a new paradigm in this context. Herein, we present crystal structure, magnetic susceptibility and specific heat accompanied by crystal electric field calculations on the polycrystalline sample of Ba3RB9O18 (R = Yb, Er) in which R3+ ions…
Rare-earth delafossites were recently proposed as promising candidates for the realization of an effective $S$=1/2 quantum spin liquid (QSL) on the triangular lattice. In contrast to the most actively studied triangular-lattice antiferromagnet YbMgGaO$_4$, which is known for considerable structural disorder due to site intermixing, NaYbS$_2$ delafossite realizes structurally ideal triangular layers. We present detailed $μ$SR studies on this regular (undistorted) triangular Yb sublattice based system with effective spin $J_{\mathrm{eff}}=1/2$ in the temperature range 0.05 - 40 K. Zero-field (ZF…
Motivated by the recent development in strong spin-orbit-coupled materials, we consider the dipole-octupole doublets on the triangular lattice. We propose the most general interaction between these unusual local moments. Due to the spin-orbit entanglement and the special form of its wavefunction, the dipole-octupole doublet has a rather peculiar property under the lattice symmetry operation. As a result, the interaction is highly anisotropic in the pseudospin space, but remarkably, is uniform spatially. We analyze the ground state properties of this generic model and emphasize the hidden multi…
Employing exact diagonalization, we systematically study the anisotropic Heisenberg model which is related to rare-earth triangular-lattice materials. We probe its full 3D phase diagram afresh and identify a large region of quantum spin liquid (QSL) phase which can extend to the QSL region of the $J_1$--$J_2$ triangular Heisenberg model. Furthermore, we explore the magnetization curves of different phases and reproduce the 1/3-magnetization plateau in the quantum spin liquid phase region. More importantly, to study the possible chemical disorders in real materials, we consider the randomness o…
Interleaved bond frustration in a triangular lattice antiferromagnet
University of California, Santa Barbara（加州大学圣塔芭芭拉分校）；Technical University of Munich（慕尼黑工业大学）；Oak Ridge National Laboratory（橡树岭国家实验室）；Cornell High Energy Synchrotron Source, Cornell University（康奈尔大学高能同步辐射光源，康奈尔大学）；Advanced Photon Source, Argonne National Laboratory（阿贡国家实验室先进光子源）
Rare earth triangular lattice materials have been proposed as a good platform for the investigation of frustrated magnetic ground states. KErSe$_2$ with the delafossite structure, contains perfect two-dimensional Er$^{3+}$ triangular layers separated by potassium ions, realizing this ideal configuration and inviting study. Here we investigate the magnetism of KErSe$_2$ at miliKelvin temperatures by heat capacity and neutron powder diffraction. Heat capacity results reveal a magnetic transition at 0.2 K in zero applied field. This long-range order is suppressed by an applied magnetic field of 0…
RbFe(MoO4)2 is a rare example of a nearly two-dimensional Heisenberg antiferromagnet on a triangular lattice. Magnetic resonance spectra and magnetization curves reveal that the system has a layered spin structure with six magnetic sublattices. The sublattices within a layer are arranged in a triangular manner with the magnetization vectors 120 degree apart. The H-T phase diagram, containing at least five different magnetic phases is constructed. In zero field, RbFe(MoO4)2 undergoes a phase transition at T_N=3.8 K into a non-collinear triangular spin structure with all the spins confined in th…
We report high resolution neutron scattering measurements on the triangular lattice Mott insulator Na$_x$CrO$_2$ ($x$=1) which has recently been shown to exhibit an unusually broad fluctuating crossover regime extending far below the onset of spin freezing ($T_c\sim$41K). Our results show that below some crossover temperature ($T\sim0.75T_c$) a small incommensuration develops which helps resolve the spin frustration and drives three-dimensional magnetic order supporting coherent spin wave modes. This incommensuration assisted dimensional crossover suggests that inter-layer frustration is respo…
The family of rare earth chalcogenides $ARECh_{2}$ (A = alkali or monovalent ions, RE = rare earth, and Ch = O, S, Se, and Te) appears as an inspiring playground for studying quantum spin liquids (QSL). The crucial low-energy spin dynamics remain to be uncovered. By employing muon spin relaxation ($μ$SR) and zero-field (ZF) AC susceptibility down to 50 mK, we are able to identify the gapless QSL in $NaYbSe_{2}$, a representative member with an effective spin-1/2, and explore its unusual spin dynamics. The ZF $μ$SR experiments unambiguously rule out spin ordering or freezing in $NaYbSe_{2}$ dow…
Motivated by the recent experimental progress on the strong spin-orbit-coupled rare earth triangular antiferromagnet, we analyze the highly anisotropic spin model that describes the interaction between the spin-orbit-entangled Kramers' doublet local moments on the triangular lattice. We apply the Luttinger-Tisza method, the classical Monte Carlo simulation, and the self-consistent spin wave theory to analyze the anisotropic spin Hamiltonian. The classical phase diagram includes the 120-degree state and two distinct stripe ordered phases. The frustration is very strong and significantly suppres…
Antiferromagnetically coupled S=1/2 spins on an isotropic triangular lattice is the paradigm of frustrated quantum magnetism, but structurally ideal realizations are rare. Here we investigate NaYbO$_2$, which hosts an ideal triangular lattice of $J_{eff}=1/2$ moments with no inherent site disorder. No signatures of conventional magnetic order appear down to 50 mK, strongly suggesting a quantum spin liquid ground state. We observe a two-peak specific heat and a nearly quadratic temperature dependence in accord with expectations for a two-dimensional Dirac spin liquid. Application of a magnetic …
Disordered magnetic states known as spin liquids are of paramount importance in both fundamental and applied science. A classical state of this kind was predicted for the Ising antiferromagnetic triangular model more than half a century ago, while additional non-commuting exchange terms were proposed to induce its quantum version -- a quantum spin liquid. These predictions have not been yet confirmed experimentally. Here we report a discovery of such a state in the structurally perfect triangular-lattice antiferromagnet NdTa$_7$O$_{19}$. Its magnetic ground state is characterized by spin-1/2 d…
We have grown single crystals of Na$_2$BaNi(PO$_4$)$_2$, a new spin-1 equilateral triangular lattice antiferromagnet (ETLAF), and performed magnetic susceptibility, specific heat and thermal conductivity measurements at ultralow temperatures. The main results are (i) at zero magnetic field, Na$_2$BaNi(PO$_4$)$_2$ exhibits a magnetic ordering at 430 mK with a weak ferromagnetic moment along the $c$ axis. This suggests a canted 120$^\circ$ spin structure, which is in a plane including the crystallographic $c$ axis due to the existence of an easy-axis anisotropy and ferromagnetically stacked alon…
The rare-earth magnet TmMgGaO$_{4}$ is proposed to be an intrinsic quantum Ising magnet described by the antiferromagnetic transverse field Ising model (TFIM) on a triangular lattice, where the relevant degrees of freedom are the non-degenerate dipole-multipole doublets of the Tm$^{3+}$ ions and the transverse field has an intrinsic origin from the weak splitting of the doublet. We compare this special doublet of Tm$^{3+}$ with the dipole-octupole Kramers doublet. We study the proposed effective model for the Tm-based triangular lattice and consider the effects of external magnetic fields and …
Absence of Long-Range Order and Magnetic Anisotropy in the Triangular Magnet NdMgAl$_{11}$O$_{19}$
Charles University（查理大学）；Adam Mickiewicz University（亚当·密茨凯维奇大学）；Institute of Molecular Physics, Polish Academy of Sciences（波兰科学院分子物理研究所）；NanoBioMedical Centre（纳米生物医学中心）；Institute of Physics of the Czech Academy of Sciences（捷克科学院物理研究所）；University of Augsburg（奥格斯堡大学）
Non-collinear magnetic order arises for various reasons in several magnetic systems and exhibits interesting spin dynamics. Despite its ubiquitous presence, little is known of how magnons, otherwise stable quasiparticles, decay in these systems, particularly in metallic magnets. Using inelastic neutron scattering, we examine the magnetic excitation spectra in a metallic non-collinear antiferromagnet CrB$_{2}$, in which Cr atoms form a triangular lattice and display incommensurate magnetic order. Our data show intrinsic magnon damping and continuum-like excitations that cannot be explained by l…
Noncentrosymmetric Triangular Magnet CaMnTeO$_6$: Strong Quantum Fluctuations and Role of s0 vs. s2 Electronic States in Competing Exchange Interactions
