Systematic extraction of crystal electric-field effects and quantum magnetic model parameters in triangular rare-earth magnets

Abstract

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 recent attention as candidates for hosting spin-1/2 QSL physics, the reliable extraction of effective spin models from the initial many-parameter CEF spectrum is a hard problem. Using the example of CsYbSe2, we demonstrate the unambiguous extraction of the Stevens-operators coefficients dictating the full CEF spectrum of Yb${}^{3+}$ by translating these into parameters with a direct physical interpretation. Specifically, we combine low-field susceptibility measurements with resonant torsion magnetometry experiments in fields up to 60 T to determine a sufficiently large number of physical parameters -- effective Zeeman splittings, anisotropic van Vleck coefficients, and magnetotropic coefficients -- that the set of Stevens-operator coefficients is unique. Our crucial identification of the strong corrections to the Zeeman splitting of Kramers doublets as van Vleck coefficients has direct consequences for the interpretation of all anisotropic magnetic susceptibility measurements. Our results allow us to determine the nature and validity of an effective spin-1/2 model for CsYbSe2, to provide input for theoretical studies of such models on the triangular lattice, and to provide additional materials insight into routes for achieving magnetic frustration and candidate QSL systems in rare-earth compounds.

arXiv comment17 pages, 7 figures

References in corpus (67)

• Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
• Quantum Spin Liquids
• Magnetic Pyrochlore Oxides
• Spin Liquid State in an Organic Mott Insulator with Triangular Lattice
• Spin Dynamics of the Spin-1/2 Kagome Lattice Antiferromagnet ZnCu_3(OH)_6Cl_2
• $\alpha$-RuCl3: a Spin-Orbit Assisted Mott Insulator on a Honeycomb Lattice
• Relevance of the Heisenberg-Kitaev model for the honeycomb lattice iridates A_2IrO_3
• Spin waves and revised crystal structure of honeycomb iridate Na2IrO3
• Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO4
• Experimental realization of a 2D fractional quantum spin liquid
• Rare-earth triangular lattice spin liquid: a single-crystal study of YbMgGaO${}_4$
• Evidence for a spinon Fermi surface in a triangular lattice quantum spin liquid candidate
• Experimental Realization of Spin-1/2 Triangular-Lattice Heisenberg Antiferromagnet
• Spin liquid nature in the Heisenberg $J_1$-$J_2$ triangular antiferromagnet
• Spin liquid phase of the $S=\frac{1}{2}$ $J_1-J_2$ Heisenberg model on the triangular lattice
• Field-tunable quantum disordered ground state in the triangular lattice antiferromagnet NaYbO${}_2$
• Observation of extended scattering continua characteristic of spin fractionalization in the 2D frustrated quantum magnet Cs2CuCl4 by neutron scattering
• Unusual ordered phases of highly frustrated magnets: a review
• Disorder-Induced Mimicry of a Spin Liquid in YbMgGaO${}_4$
• Direct Measurement of the Spin Hamiltonian and Observation of Condensation of Magnons in the 2D Frustrated Quantum Magnet Cs2CuCl4
• Competing Spin Liquid States in the Spin-$1/2$ Heisenberg Model On Triangular Lattice
• Crystalline Electric Field Randomness in the Triangular Lattice Spin-Liquid YbMgGaO${}_4$
• Frustrated quantum rare-earth pyrochlores
• Quantum Phase Diagram of the Triangular-Lattice XXZ Model in a Magnetic Field
• NaYbS${}_2$ - a new planar spin-$\frac{1}{2}$ triangular-lattice magnet and putative spin liquid
• Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore
• An anisotropic spin model of strong spin-orbit-coupled triangular antiferromagnets
• Quantum spin ices and topological phases from dipolar-octupolar doublets on the pyrochlore lattice
• Anisotropic field-induced ordering in the triangular-lattice quantum spin liquid NaYbSe${}_2$
• Topography of Spin Liquids on a Triangular Lattice
• Dirac Spin Liquid on the Spin-1/2 Triangular Heisenberg Antiferromagnet
• Field-induced instability of the quantum-spin-liquid ground state in the $J_{\mathrm{eff}}=\frac{1}{2}$ triangular-lattice compound NaYbO${}_2$
• Gapless spin-liquid phase in an extended spin 1/2 triangular Heisenberg model
• Static and Dynamical Properties of the Spin-1/2 Equilateral Triangular-Lattice Antiferromagnet Ba${}_3$CoSb${}_2$O${}_9$
• Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce${}_2$Zr${}_2$O${}_7$
• Time Evolution of an Infinite Projected Entangled Pair State: an Efficient Algorithm
• Anisotropic-Exchange Magnets on a Triangular Lattice: Spin Waves, Accidental Degeneracies, and Dual Spin Liquids
• Magnetic orders and topological phases from f-d exchange in pyrochlore iridates
• PyCrystalField: Software for Calculation, Analysis, and Fitting of Crystal Electric Field Hamiltonians
• Quantum spin liquid ground state in the disorder free triangular lattice NaYbS${}_2$
• Candidate Quantum Spin Liquid in the Ce\textsuperscript{3+} Pyrochlore Stannate Ce${}_2$Sn${}_2$O${}_7$
• Spinon Fermi surface spin liquid in a triangular lattice antiferromagnet NaYbSe${}_2$
• Dynamical structure factor of the $J_1-J_2$ Heisenberg model on the triangular lattice: magnons, spinons, and gauge fields
• Symmetry Enriched U(1) Topological Orders for Dipole-Octupole Doublets on a Pyrochlore Lattice
• Field-induced magnetic transition and spin fluctuation in quantum spin liquid candidate CsYbSe${}_2$
• A Class of Compounds Featuring Frustrated Triangular Magnetic Lattice CsRESe${}_2$ (RE=La-Lu): Quantum Spin-Liquid Candidates
• Spin liquids in geometrically perfect triangular antiferromagnets
• Spin excitations in the frustrated triangular lattice antiferromagnet NaYbO${}_2$
• Dynamical structure factor of the triangular antiferromagnet: the Schwinger boson theory beyond the mean field approach
• Direct determination of exchange parameters in Cs2CuBr4 and Cs2CuCl4: high-field ESR studies
• Fractionalized excitations in the partially magnetized spin liquid candidate YbMgGaO4
• Two-temperature scales in the triangular-lattice Heisenberg antiferromagnet
• Magnetic Phase Diagram of the S=1/2 Triangular-Lattice Heisenberg Antiferromagnet Ba3CoNb2O9
• Crystalline Electric-Field Excitations in Quantum Spin Liquids Candidate $NaYbS{e}_2$
• Ground States of Spin-1/2 Triangular Antiferromagnets in a Magnetic Field
• The effect of spin-orbit coupling on the effective-spin correlation in YbMgGaO4
• Yb delafossites: unique exchange frustration of 4f spin 1/2 moments on a perfect triangular lattice
• Scale-invariant magnetic anisotropy in RuCl${}_3$ at high magnetic fields
• Crystal field Hamiltonian and anisotropy in KErSe2 and CsErSe2
• Resonant torsion magnetometry in anisotropic quantum materials
• Determination of effective microscopic models for the frustrated antiferromagnets Cs${}_2$CuCl${}_4$ and Cs${}_2$CuBr${}_4$ by density functional methods
• Magnetoelastic hybrid excitations in CeAuAl${}_3$
• Mermin-Wagner physics, (H,T) phase diagram, and candidate quantum spin-liquid phase in the spin-1/2 triangular-lattice antiferromagnet Ba8CoNb6O24
• Crystalline electric field of Ce in trigonal symmetry: CeIr3Ge7 as a model case
• Dipolar-Octupolar Ising Antiferromagnetism in Sm${}_2$Ti${}_2$O${}_7$: A Moment Fragmentation Candidate
• Effective Spin-1/2 Moments on a Yb${}^{3+}$ Triangular Lattice: an ESR Study
• Lattice dynamics and coupled quadrupole-phonon excitations in CeAuAl${}_3$

Cited by in corpus (12)

• Field-Induced Spin Excitations in the Spin-1/2 Triangular-Lattice Antiferromagnet CsYbSe${}_2$
• Complete field-induced spectral response of the spin-1/2 triangular-lattice antiferromagnet CsYbSe${}_2$
• Exchange renormalized crystal field excitation in a quantum Ising magnet KTmSe${}_2$
• Tracking the evolution from isolated dimers to many-body entanglement in NaLu${}_x$Yb${}_{1-x}$Se${}_2$
• Nearly-Resonant Crystalline-Phononic Coupling in Quantum Spin Liquid Candidate CsYbSe${}_2$
• Magnetic properties of a spin-orbit entangled Jeff = 1/2 honeycomb lattice
• Quantifying uncertainties in crystal electric field Hamiltonian fits to neutron data
• Crystalline electric field excitations and their nonlinear splitting under magnetic fields in YbOCl
• Magnetotropic susceptibility
• Field-driven transition from quantum spin liquid to magnetic order in triangular-lattice antiferromagnets
• Heat conduction in magnetic insulators via hybridization of acoustic phonons and spin-flip excitations
• Field-Induced Magnon Decay, Magnon Shadows, and Roton-like Excitations in the Honeycomb Antiferromagnet YbBr${}_3$