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L. S. Wu

Publications and source records attributed to L. S. Wu.

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Magnetic phase diagrams and large magnetocaloric effects of the two-dimensional antiferromagnetic triangular lattice of Gd$^{3+}$ ions in KBaGd(BO$_3$)$_2$

We report a detailed study of the magnetic properties of KBaGd(BO$_3$)$_2$, in which magnetic Gd$^{3+}$ ($S=7/2$) ions form into two-dimensional triangular layers. Magnetization, specific heat and magnetocaloric effect (MCE) measurements have been performed on KBaGd(BO$_3$)$_2$ single crystals. The results show that a long-range antiferromagnetic state is established below $T_{\rm N}=0.24$ K. In zero fields, only about half of the full entropy is released at $T_{\rm N}$, indicating that not all the magnetic moments are frozen below the ordering temperature, as expected from the geometrical frustration of the triangular spin lattice. Further studies under external fields were performed down to 50 mK, and the magnetic phase diagrams are established with magnetic fields applied both within and perpendicular to the triangular plane. KBaGd(BO$_3$)$_2$ serves as an example of a two-dimensional triangular lattice with large spin values ($S=7/2$) and can be directly compared with the iso-structure KBaR(BO$_3$)$_2$ (R = Dy-Yb) family of doublet ground states, which exhibit effective spins of $S=1/2$.

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Antiferromagnetism and Ising Ground States in the Rare-earth Garnet Nd$_3$Ga$_5$O$_{12}$

In this paper, we investigate the low temperature magnetic properties of the rare-earth garnet compound Nd$_3$Ga$_5$O$_{12}$ in detail by means of magnetization, specific heat and magnetocaloric effect measurements. The magnetic thermal properties along with the crystal field calculations reveal that the Nd$^{3+}$ ions form into a frustrated hyper-kagome lattice with connected triangles have an Ising-like ground state with the easy axis along the local [100], [010] and [001] directions. Instead of a quantum spin liquid ground state, an antiferromagnetically ordered state is found below $T_{\mathrm{N}}=0.52~\rm K$. With applying field in the [111] direction, the antiferromagnetic order is suppressed at the critical field of $B_{\mathrm{c}}=0.75~\rm T$, and enhancement of the critical fluctuations with linear crossover behaviors is observed near the critical point.

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Successive magnetic orderings in the Ising spin chain magnet DyNi$_5$Ge$_3$

In this report, we investigated a new rare earth based one-dimensional Ising spin chain magnet~\DNG~by means of magnetization, specific heat and powder neutron diffraction measurements. Due to the crystalline electrical field splitting, the magnetic Dy ions share an Ising like ground doublet state. Owning to the local point symmetry, these Ising moments form into two canted magnetic sublattices, which were further confirmed by the angle-dependent magnetization measurement. In zero fields, two successive antiferromagnetic phase transitions were found at temperatures $T_{\mathrm{N1}}=6~\rm K$ and $T_{\mathrm{N2}}=5~\rm K$, respectively. Only part of the moments are statically ordered in this intermediate state between $T_{\mathrm{N1}}$ and $T_{\mathrm{N2}}$. Powder neutron diffraction experiments at different temperatures were performed as well. An incommensurate magnetic propagation vector of $\mathbf{k_{\rm m}}=(0.5,0.4,0.5)$ was identified. The refined spin configurations through the irreducible representation analysis confirmed that these Ising spins are canted in the crystal $ab$~plane.

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Interplay of itinerant electrons and Ising moments in a hybrid honeycomb quantum magnet TmNi$_3$Al$_9$

The interplay between itinerant electrons and local magnetic moments in quantum materials brings about rich and fascinating phenomena and stimulates various developments in the theoretical framework. In this work, thermodynamic, electric transport, and neutron diffraction measurements were performed on a newly synthesized honeycomb lattice magnet TmNi$_3$Al$_9$. Based on the experimental data, a magnetic field temperature phase diagram was constructed, exhibiting three essentially different magnetic regions. Below ${T_{\rm N}=2.97 \pm 0.02}\ \rm K$ Tm$^{3+}$ moments order antiferromagnetically in zero field. We found that the Tm$^{3+}$ ions form a pseudo-doublet ground state with the Ising-like moments lying normal to the two-dimensional honeycomb layers. Application of a magnetic field along the easy axis gradually suppresses the antiferromagnetic order in favor of an induced ferromagnetic state above the critical field ${B_c=0.92 \pm 0.05}\ \rm T$. In the vicinity of $B_c$, a strong enhancement of the quantum spin fluctuations was observed. The quantum Ising nature of the local moments and the coupling to itinerant electrons are discussed.

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Spinon Confinement and a Sharp Longitudinal Mode in Yb$_2$Pt$_2$Pb in Magnetic Fields

The fundamental excitations in an antiferromagnetic chain of spins-1/2 are spinons, de-confined fractional quasiparticles that when combined in pairs, form a triplet excitation continuum. In an Ising-like spin chain the continuum is gapped and the ground state is N{é}el ordered. Here, we report high resolution neutron scattering experiments, which reveal how a magnetic field closes this gap and drives the spin chains in \YPP\ to a critical, disordered Luttinger-liquid state. In \YPP\ the effective spins-1/2 describe the dynamics of large, Ising-like Yb magnetic moments, ensuring that the measured excitations are exclusively longitudinal, which we find to be well described by time-dependent density matrix renormalization group calculations. The inter-chain coupling leads to the confinement of spinons, a condensed matter analog of quark confinement in quantum chromodynamics. Insensitive to transverse fluctuations, our measurements show how a gapless, dispersive longitudinal mode arises from confinement and evolves with magnetic order.

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Antiferromagnetic ordering and dipolar interactions of YbAlO$_3$

In this paper we report low-temperature magnetic properties of the rare-earth perovskite material YbAlO$_3$. Results of elastic and inelastic neutron scattering experiment, magnetization measurements along with the crystalline electrical field (CEF) calculations suggest that the ground state of Yb moments is a strongly anisotropic Kramers doublet, and the moments are confined in the $ab$-plane, pointing at an angle of $φ= \pm 23.5^{\circ}$ to the $a$-axis. With temperature decreasing below $T_{\rm N}=0.88$ K, Yb moments order into the coplanar, but non-collinear antiferromagnetic (AFM) structure $AxGy$, where the moments are pointed along their easy-axes. In addition, we highlight the importance of the dipole-dipole interaction, which selects the type of magnetic ordering and may be crucial for understanding magnetic properties of other rare-earth orthorhombic perovskites. Further analysis of the broad diffuse neutron scattering shows that one-dimensional interaction along the $c$-axis is dominant, and suggests YbAlO$_3$ as a new member of one dimensional quantum magnets.

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Tomonaga-Luttinger Liquid Behavior and Spinon Confinement in YbAlO$_3$

Low dimensional quantum magnets are interesting because of the emerging collective behavior arising from strong quantum fluctuations. The one-dimensional (1D) S = 1/2 Heisenberg antiferromagnet is a paradigmatic example, whose low-energy excitations, known as spinons, carry fractional spin S = 1/2. These fractional modes can be reconfined by the application of a staggered magnetic field. Even though considerable progress has been made in the theoretical understanding of such magnets, experimental realizations of this low-dimensional physics are relatively rare. This is particularly true for rare-earth based magnets because of the large effective spin anisotropy induced by the combination of strong spin-orbit coupling and crystal field splitting. Here, we demonstrate that the rare-earth perovskite YbAlO$_3$ provides a realization of a quantum spin S = 1/2 chain material exhibiting both quantum critical Tomonaga-Luttinger liquid behavior and spinon confinement-deconfinement transitions in different regions of magnetic field-temperature phase diagram.

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Behavior of the breathing pyrochlore lattice Ba$_3$Yb$_2$Zn$_5$O$_{11}$ in applied magnetic field

The breathing pyrochlore lattice material Ba$_3$Yb$_2$Zn$_5$O$_{11}$ exists in the nearly decoupled limit, in contrast to most other well-studied breathing pyrochlore compounds. As a result, it constitutes a useful platform to benchmark theoretical calculations of exchange interactions in insulating Yb$^{3+}$ magnets. Here we study Ba$_3$Yb$_2$Zn$_5$O$_{11}$ at low temperatures in applied magnetic fields as a further probe of the physics of this model system. Experimentally, we consider the behavior of polycrystalline samples of Ba$_3$Yb$_2$Zn$_5$O$_{11}$ with a combination of inelastic neutron scattering and heat capacity measurements down to 75 mK and up to fields of 10 T. Consistent with previous work, inelastic neutron scattering finds a level crossing near 3 T, but no significant dispersion of the spin excitations is detected up to the highest applied fields. Refinement of the theoretical model previously determined at zero field can reproduce much of the inelastic neutron scattering spectra and specific heat data. A notable exception is a low temperature peak in the specific heat near 0.1 K. This may indicate the scale of interactions between tetrahedra or may reflect undetected disorder in Ba$_3$Yb$_2$Zn$_5$O$_{11}$.

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Decoupled spin dynamics in the rare-earth orthoferrite YbFeO$_3$: Evolution of magnetic excitations through the spin-reorientation transition

In this paper we present a comprehensive study of magnetic dynamics in the rare-earth orthoferrite YbFeO$_3$ at temperatures below and above the spin-reorientation (SR) transition $T_{\mathrm{SR}}=7.6$ K, in magnetic fields applied along the $a, b$ and $c$ axes. Using single-crystal inelastic neutron scattering, we observed that the spectrum of magnetic excitations consists of two collective modes well separated in energy: 3D gapped magnons with a bandwidth of $\sim$60 meV, associated with the antiferromagnetically (AFM) ordered Fe subsystem, and quasi-1D AFM fluctuations of $\sim$1 meV within the Yb subsystem, with no hybridization of those modes. The spin dynamics of the Fe subsystem changes very little through the SR transition and could be well described in the frame of semiclassical linear spin-wave theory. On the other hand, the rotation of the net moment of the Fe subsystem at $T_{\mathrm{SR}}$ drastically changes the excitation spectrum of the Yb subsystem, inducing the transition between two regimes with magnon and spinon-like fluctuations. At $T < T_{\mathrm{SR}}$, the Yb spin chains have a well defined field-induced ferromagnetic (FM) ground state, and the spectrum consists of a sharp single-magnon mode, a two-magnon bound state, and a two-magnon continuum, whereas at $T > T_{\mathrm{SR}}$ only a gapped broad spinon-like continuum dominates the spectrum. In this work we show that a weak quasi-1D coupling within the Yb subsystem $J_\text{Yb-Yb}$, mainly neglected in previous studies, creates unusual quantum spin dynamics on the low energy scales. The results of our work may stimulate further experimental search for similar compounds with several magnetic subsystems and energy scales, where low-energy fluctuations and underlying physics could be "hidden" by a dominating interaction.

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Unveiling the role of competing fluctuations at an unconventional quantum critical point

Quantum critical points (QCPs) are widely accepted as a source of a diverse set of collective quantum phases of matter. A central question is how the order parameters of phases near a QCP interact and determine the fundamental character of the critical dynamics which drive the quantum critical behavior. One of the most interesting proposals for the quantum critical behavior that occurs in correlated electron systems is that the behavior may arise from local, as opposed to long wavelength, critical fluctuations of the order parameter. The local criticality is believed to give rise to energy over temperature ($E/T$) scaling of the dynamic susceptibility with a fractional exponent near the quantum critical point (QCP). Here we show that $E/T$ scaling is indeed observed for CeCu$_{6-x}$Ag$_x$ but on closer inspection, the fluctuations can be separated into two components, implying that multiple order parameters play an important role in the unconventional critical behavior. Additionally, when the fluctuations corresponding to the magnetically ordered side of the phase diagram are separated, they are found to be three dimensional and to obey the scaling behavior expected for long wavelength fluctuations near an itinerant antiferromagnetic QCP.

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Magnetic ground state of the Ising-like antiferromagnet DyScO$_3$

We report the low temperature magnetic properties of the DyScO$_3$ perovskite, which were characterized by means of single crystal and powder neutron scattering, and by magnetization measurements. Below $T_{\mathrm{N}}=3.15$ K, Dy$^{3+}$ moments form an antiferromagnetic structure with an easy axis of magnetization lying in the $ab$-plane. The magnetic moments are inclined at an angle of $\sim\pm{28}^{\circ}$ to the $b$-axis. We show that the ground state Kramers doublet of Dy$^{3+}$ is made up of primarily $|\pm 15/2\rangle$ eigenvectors and well separated by crystal field from the first excited state at $E_1=24.9$ meV. This leads to an extreme Ising single-ion anisotropy, $M_{\perp}/M_{\|}\sim{0.05}$. The transverse magnetic fluctuations, which are proportional to $M^{2}_{\perp}/M^{2}_{\|}$, are suppressed and only moment fluctuations along the local Ising direction are allowed. We also found that the Dy-Dy dipolar interactions along the crystallographic $c$-axis are 2-4 times larger than in-plane interactions.

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Orbital-Exchange and Fractional Quantum Number Excitations in an f-electron Metal Yb$_2$Pt$_2$Pb

Exotic quantum states and fractionalized magnetic excitations, such as spinons in one-dimensional chains, are generally viewed as belonging to the domain of 3d transition metal systems with spins 1/2. Our neutron scattering experiments on the 4f-electron metal Yb$_2$Pt$_2$Pb overturn this common wisdom. We observe broad magnetic continuum dispersing in only one direction, which indicates that the underlying elementary excitations are spinons carrying fractional spin-1/2. These spinons are the quantum dynamics of the anisotropic, orbital-dominated Yb moments, and thus these effective quantum spins are emergent variables that encode the electronic orbitals. The unique birthmark of their unusual origin is that only longitudinal spin fluctuations are measurable, while the transverse excitations such as spin waves are virtually invisible to magnetic neutron scattering. The proliferation of these orbital-spinons strips the electrons of their orbital identity, and we thus report here a new electron fractionalization phenomenon, charge-orbital separation.

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Anisotropic exchange within decoupled tetrahedra in the quantum breathing pyrochlore Ba3Yb2Zn5O11

The low energy spin excitation spectrum of the breathing pyrochlore Ba3Yb2Zn5O11 has been investigated with inelastic neutron scattering. Several nearly resolution limited modes with no observable dispersion are observed at 250 mK while, at elevated temperatures, transitions between excited levels become visible. To gain deeper insight, a theoretical model of isolated Yb3+ tetrahedra parametrized by four anisotropic exchange constants is constructed. The model reproduces the inelastic neutron scattering data, specific heat, and magnetic susceptibility with high fidelity. The fitted exchange parameters reveal a Heisenberg antiferromagnet with a very large Dzyaloshinskii-Moriya interaction. Using this model, we predict the appearance of an unusual octupolar paramagnet at low temperatures and speculate on the development of inter-tetrahedron correlations.

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Magnetic structure of Yb2Pt2Pb: Ising moments on the Shastry-Sutherland Lattice

Neutron diffraction measurements were carried out on single crystals and powders of Yb2Pt2Pb, where Yb moments form planes of orthogonal dimers in the frustrated Shastry-Sutherland Lattice (SSL). Yb2Pt2Pb orders antiferromagnetically at TN=2.07 K, and the magnetic structure determined from these measurements features the interleaving of two orthogonal sublattices into a 5*5*1 magnetic supercell that is based on stripes with moments perpendicular to the dimer bonds, which are along (110) and (-110). Magnetic fields applied along (110) or (-110) suppress the antiferromagnetic peaks from an individual sublattice, but leave the orthogonal sublattice unaffected, evidence for the Ising character of the Yb moments in Yb2Pt2Pb. Specific heat, magnetic susceptibility, and electrical resistivity measurements concur with neutron elastic scattering results that the longitudinal critical fluctuations are gapped with E about 0.07 meV.

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Field tuned critical fluctuations in YFe2Al10: Evidence from magnetization, 27Al (NMR, NQR) investigations

We report magnetization, specific heat, and NMR investigations on YFe2Al10 over a wide range in temperature and magnetic field and zero field (NQR) measurements. Magnetic susceptibility, specific heat and spin-lattice relaxation rate divided by T (1/T1T) follow a weak power law (T^-0.4) temperature dependence, which is a signature of critical fluctuations of Fe moments. The value of the Sommerfeld-Wilson ratio and linear relation between 1/T1T and chi(T) suggest the existence of ferromagnetic correlations in this system. No magnetic ordering down to 50 mK in Cp(T) and the unusual temperature and field scaling of the bulk and NMR data are associated with a magnetic instability which drives the system to quantum criticality. The magnetic properties of the system are tuned by field wherein ferromagnetic fluctuations are suppressed and a crossover from quantum critical to FL behavior is observed with increasing magnetic field.

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Localized moments and the stability of antiferromagnetic order in Yb3Pt4

We present here the results of electrical resistivity ρ, magnetization M, ac susceptibility \c{hi}ac', and specific heat CM measurements that have been carried out on single crystals of Yb3Pt4 over a wide range of fields and temperatures. The 2.4-K Néel temperature that is found in zero field collapses under field to a first-order transition TN=0 at BCEP=1.85 T. In the absence of antiferromagnetic order, the specific heat CM(T,B), the magnetization M(T,B), and even the resistivity ρ(T,B) all display B/T scaling, indicating that they are dominated by strong paramagnetic fluctuations, where the only characteristic energy scale results from the Zeeman splitting of an energetically isolated, Yb doublet ground state. This paramagnetic scattering disappears with the onset of antiferromagnetic order, revealing Fermi liquid behavior Δρ=AT2 that persists up to the antiferromagnetic phase line TN(B), but not beyond. The first-order character of TN=0 and the ubiquity of the paramagnetic fluctuations imply that non-Fermi-liquid behaviors are absent in Yb3Pt4. In contrast to heavy fermions such as YbRh2Si2, Yb3Pt4 represents an extremely simple regime of f-electron behavior where the Yb moments and conduction electrons are almost decoupled, and where Kondo physics plays little role.

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Magnetic field tuning of antiferromagnetic Yb$_{3}$Pt$_{4}$

We present measurements of the specific heat, magnetization, magnetocaloric effect and magnetic neutron diffraction carried out on single crystals of antiferromagnetic Yb$_{3}$Pt$_{4}$, where highly localized Yb moments order at $T_{\rm N}=2.4$ K in zero field. The antiferromagnetic order was suppressed to $T_{\rm N}\rightarrow 0$ by applying a field of 1.85 T in the $ab$ plane. Magnetocaloric effect measurements show that the antiferromagnetic phase transition is always continuous for $T_{\rm N}>0$, although a pronounced step in the magnetization is observed at the critical field in both neutron diffraction and magnetization measurements. These steps sharpen with decreasing temperature, but the related divergences in the magnetic susceptibility are cut off at the lowest temperatures, where the phase line itself becomes vertical in the field-temperature plane. As $T_{\rm N}\rightarrow0$, the antiferromagnetic transition is increasingly influenced by a quantum critical endpoint, where $T_{\rm N}$ ultimately vanishes in a first order phase transition.

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Determination of the magnetic structure of Yb3Pt4: a k=0 local-moment antiferromagnet

We have used neutron diffraction measurements to study the zero-field magnetic structure of the intermetallic compound Yb3Pt4, which was earlier found to order antiferromagnetically at the Neel temperature TN=2.4 K, and displays a field-driven quantum critical point at 1.6 T. In Yb3Pt4, the Yb moments sit on a single low-symmetry site in the rhombohedral lattice with space group R-3. The Yb ions form octahedra with edges that are twisted with respect to the hexagonal unit cell, a twisting that results in every Yb ion having exactly one Yb nearest neighbor. Below TN, we found new diffracted intensity due to a k=0 magnetic structure. This magnetic structure was compared to all symmetry-allowed magnetic structures, and was subsequently refined. The best fitting magnetic structure model is antiferromagnetic, and involves pairs of Yb nearest neighbors on which the moments point almost exactly towards each other. This structure has moment components within the ab-plane as well as parallel to the c-axis, although the easy magnetization direction lies in the ab-plane. Our magnetization results suggest that besides the crystal-electric field anisotropy, anisotropic exchange favoring alignment along the c-axis is responsible for the overall direction of the ordered moments. The magnitude of the ordered Yb moments in Yb3Pt4 is 0.81 uB/Yb at 1.4 K. The analysis of the bulk properties, the size of the ordered moment, and the observation of well-defined crystal-field levels argue that the Yb moments are spatially localized in zero field.

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