arXiv subjects

M. D. Lumsden

Publications and source records attributed to M. D. Lumsden.

At least 19 recordsLinked to original sources

arXiv2024

Incident Beamline Design for a Modern Cold Triple Axis Spectrometer at the High Flux Isotope Reactor

A modern cold triple axis spectrometer is being planned for the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory. Here, we describe the design of an incident beamline that will put a flux of $\sim 10^8\mathrm{\frac{n}{cm^2 s}}$ on a sample with an area of 2 cm x 2 cm. It takes current physical constraints at HFIR into account and it can accommodate both single and multiplexed analyzer-detector secondary spectrometers and large superconducting magnets. The proposed incident beamline includes a multi-channel guide with horizontal focusing, a neutron velocity selector, components to facilitate an incident beam polarization option, and a double-focusing pyrolytic graphite monochromator. This work describes the process of optimizing the guide system and monochromator and summarizes the expected performance of the incident beamline for non-polarized operation.

physics.ins-det↗

arXiv2020

Van Hove singularity in the magnon spectrum of the antiferromagnetic quantum honeycomb lattice

The magnetic excitation spectrum of the quantum magnet YbCl$_3$ is studied with inelastic neutron scattering. The spectrum exhibits an unusually sharp feature within a broad continuum, as well as conventional spin waves. By including both transverse and longitudinal channels of the neutron response, linear spin wave theory with a single Heisenberg interaction on the honeycomb lattice reproduces all of the key features in the spectrum. In particular, the broad continuum corresponds to a two-magnon contribution from the longitudinal channel, while the sharp feature within this continuum is identified as a Van Hove singularity in the joint density of states, which indicates the two-dimensional nature of the two-magnon continuum. We term these singularities magneto-caustic features in analogy with caustic features in ray optics where focused envelopes of light are generated when light passes through or reflects from curved or distorted surfaces. The experimental demonstration of a sharp Van Hove singularity in a two-magnon continuum is important because analogous features in potential two-spinon continua could distinguish quantum spin liquids from merely disordered systems. These results establish YbCl$_3$ as a nearly ideal two-dimensional honeycomb lattice material hosting strong quantum effects in the unfrustrated limit.

cond-mat.str-el↗

arXiv2019

Crystal field splitting, local anisotropy, and low energy excitations in the quantum magnet YbCl$_3$

We study the correlated quantum magnet, YbCl$_3$, with neutron scattering, magnetic susceptibility, and heat capacity measurements. The crystal field Hamiltonian is determined through simultaneous refinements of the inelastic neutron scattering and magnetization data. The ground state doublet is well isolated from the other crystal field levels and results in an effective spin-1/2 system with local easy plane anisotropy at low temperature. Cold neutron spectroscopy shows low energy excitations that are consistent with nearest neighbor antiferromagnetic correlations of reduced dimensionality.

cond-mat.str-el↗

arXiv2019

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.

cond-mat.str-el↗

arXiv2019

Frustrated Magnetism in Mott Insulating (V$_{1-x}$Cr$_x$)$_2$O$_3$

V2O3 famously features all four combinations of paramagnetic vs antiferromagnetic, and metallic vs insulating states of matter in response to %-level doping, pressure in the GPa range, and temperature below 300 K. Using time-of-flight neutron spectroscopy combined with density functional theory calculations of magnetic interactions, we have mapped and analyzed the inelastic magnetic neutron scattering cross section over a wide range of energy and momentum transfer in the chromium stabilized antiferromagnetic and paramagnetic insulating phases (AFI & PI). Our results reveal an important magnetic frustration and degeneracy of the PI phase which is relieved by the rhombohedral to monoclinic transition at $T_N=185$ K due to a significant magneto-elastic coupling. This leads to the recognition that magnetic frustration is an inherent property of the paramagnetic phase in $\rm (V_{1-x}Cr_x)_2O_3$ and plays a key role in suppressing the magnetic long range ordering temperature and exposing a large phase space for the paramagnetic Mott metal-insulator transition to occur.

cond-mat.str-el↗

arXiv2019

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.

cond-mat.str-el↗

arXiv2018

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$_{11}$.

cond-mat.str-el↗

arXiv2018

Physical properties of the trigonal binary compound Nd$_2$O$_3$

We have studied the physical properties of Nd$_2$O$_3$ with neutron diffraction, inelastic neutron scattering, heat capacity, and magnetic susceptibility measurements. Nd$_2$O$_3$ crystallizes in a trigonal structure, with Nd$^{3+}$ ions surrounded by cages of 7 oxygen anions. The crystal field spectrum consists of four excitations spanning the energy range 3-60 meV. The refined eigenfunctions indicate XY-spins in the $ab$ plane. The Curie-Weiss temperature of $θ_{CW}=-23.7(1)$ K was determined from magnetic susceptibility measurements. Heat capacity measurements show a sharp peak at 550 mK and a broader feature centered near 1.5 K. Neutron diffraction measurements show that the 550 mK transition corresponds to long-range anti-ferromagnetic order implying a frustration index of $θ_{CW}/T_N\approx43$. These results indicate that Nd$_2$O$_3$ is a structurally and chemically simple model system for frustration caused by competing interactions with moments with predominate XY anisotropy.

cond-mat.str-el↗

arXiv2018

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.

cond-mat.str-el↗

arXiv2018

Origin of magnetic excitation gap in double perovskite Sr$_2$FeOsO$_6$

Sr$_2$FeOsO$_6$ is an insulating double perovskite compound which undergoes antiferromagnetic transitions at 140 K ($T_{N1}$) and 67 K ($T_{N2}$). To study the underlying electronic and magnetic interactions giving rise to this behavior we have performed inelastic neutron scattering (INS) and resonant inelastic x-ray scattering (RIXS) experiments on polycrystalline samples of Sr$_2$FeOsO$_6$. The INS data reveal that the spectrum of spin excitations remains ungapped below T$_{N1}$, however below T$_{N2}$ a gap of 6.8 meV develops. The RIXS data reveals splitting of the T$_{2g}$ multiplet consistent with that seen in other 5d$^3$ osmium based double perovskites. Together these results suggest that spin-orbit coupling is important for ground state selection in 3d-5d$^3$ double perovskite materials.

cond-mat.str-el↗

arXiv2017

Interplay of spin-orbit coupling and hybridization in Ca3LiOsO6 and Ca3LiRuO6

The electronic ground state of Ca3LiOsO6 was recently considered within an intermediate coupling regime that revealed J=3/2 spin-orbit entangled magnetic moments. Through inelastic neutron scattering and density functional theory we investigate the magnetic interactions and probe how the magnetism is influenced by the change in hierarchy of interactions as we move from Ca3LiOsO6 (5d3) to Ca3LiRuO6 (4d3). An alteration of the spin-gap and ordered local moment is observed, however the magnetic structure, Neel temperature and exchange interactions are unaltered. To explain this behavior it is necessary to include both spin-orbit coupling and hybridization, indicating the importance of an intermediate coupling approach when describing 5$d$ oxides.

cond-mat.str-el↗

arXiv2017

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.

cond-mat.str-el↗

arXiv2017

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.

cond-mat.str-el↗

arXiv2017

Excitations in the field-induced quantum spin liquid state of alpha-RuCl3

The Kitaev model on a honeycomb lattice predicts a paradigmatic quantum spin liquid (QSL) exhibiting Majorana Fermion excitations. The insight that Kitaev physics might be realized in practice has stimulated investigations of candidate materials, recently including alpha-RuCl3. In all the systems studied to date, non-Kitaev interactions induce magnetic order at low temperature. However, in-plane magnetic fields of roughly 8 Tesla suppress the long-range magnetic order in alpha-RuCl3 raising the intriguing possibility of a field-induced QSL exhibiting non-Abelian quasiparticle excitations. Here we present inelastic neutron scattering in alpha-RuCl3 in an applied magnetic field. At a field of 8 Tesla, the spin waves characteristic of the ordered state vanish throughout the Brillouin zone. The remaining single dominant feature of the response is a broad continuum centered at the Gamma point, previously identified as a signature of fractionalized excitations. This provides compelling evidence that a field-induced QSL state has been achieved.

cond-mat.mtrl-sci↗

arXiv2016

Strong anisotropy within a Heisenberg model in the J=1/2 insulating state of Sr2Ir0.8Ru0.2O4

The dispersive magnetic excitations in Sr2IrO4 have previously been well described within an isospin-1/2 Heisenberg model on a square lattice that revealed parallels with La2CuO4. Here we investigate the inelastic spectra of Sr2Ir0.8Ru0.2O4 with resonant inelastic x-ray scattering (RIXS) at the Ir L3-edge. The results are well described using linear spin-wave theory within a similar Heisenberg model applicable to Sr2IrO4, however the disorder induced by the substitution of 20% Ir4+ ions for Ru4+ removes longer range exchange interactions. A large spin-gap (40 meV) is measured indicating strong anisotropy from spin-orbit coupling that is manifest due to the altered magnetic structure in Sr2Ir0.8Ru0.2O4 with c-axis aligned moments compared to the basal plane moments in the parent. Collectively the results indicate the robustness of a Heisenberg model description even when the magnetic structure is altered and the J=1/2 moments diluted.

cond-mat.str-el↗

arXiv2016

Spin-orbit coupling controlled $J=3/2$ electronic ground state in 5$d^{3}$ oxides

Entanglement of spin and orbital degrees of freedom drives the formation of novel quantum and topological physical states. Discovering new spin-orbit entangled ground states and emergent phases of matter requires both experimentally probing the relevant energy scales and applying suitable theoretical models. Here we report resonant inelastic x-ray scattering measurements of the transition metal oxides Ca$_3$LiOsO$_6$ and Ba$_2$YOsO$_6$. We invoke an intermediate coupling approach that incorporates both spin-orbit coupling and electron-electron interactions on an even footing and reveal the ground state of $5d^3$ based compounds, which has remained elusive in previously applied models, is a novel spin-orbit entangled J=3/2 electronic ground state. This work reveals the hidden diversity of spin-orbit controlled ground states in 5d systems and introduces a new arena in the search for spin-orbit controlled phases of matter.

cond-mat.str-el↗

arXiv2016

Spin-orbit coupling controlled ground state in Sr$_2$ScOsO$_6$

We report neutron scattering experiments which reveal a large spin gap in the magnetic excitation spectrum of weakly-monoclinic double perovskite Sr2ScOsO6. The spin gap is demonstrative of appreciable spin-orbit-induced anisotropy, despite nominally orbitally-quenched 5d3 Os5+ ions. The system is successfully modeled including nearest neighbor interactions in a Heisenberg Hamiltonian with exchange anisotropy. We find that the presence of the spin-orbit-induced anisotropy is essential for the realization of the type I antiferromagnetic ground state. This demonstrates that physics beyond the LS or JJ coupling limits plays an active role in determining the collective properties of 4d3 and 5d3 systems, and that theoretical treatments must include spin-orbit coupling.

cond-mat.str-el↗

arXiv2016

Low-temperature crystal and magnetic structure of $α$-RuCl3

Single crystals of the Kitaev spin-liquid candidate $α$-RuCl$_3$ have been studied to determine low-temperature bulk properties, structure and the magnetic ground state. Refinements of x-ray diffraction data show that the low temperature crystal structure is described by space group $C2/m$ with a nearly-perfect honeycomb lattice exhibiting less than 0.2 \% in-plane distortion. The as-grown single crystals exhibit only one sharp magnetic transition at $T_{N}$ = 7~K. The magnetic order below this temperature exhibits a propagation vector of $k$ = (0, 1, 1/3), which coincides with a 3-layer stacking of the $C2/m$ unit cells. Magnetic transitions at higher temperatures up to 14~K can be introduced by deformations of the crystal that result in regions in the crystal with a 2-layer stacking sequence. The best fit symmetry allowed magnetic structure of the as-grown crystals shows that the spins lie in the $ac$-plane, with a zigzag configuration in each honeycomb layer. The three layer repeat out-of-plane structure can be refined as a 120$^o$ spiral order or a collinear structure with spin direction 35$^o$ away from the $a$-axis. The collinear spin configuration yields a slightly better fit and also is physically preferred. The average ordered moment in either structure is less than 0.45(5) $μ_B$ per Ru$^{3+}$ ion.

cond-mat.str-el↗