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E. M. Smith

Publications and source records attributed to E. M. Smith.

15 recordsLinked to original sources
arXiv2026

Observation of Dipolar Spin-ice--like Correlations in the Quantum Spin Ice Candidate Ce$_2$Sn$_2$O$_7$

We report diffuse scattering measurements on the dipolar-octupolar pyrochlore, Ce$_2$Sn$_2$O$_7$, to elucidate its magnetic correlations within the correlated paramagnetic regime above its ordering temperature, $\mathrm{T_N}\sim 40~$mK. The magnetic transition at $\mathrm{T_N}$, observed in recent specific heat measurements, has been interpreted within the nearest-neighbor XYZ model as a transition into an all-in-all-out (AIAO) magnetic order. However, the observed diffuse scattering above $\mathrm{T_N}$ argues against an AIAO magnetic order by exhibiting $no$ short-range order at the AIAO wave-vectors, inconsistent with the nearest neighbor model. Instead, the observed diffuse scattering strongly resembles that observed in classical dipolar spin ice, Dy$_2$Ti$_2$O$_7$, and suggests the presence of short-range correlated structures such as chains, or clusters in the low energy manifold of Ce$_2$Sn$_2$O$_7$, favored by further neighbor interactions. We discuss how chain-like states qualitatively account for the observed H-T phase diagram under a [1,1,0]-field.

cond-mat.str-el↗
arXiv2026

Zero-Field Long Range Order at $T \sim 40$ mK in the Proximate Quantum Spin Ice Ce$_2$Sn$_2$O$_7$ and Phase Diagram for Magnetic Fields Along [1,1,0]

The Ce$^{3+}$ pseudospin-1/2 degrees of freedom in the pyrochlore magnets Ce$_2$X$_2$O$_7$, with $X$ = Zr, Hf, or Sn, possess dipole-octupole character. The XYZ nearest-neighbor model Hamiltonians which have successfully described their properties make them attractive candidates for quantum spin ice ground states. We report new heat capacity measurements to very low temperatures on a high-quality single crystal of Ce$_2$Sn$_2$O$_7$ grown by hydrothermal techniques. Our zero-field measurements uncover a clear first order transition to long-ranged order at $T \sim 0.04$ K, well below the downturn in the broader Schottky-like anomaly that is a common feature in the zero-field heat capacity for cerium pyrochlores. This observation settles the debate as to whether Ce$_2$Sn$_2$O$_7$ possesses a QSI ground state in zero field - it does not. However, we also find compelling evidence suggesting that spin ice physics is nearby, and remains relevant to Ce$_2$Sn$_2$O$_7$. Application of a magnetic field along the $[1,1,0]$ direction leads to an evolution of this peak to a weak anomaly at higher temperature more characteristic of a continuous, mean field transition. At higher fields along $[1,1,0]$, the Schottky-like anomaly bifurcates similar to expectations for independent polarized $α$ and orthogonal $β$ chains in classical spin ice. These new experimental results demonstrate richness to the phase diagram for Ce-based pyrochlores.

cond-mat.str-el↗
arXiv2026

Proximate Spin Liquid Ground State Arising from Competing Stripy and 120$^{\circ}$ Spin Correlations in the Triangular Quantum Antiferromagnet ErMgGaO$_4$

ErMgGaO$_4$ is a quantum antiferromagnet wherein the pseudospin-1/2 degrees of freedom of Er$^{3+}$ decorate two-dimensional triangular planes separated by disordered non-magnetic bilayers of Mg$^{2+}$ and Ga$^{3+}$. Unlike its sister compound, YbMgGaO$_4$, our powder ErMgGaO$_4$ sample shows a clear spin glass transition near $T_g \sim 2.5$~K, about 1/6 of its Curie-Weiss temperature. We have carried out new inelastic neutron scattering measurements on these powder ErMgGaO$_4$ samples. At high energies, we observed crystalline electric field (CEF) transitions within the $J=15/2$ multiplet of Er$^{3+}$, but with the first excited CEF level sufficiently low in energy ($\sim$ 3~meV) so as to allow the possibility that virtual CEF transitions influence the exchange couplings. At E=0, we observe diffuse elastic scattering which is analysed using Warren lineshapes appropriate for two dimensional correlations. This reveals dominant 2D stripy correlations below $T_g$, coexisting with 2D 120$^\circ$-type correlations that persist above $T_g$. At low temperatures, the low energy inelastic component of the scattering shows a continuum with bandwidth of $\sim$ 0.8~meV. This dynamic magnetic spectral weight can be modeled at all $Q$, energies, and temperatures as the sum of high energy and low energy damped harmonic oscillators (DHO), with the high energy DHO defining the bandwidth of $\sim$ 0.8~meV. We use linear spin wave theory to model this inelastic scattering and to estimate its spin Hamiltonian parameters in terms of a $J_1-J_2-Δ$ model on the triangular lattice. This gives a good description of the low lying spectral weight for ErMgGaO4, and allows us to place it on the theoretical $J_1-J_2-Δ$ phase diagram with $\frac{J_1}{J_2}=0.13 \pm 0.03$ and $Δ=0.4 \pm 0.1$, which is close to the expected quantum phase boundary between the spin liquid and the stripy ordered phases.

cond-mat.str-el↗
arXiv2025

Two-Peak Heat Capacity Accounts for $R\ln(2)$ Entropy and Ground State Access in the Dipole-Octupole Pyrochlore Ce$_2$Hf$_2$O$_7$

Magnetic heat capacity measurements of a high-quality single crystal of the dipole-octupole pyrochlore Ce$_2$Hf$_2$O$_7$ down to a temperature of $T = 0.02$ K are reported. These show a two-peaked structure, with a Schottky-like peak at $T_1 \sim 0.065$ K, similar to what is observed in its sister Ce-pyrochlores Ce$_2$Zr$_2$O$_7$ and Ce$_2$Sn$_2$O$_7$. However, a second sharper peak is observed at $T_2 \sim 0.025$ K, signifying the entrance to the ground state. The ground state appears to have gapped excitations, as even the most abrupt extrapolation to $C_P=0$ at $T = 0$ K fully accounts for the $R\ln(2)$ entropy associated with the pseudospin-1/2 doublet for Ce$^{3+}$ in this environment. The ground state could be conventionally ordered, although theory predicts a much larger anomaly in $C_P$ at much higher temperatures than the measured $T_2$ for expectations from an all-in all-out ground state of the XYZ Hamiltonian for Ce$_2$Hf$_2$O$_7$. The sharp low-temperature peak could also signify a cross-over from a classical spin liquid to a quantum spin liquid (QSL). For both scenarios, comparison of the measured $C_P$ with NLC calculations suggests that weak interactions beyond the nearest-neighbor XYZ Hamiltonian become relevant below $T \sim 0.25$ K. The diffuse magnetic neutron scattering observed from Ce$_2$Hf$_2$O$_7$ at low temperatures between $T_2$ and $T_1$ resembles that observed from Ce$_2$Zr$_2$O$_7$, which is well established as a $π$-flux quantum spin ice (QSI). Together with the peak in the heat capacity at $T_2$, this diffuse scattering from Ce$_2$Hf$_2$O$_7$ is suggestive of a classical spin liquid regime above $T_2$ that is distinct from the zero-entropy quantum ground state below $T_2$.

cond-mat.str-el↗
arXiv2025

Single Crystal Diffuse Neutron Scattering Study of the Dipole-Octupole Quantum Spin Ice Candidate Ce$_2$Zr$_2$O$_7$: No Apparent Octupolar Correlations Above $T = 0.05$ K

The insulating magnetic pyrochlore Ce$_2$Zr$_2$O$_7$ has gained attention as a quantum spin ice candidate with dipole-octupole character arising from the crystal electric field ground state doublet for the Ce$^{3+}$ ion. This permits both spin ice phases based on magnetic dipoles and those based on more-exotic octupoles. We report low-temperature neutron diffraction measurements on single crystal Ce$_2$Zr$_2$O$_7$ with $Q$-coverage both at low $Q$ where the magnetic form factor for dipoles is near maximal and at high $Q$ where the magnetic form factor for Ce$^{3+}$ octupoles is near maximal. This study was motivated by recent powder neutron diffraction studies of other Ce-based dipole-octupole pyrochlores, Ce$_2$Sn$_2$O$_7$ and Ce$_2$Hf$_2$O$_7$, which each showed temperature-dependent diffuse diffraction at high $Q$ that was interpreted as arising from octupolar correlations. Our measurements use an optimized single crystal diffuse scattering instrument that allows us to screen against strong Bragg scattering from Ce$_2$Zr$_2$O$_7$. The temperature-difference neutron diffraction reveals a low-$Q$ peak consistent with dipolar spin ice correlations reported in previous work, and an alternation between positive and negative net intensity at higher $Q$. These features are consistent with our numerical-linked-cluster calculations using pseudospin interaction parameters previously reported for Ce$_2$Zr$_2$O$_7$, Ce$_2$Sn$_2$O$_7$, and Ce$_2$Hf$_2$O$_7$. Importantly, neither the measured data nor any of the NLC calculations show evidence for increased scattering at high $Q$ resulting from octupolar correlations. We conclude that at the lowest attainable temperature for our measurements ($T = 0.05$ K), scattering from octupolar correlations in Ce$_2$Zr$_2$O$_7$ is not present in the neutron diffraction signal on the level of our observation threshold of ~ 0.1 % of the low-$Q$ dipole scattering.

cond-mat.str-el↗
arXiv2024

Dipolar spin ice regime proximate to an all-in-all-out Néel ground state in the dipolar-octupolar pyrochlore Ce$_2$Sn$_2$O$_7$

The dipolar-octupolar (DO) pyrochlores, R$_2$M$_2$O$_7$ (R = Ce, Sm, Nd), are key players in the search for realizable novel quantum spin liquid (QSL) states as a large parameter space within the DO pyrochlore phase diagram is theorized to host QSL states of both dipolar and octupolar nature. New single crystals and powders of Ce$_2$Sn$_2$O$_7$, synthesized by hydrothermal techniques, present an opportunity for a new characterization of the exchange parameters in Ce$_2$Sn$_2$O$_7$ using the near-neighbor $XYZ$ model Hamiltonian associated with DO pyrochlores. Utilizing quantum numerical linked cluster expansion fits to heat capacity and magnetic susceptibility measurements, and classical Monte Carlo calculations to the diffuse neutron diffraction of the new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples, we place Ce$_2$Sn$_2$O$_7$'s ground state within the ordered dipolar all-in-all-out (AIAO) Néel phase, with quantum Monte Carlo calculations showing a transition to long-range order at temperatures below those accessed experimentally. Indeed, our new neutron diffraction measurements on the hydrothermally grown Ce$_2$Sn$_2$O$_7$ powders show a broad signal at low scattering wave vectors, reminiscent of a \textit{dipolar} spin ice, in striking contrast from previous powder neutron diffraction on samples grown from solid-state synthesis, which found diffuse scattering at high scattering wave vectors associated with magnetic {\it octupoles} and suggested an octupolar quantum spin ice state. We conclude that new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples host a finite-temperature proximate dipolar spin ice phase, above the expected transition to AIAO Néel order.

cond-mat.str-el↗
arXiv2023

$μ$SR Study of the Dipole-Octupole Quantum Spin Ice Candidate Ce$_2$Zr$_2$O$_7$

The Ce$^{3+}$ pseudospin-1/2 degrees of freedom in Ce$_2$Zr$_2$O$_7$ possess both dipolar and octupolar character which enables the possibility of novel quantum spin liquid ground states in this material. Here we report new muon spin relaxation and rotation ($μ$SR) measurements on single crystal samples of Ce$_2$Zr$_2$O$_7$ in zero magnetic field and in magnetic fields directed along the $[1,\bar{1},0]$ and $[1,1,1]$ crystallographic directions, and for magnetic fields directed both longitudinal and transverse to the direction of muon polarization. Our zero-field results show no signs of magnetic ordering or spin freezing, consistent with earlier zero-field $μ$SR measurements on a powder sample of Ce$_2$Zr$_2$O$_7$, and also with the expectations for a quantum spin ice. However, we measure a more gentle relaxation rate for Ce$_2$Zr$_2$O$_7$ in zero-field at low temperatures than was previously reported. This difference in relaxation rate is likely due to the low oxidation, and correspondingly, the high stoichiometry of our single crystal samples. Longitudinal field measurements confirm that the magnetic dipole moments in Ce$_2$Zr$_2$O$_7$ remain dynamic at $T = 0.1$ $\mathrm{K}$. For both $[1,\bar{1},0]$ and $[1,1,1]$ magnetic fields, our $μ$SR Knight shift measurements show a field-induced leveling off of the magnetic susceptibility at low temperature which is qualitatively consistent with corresponding calculations using the numerical-linked-cluster method in combination with recent estimates for the nearest-neighbour exchange parameters of Ce$_2$Zr$_2$O$_7$.

cond-mat.str-el↗
arXiv2023

Random Fields from Quenched Disorder in an Archetype for Correlated Electrons: the Parallel Spin Stripe Phase of La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ at the 1/8 Anomaly

The parallel stripe phase is remarkable both in its own right, and in relation to the other phases it co-exists with. Its inhomogeneous nature makes such states susceptible to random fields from quenched magnetic vacancies. We argue this is the case by introducing low concentrations of nonmagnetic Zn impurities (0-10%) into La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ (Nd-LSCO) with $x$ = 0.125 in single crystal form, well below the percolation threshold of $\sim$ 41% for two-dimensional (2D) square lattice. Elastic neutron scattering measurements on these crystals show clear magnetic quasi-Bragg peaks at all Zn dopings. While all the Zn-doped crystals display order parameters that merge into each other and the background at $\sim$ 68 K, the temperature dependence of the order parameter as a function of Zn concentration is drastically different. This result is consistent with meandering charge stripes within the parallel stripe phase, which are pinned in the presence of quenched magnetic vacancies. In turn it implies vacancies that preferentially occupy sites within the charge stripes, and hence that can be very effective at disrupting superconductivity in Nd-LSCO ($x$ = 0.125), and, by extension, in all systems exhibiting parallel stripes.

cond-mat.supr-con↗
arXiv2023

Quantum Spin Ice Response to a Magnetic Field in the Dipole-Octupole Pyrochlore Ce$_2$Zr$_2$O$_7$

We report new heat capacity measurements on single crystal Ce$_2$Zr$_2$O$_7$ down to $\sim$ 0.1 K in a magnetic field along the $[1,\bar{1}, 0]$ direction. These new measurements show that the broad hump in the zero-field heat capacity moves higher in temperature with increasing field strength and is split into two humps by the $[1,\bar{1}, 0]$ field at $\sim$ 2 T. These separate features are due to the decomposition of the pyrochlore lattice into effectively decoupled chains for fields in this direction: one set of chains ($α$-chains) is polarized by the field while the other ($β$-chains) remains free. Our theoretical modelling suggests that the $β$-chains are close to a critical state, with nearly-gapless excitations. We also report new elastic and inelastic neutron scattering measurements on single crystal Ce$_2$Zr$_2$O$_7$ in $[1, \bar{1}, 0]$ and $[0, 0, 1]$ magnetic fields at temperatures down to 0.03 K. The elastic scattering behaves consistently with the formation of independent chains for a $[1, \bar{1}, 0]$ field, while the $[0, 0, 1]$ field produces a single field-induced magnetic Bragg peak at $(0, 2, 0)$ and equivalent wavevectors, indicating a polarized spin ice for fields above $\sim$ 3 T. For both $[1, \bar{1}, 0]$ and $[0, 0, 1]$ fields, our inelastic neutron scattering results show an approximately-dispersionless continuum of scattering that increases in both energy and intensity with increasing field strength. By modelling the complete set of experimental data using numerical linked cluster and semiclassical molecular dynamics calculations, we demonstrate the dominantly multipolar nature of the exchange interactions in Ce$_2$Zr$_2$O$_7$ and the smallness of the parameter $θ$ which controls the mixing between dipolar and octupolar degrees of freedom. These results support previous estimates of the microscopic exchange parameters.

cond-mat.str-el↗
arXiv2023

Spin-orbital order and excitons in magnetoresistive HoBi

The magnetism of the rock-salt $fcc$ rare-earth monopnictide HoBi, a candidate topological material with extreme magnetoresistance, is investigated. From the Ho$^{3+}$ non-Kramers $J$=8 spin-orbital multiplet, the cubic crystal electric field yields six nearly degenerate low-energy levels. These constitute an anisotropic magnetic moment with a Jahn-Teller-like coupling to the lattice. In the cubic phase for $T>T_N~=~5.72(1)~K$, the paramagnetic neutron scattering is centered at $\mathbf{k}=(\frac{1}{2}\frac{1}{2}\frac{1}{2})$ and was fit to dominant antiferromagnetic interactions between Ho spins separated by $\{100\}$ and ferromagnetic interactions between spins displaced by $\{\frac{1}{2}\frac{1}{2}0\}$. For $T<T_N$, a type-II AFM long-range order with $\mathbf{k}=(\frac{1}{2}\frac{1}{2}\frac{1}{2})$ develops along with a tetragonal lattice distortion. While neutron diffraction from a multi-domain sample cannot unambiguously determine the spin orientation within a domain, the bulk magnetization, structural distortion, and our measurements of the magnetic excitations all show the easy axis coincides with the tetragonal axis. The weakly dispersive excitons for $T<T_N$ can be accounted for by a spin Hamiltonian that includes the crystal electric field and exchange interactions within the Random Phase Approximation.

cond-mat.str-el↗
arXiv2022

Reply to "Comment on: 'Case for a U(1)$_π$ Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore $\mathrm{Ce}_2\mathrm{Zr}_2\mathrm{O}_7$' "

In his comment [arXiv:2209.03235], S. W. Lovesey argues that our analysis of neutron scattering experiments performed on Ce$_2$Zr$_2$O$_7$ is invalid. Lovesey argues that we have not properly accounted for the higher-order multipolar contributions to the magnetic scattering and that our use of pseudospin-$1/2$ operators to describe the scattering is inappropriate. In this reply, we show that the multipolar corrections discussed by Lovesey only become significant at scattering wavevectors exceeding those accessed in our experiments. This in no way contradicts or undermines our work, which never claimed a direct observation of scattering from higher-order multipoles. We further show that Lovesey's objections to our use of pseudospins are unfounded, and that the pseudospin operators are able to describe all magnetic scattering processes at the energy scale of our experiments, far below the crystal field gap. Finally, we comment on certain assumptions in Lovesey's calculations of the scattering amplitude which are inconsistent with experiment.

cond-mat.str-el↗
arXiv2022

Skyrmion Alignment and Pinning Effects in a Disordered Multi-Phase Skyrmion Material Co8Zn8Mn4

Underlying disorder in skyrmion materials may both inhibit and facilitate skyrmion reorientations and changes in topology. The identification of these disorder-induced topologically active regimes is critical to realizing robust skyrmion spintronic implementations, yet few studies exist for disordered bulk samples. Here, we employ small-angle neutron scattering (SANS) and micromagnetic simulations to examine the influence of skyrmion order on skyrmion lattice formation, transition, and reorientation dynamics across the phase space of a disordered polycrystalline Co$_{8}$Zn$_{8}$Mn$_{4}$ bulk sample. Our measurements reveal a new disordered-to-ordered skyrmion square lattice transition pathway characterized by the novel promotion of four-fold order in SANS and accompanied by a change in topology of the system, reinforced through micromagnetic simulations. Pinning responses are observed to dominate skyrmion dynamics in the metastable triangular lattice phase, enhancing skyrmion stabilization through a remarkable and previously undetected skyrmion memory effect which reproduces previous ordering processes and persists in zero field. These results uncover the cooperative interplay of anisotropy and disorder in skyrmion formation and restructuring dynamics, establishing new tunable pathways for skyrmion manipulation.

cond-mat.mtrl-sci↗
arXiv2021

The case for a U(1)$_π$ Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore Ce$_2$Zr$_2$O$_7$

The Ce$^{3+}$ pseudospin-$\frac{1}{2}$ degrees of freedom in the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ are known to possess dipole-octupole (DO) character, making it a candidate for novel quantum spin liquid (QSL) ground states at low temperatures. We report new polarized neutron diffraction at low temperatures, as well as heat capacity ($C_p$) measurements on single crystal Ce$_2$Zr$_2$O$_7$. The former bears both similarities and differences from that measured in the canonical dipolar spin ice compound Ho$_2$Ti$_2$O$_7$, while the latter rises sharply at low temperatures, initially plateauing near 0.08 K, before falling off towards a high temperature zero beyond 3 K. Above $\sim$0.5 K, the $C_p$ data set can be fit to the results of a quantum numerical linked cluster (NLC) calculation, carried out to 4$^{\mathrm{th}}$ order, that allows estimates for the terms in the near-neighbour XYZ Hamiltonian expected for such DO pyrochlore systems. Fits of the same theory to the temperature dependence of the magnetic susceptibility and unpolarized neutron scattering complement this analysis. A comparison between the resulting best fit NLC calculation and the polarized neutron diffraction shows both agreement and discrepancies, mostly in the form of zone-boundary diffuse scattering in the non-spin flip channel, which are attributed to interactions beyond near-neighbours. The lack of an observed thermodynamic anomaly and the constraints on the near-neighbour XYZ Hamiltonian suggest that Ce$_2$Zr$_2$O$_7$ realizes a U(1)$_π$ QSL state at low temperatures, and one that likely resides near the boundary between dipolar and octupolar character.

cond-mat.str-el↗
arXiv2020

Characterization of a Disordered Above Room Temperature Skyrmion Material Co8Zn8Mn4

Topologically non trivial spin textures host great promise for future spintronic applications. Skyrmions in particular are of burgeoning interest owing to their nanometric size, topological protection, and high mobility via ultra-low current densities. It has been previously reported through magnetic susceptibility, microscopy, and scattering techniques that Co$_{8}$Zn$_{8}$Mn$_{4}$ forms an above room temperature triangular skyrmion lattice. Here we report the synthesis procedure and characterization of a polycrystalline Co$_{8}$Zn$_{8}$Mn$_{4}$ bulk sample. We employ powder x-ray diffraction, backscatter Laue diffraction, and neutron diffraction as characterization tools of the crystallinity of the samples, while magnetic susceptibility and Small Angle Neutron Scattering (SANS) measurements are performed to study the skyrmion phase. Magnetic susceptibility measurements show a dip anomaly in the magnetization curves which persists over a range of approximately 305 K- 315 K. SANS measurements reveal a rotationally disordered polydomain skymrion lattice. Applying a recently developed symmetry-breaking magnetic field sequence, we were able to orient and order the previously jammed state to yield the prototypical hexagonal diffraction patterns, with secondary diffraction rings.

cond-mat.mtrl-sci↗
arXiv2019

Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce$_2$Zr$_2$O$_7$

Neutron scattering measurements on the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ reveal an unusual crystal field splitting of its lowest $J$=5/2 multiplet, such that its ground state doublet is composed of m$_J$=$\pm$3/2, giving these doublets a dipole - octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with $θ_{CW}$=-0.4(2)K, leading to a naive expectation of an All-In, All-Out ordered state at low temperatures. Instead our low energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppressed scattering near |$\textbf{Q}$|=0, and no long range order at low temperatures. This is consistent with recent theory predicting symmetry enriched U(1) quantum spin liquids for such DO doublets decorating the pyrochlore lattice. Finally, we show that disorder, especially oxidation of powder samples, is important in Ce$_2$Zr$_2$O$_7$ and could play an important role in the low temperature behaviour of this material.

cond-mat.str-el↗