arXiv subjects

Joseph A. M. Paddison

Publications and source records attributed to Joseph A. M. Paddison.

At least 19 recordsLinked to original sources

arXiv2026

Machine learning magnetic interactions from neutron powder diffraction data

Neutron diffraction is a versatile experimental technique capable of probing a material's magnetic properties. While diffraction is typically used to determine the magnetic structure of a material, magnetic diffuse scattering data from a diffraction experiment are also sensitive to the magnetic interactions in its Hamiltonian. However, accurately determining magnetic interaction parameters from neutron-scattering data involves an inverse scattering problem that is challenging to solve in general. Here, we investigate the effectiveness of a machine learning approach to predict the interaction parameters given magnetic diffuse-scattering data measured on powder samples, for a comprehensive survey of isotropic interactions on eight high-symmetry lattices. Across all lattices we considered, the machine-learning approach estimates the interaction parameters with high (~2%) accuracy, while avoiding the issue of false minima that is encountered with non-linear least squares refinement. Our results highlight that powder diffuse-scattering data can provide a compact "fingerprint" of the magnetic interactions for many materials.

cond-mat.str-el↗

arXiv2026

Disorder-induced proximate quantum spin ice phase in Pr2Sn2O7

Magnetic pyrochlores with non-Kramers rare-earth ions provide a platform for exploring emergent gauge physics and quantum spin-ice behavior, yet the influence of structural disorder on their ground states remains insufficiently understood. Here we combine bulk characterization and single-crystal neutron-scattering measurements to investigate the non-Kramers pyrochlore Pr2Sn2O7. At temperatures below ~1 K, the system exhibits key hallmarks of quantum spin-ice physics, including anisotropic spin-ice correlations and two distinct dynamical timescales. Upon further cooling, however, we observe a complete spin-freezing transition at T_f ~ 0.15 K, accompanied by recovery of the full nuclear Schottky anomaly, the emergence of a gapped magnetic excitation, and the development of incipient (100) magnetic correlations. Comparison with related Pr-based pyrochlores places Pr2Sn2O7 near the spin-frozen boundary of a disorder-perturbed phase diagram. These results establish a disorder-driven framework for the evolution of quantum spin-ice behavior into frozen ground states, revealing how signatures of a proximate quantum spin liquid can persist despite disorder-induced spin freezing in non-Kramers pyrochlores.

cond-mat.str-el↗

arXiv2026

Dynamical moment fragmentation in the all-in all-out pyrochlore Nd2Sn2O7

We report single-crystal neutron spectroscopy and bulk characterization on hydrothermally grown Nd2Sn2O7, revealing a dynamical moment fragmentation embedded within the all-in-all-out ordered state. The spectra show a nearly flat band with pinch-point-like momentum dependence, accompanied by dispersive branches that generate half-moon features across multiple Brillouin zones. These defining signatures are captured quantitatively by a minimal dipolar-octupolar spin Hamiltonian, demonstrating excellent agreement between experiment and theory. The higher flat-mode energy helps account for the absence of dynamical interference in prior muon spin relaxation (muSR) studies, while the lack of any photon-like excitation imposes strict constraints on the proposed Coulombic antiferromagnet scenario. Our results extend dynamical moment fragmentation to Nd2Sn2O7 and identify it as a clean, tractable platform for quantitative exploration of emergent gauge-field physics and multipolar spin-wave dynamics in frustrated magnets.

cond-mat.str-el↗

arXiv2026

A Fermi Surface Driven Spiral Spin Liquid

EuAg$_4$Sb$_2$ is a model material to study the interplay of electronic and spin texture degrees of freedom, exhibiting numerous multi-$q$ magnetic textures coupled with the electronic properties. It is generally understood that some combination of conduction-electron mediated interactions, frustration, and higher order interactions are responsible for complex incommensurate spin textures in centrosymmetric lanthanide materials. Here, we refine an effective model of the magnetic interactions in EuAg$_4$Sb$_2$ through measurements of diffuse magnetic neutron scattering above the ordering temperature. These diffuse measurements reveal a ring of fluctuating spin modulations that reflects a manifold of nearly degenerate propagation vectors known as a spiral spin liquid (SSL). We further identify that this approximate $U$(1) symmetric SSL emerges from magnetic interactions mediated by a quasi-2D hole pocket and exhibits critical scaling of the spatial correlations. Further, Monte Carlo simulations reveal excellent agreement with experiment and provide a comprehensive understanding of the phase diagram. This study emphasizes the connection between the rich spin textures in this material, the electronic structure, and spin liquidity$\unicode{x2014}$uncovering new insights into design principles for nano-scale spin texture materials with advantageous intertwined electronic, magnetic, and topological properties, and new mechanisms for generating the physics of spiral spin liquids.

cond-mat.str-el↗

arXiv2025

Skyrmion and Meron Crystals in Intermetallic Gd$_3$Ru$_4$Al$_{12}$: Microscopic Model Insights into Chiral Phases

Topological spin textures in frustrated intermetallics hold great promise for spintronics applications. However, understanding their origin and properties remains a significant challenge due to competing and often long-range interactions mediated by conduction electrons. Here, by combining neutron scattering experiments with theoretical modeling via unprecedented multi-target fits that further incorporate the ferromagnentic resonance data and magnetization curve, we construct a realistic microscopic model for the prototypical intermetallic skyrmion host \text{Gd}$_3$\text{Ru}$_4$\text{Al}$_{12}$. Beyond magnetic frustration, we identify the competition between dipolar interactions and easy-plane single-ion anisotropy as a key ingredient for stabilizing the rich chiral magnetic phases observed in this compound -- including a hexagonal skyrmion crystal and two distinct meron crystals. Remarkably, the meron crystal in lower field is revealed to be commensurate with the underlying lattice, and its unique three-meron-one-antimeron spin texture is verified by the polarized x-ray diffraction data. At elevated temperatures, the short-range spin correlations in \text{Gd}$_3$\text{Ru}$_4$\text{Al}$_{12}$ are well described by a codimension-two spiral spin-liquid. Perturbations from staggered Dzyaloshinskii-Moriya interactions give rise to chiral fluctuations that account for the temperature and field dependence of the anomalous Hall response. Our results highlight the unique power of neutron scattering, especially when combined with complementary experimental techniques, to unravel complex magnetic phase transitions and provide new insights into the rich variety of topological spin textures in frustrated systems.

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arXiv2025

Kitaev interactions of the spin-orbit coupled magnet UO2

Uranium dioxide, UO$_2$, is a canonical example of a magnetic material with strong spin-orbit coupling. Here, we present a study of the magnetic diffuse scattering measured on a polycrystalline sample of UO$_2$, which we interpret in terms of its magnetic interactions between U$^{4+}$ magnetic moments. By refining values of the magnetic interaction parameters to magnetic diffuse-scattering data measured above the magnetic ordering transition temperature, we show that the dominant magnetic coupling in UO$_2$ is a bond-dependent interaction analogous to the Kitaev model of honeycomb magnets. We compare our experimental results with published theoretical predictions and experimental measurements of the magnetic excitation spectrum. Our results suggest that magnetic materials with $f$-electron magnetic ions, particularly actinides, may be promising candidates for realising Kitaev magnetism, and highlight the role that magnetic diffuse-scattering data can play in identifying such materials.

cond-mat.str-el↗

arXiv2025

A planning tool for neutron powder diffraction experiments

We introduce a computer program to simulate the results of neutron powder-diffraction experiments at the High Flux Isotope Reactor at Oak Ridge National Laboratory. The program is freely available as a web application at http://addie.ornl.gov/hfirestimate, and is designed to be straightforward to use for researchers who are new to neutron diffraction. The input includes the crystal structure of the proposed sample, the sample mass, and the instrument configuration. The results include a plot of the simulated data -- including realistic estimates of background and the error bars due to counting statistics -- and suggestions of how to resolve potential problems with the experiment. Here, we explain the design and implementation of this program and demonstrate its performance using comparisons of simulated and experimental data. We hope that this program will enable researchers to plan neutron-scattering experiments more effectively, increasing the likelihood of successful experiments and improving the productivity of neutron-diffraction research.

physics.ins-det↗

arXiv2025

Stability frontiers in the AM$_6$X$_6$ kagome metals: The LnNb$_6$Sn$_6$ (Ln:Ce-Lu,Y) family and density-wave transition in LuNb$_6$Sn$_6$

The kagome motif is a versatile platform for condensed matter physics, hosting rich interactions between magnetic, electronic, and structural degrees of freedom. In recent years, the discovery of a charge density wave (CDW) in the AV$_3$Sb$_5$ superconductors and structurally-derived bond density waves in FeGe and ScV$_6$Sn$_6$ have stoked the search for new kagome platforms broadly exhibiting density wave (DW) transitions. In this work, we evaluate the known AM$_6$X$_6$ chemistries and construct a stability diagram that summarizes the structural relationships between the $\approx$125 member family. Subsequently we introduce our discovery of the broader LnNb$_6$Sn$_6$ (Ln:Ce-Nd,Sm,Gd-Tm,Lu,Y) family of kagome metals and an analogous DW transition in LuNb$_6$Sn$_6$. Our X-ray scattering measurements clearly indicate a (1/3, 1/3, 1/3) ordering wave vector ($\sqrt{3}\times\sqrt{3}\times3$ superlattice) and diffuse scattering on half-integer $L$-planes. Our analysis of the structural data supports the ``rattling mode'' DW model proposed for ScV$_6$Sn$_6$ and paints a detailed picture of the steric interactions between the rare-earth filler element and the host Nb-Sn kagome scaffolding. We also provide a broad survey of the magnetic properties within the HfFe$_6$Ge$_6$-type LnNb$_6$Sn$_6$ members, revealing a number of complex antiferromagnetic and metamagnetic transitions throughout the family. This work integrates our new LnNb$_6$Sn$_6$ series of compounds into the broader AM$_6$X$_6$ family, providing new material platforms and forging a new route forward at the frontier of kagome metal research.

cond-mat.str-el↗

arXiv2024

ASb3Mn9O19 (A = K or Rb): New Mn-Based Two-Dimensional Magnetoplumbites with Geometric and Magnetic Frustration

Magnetoplumbites are one of the most broadly studied families of hexagonal ferrites, typically with high magnetic ordering temperatures, making them excellent candidates for permanent magnets. However, magnetic frustration was rarely observed in magnetoplumbites. Herein, we report the discovery, synthesis and characterization of the first Mn-based magnetoplumbite, as well as the first magnetoplumbite involving pnictogens (Sb), ASb3Mn9O19 (A = K or Rb). The Mn3+ (S = 2) cations, further confirmed by DC magnetic susceptibility and X-ray photoelectron spectroscopy, construct three geometrically frustrated sublattices, including Kagome, triangular and puckered honeycomb lattices. Magnetic properties measurements revealed strong antiferromagnetic spin-spin coupling as well as multiple low-temperature magnetic features. Heat capacity data did not show any prominent lambda-anomaly, suggesting minimal associated magnetic entropy. Moreover, neutron powder diffraction implied the absence of long-range magnetic ordering in KSb3Mn9O19 down to 3 K. However, several magnetic peaks were observed in RbSb3Mn9O19 at 3 K, corresponding to an incommensurate magnetic structure. Interestingly, strong diffuse scattering was seen in the neutron powder diffraction patterns of both compounds at low angles, and was analyzed by reverse Monte Carlo refinements, indicating short-range spin ordering related to frustrated magnetism as well as two-dimensional magnetic correlations in ASb3Mn9O19 (A = K or Rb).

cond-mat.mtrl-sci↗

arXiv2024

Absolute intensity normalisation of powder neutron scattering data

An important property of neutron scattering data is that they can be normalised in absolute intensity units. In practice, however, such normalisation is often not performed, since it can be time-consuming and subject to systematic uncertainties. Here, a straightforward approach is presented for absolute intensity normalisation of neutron scattering data from polycrystalline samples. This approach uses the intensity scale factor obtained from a Rietveld refinement to normalise the data to the nuclear Bragg profile of the sample. Factors to convert the Rietveld scale factor into an absolute normalisation factor are tabulated for constant-wavelength and time-of-flight data refined using the popular programs Fullprof and GSAS-II. An example of the application of this method to experimental data is presented. Advantages, disadvantages, and extensions of this approach to spectroscopic data are discussed.

cond-mat.mtrl-sci↗

arXiv2024

Frustrated Ising charge correlations in the kagome metal ScV$_6$Sn$_6$

Here we resolve the real-space nature of the high-temperature, short-range charge correlations in the kagome metal ScV$_6$Sn$_6$. Diffuse scattering appears along a frustrated wave vector $\textbf{q}_H=(\frac{1}{3},\frac{1}{3},\frac{1}{2})$ at temperatures far exceeding the charge order transition $T_{CO}=92~\mathrm{K}$, preempting long-range charge order with wave vectors along $\textbf{q}_{\bar{K}}=(\frac{1}{3},\frac{1}{3},\frac{1}{3})$. Using a combination of real space and reciprocal space analysis, we resolve the nature of the interactions between the primary out-of-plane Sc-Sn chain instability and the secondary strain-mediated distortion of the in-plane V kagome network. A minimal model of the diffuse scattering data reveals a high-temperature, short-ranged "zig-zag" phase of in-plane correlations that maps to a frustrated triangular lattice Ising model with antiferromagnetic interactions and provides a real-space understanding of the origin of frustrated charge order in this material.

cond-mat.str-el↗

arXiv2024

Anomalous continuum scattering and higher-order van Hove singularity in the strongly anisotropic S = 1/2 triangular lattice antiferromagnet

The S = 1/2 triangular lattice antiferromagnet (TLAF) is a paradigmatic example of frustrated quantum magnetism. An ongoing challenge involves understanding the influence of exchange anisotropy on the collective behavior within such systems. Using inelastic neutron scattering (INS) and advanced calculation techniques, we have studied the low and high-temperature spin dynamics of Ba2La2CoTe2O12 (BLCTO): a Co2+-based Jeff = 1/2 TLAF that exhibits 120° order below TN = 3.26 K. We determined the spin Hamiltonian by fitting the energy-resolved paramagnetic excitations measured at T > TN, revealing exceptionally strong easy-plane XXZ anisotropy. Below TN, the excitation spectrum exhibits a high energy continuum having a larger spectral weight than the single-magnon modes, suggesting a scenario characterized by a spinon confinement length that markedly exceeds the lattice spacing. We conjecture that this phenomenon arises from the proximity to a quantum melting point, even under strong easy-plane XXZ anisotropy. Finally, we highlight characteristic flat features in the excitation spectrum, which are connected to higher-order van Hove singularities in the magnon dispersion directly induced by easy-plane XXZ anisotropy. Our results provide a rare experimental insight into the nature of highly anisotropic S = 1/2 TLAFs between the Heisenberg and XY limits.

cond-mat.str-el↗

arXiv2024

Discovering classical spin liquids by topological search of high symmetry nets

Spin liquids are a paradigmatic example of a non-trivial state of matter, and the search for new spin liquids is a key direction of physics, chemistry, and materials science. Geometric frustration -- where the geometry of the net that the spins occupy precludes the generation of a simple ordered state -- is a particularly fruitful way to generate these intrinsically disordered states. A particular focus has been on a handful of high symmetry nets. There are, however, many three-dimensional nets, each of which has the potential to form unique states. In this paper, we investigate the high symmetry nets -- those which are both node- and edge-transitive -- for the simplest possible interaction sets: nearest-neighbor couplings of antiferromagnetic Heisenberg and Ising spins. While the well-known crs (pyrochlore) net is the only nearest-neighbor Heisenberg antiferromagnet which does not order, we identify two new frustrated nets (lcx and thp) that possess finite temperature Heisenberg spin-liquid states with strongly suppressed magnetic ordering and non-collinear ground states. With Ising spins, we identify three new classical spin liquids that do not order down to $T/J = 0.01$. We highlight materials that contain these high symmetry nets, and which could, if substituted with appropriate magnetic ions, potentially host these unusual states. Our systematic survey will guide searches for novel magnetic phases.

cond-mat.str-el↗

arXiv2024

MnRhBi3: A Cleavable Antiferromagnetic Metal

Cleavable metallic antiferromagnets may be of use for low-dissipation spintronic devices; however, few are currently known. Here we present orthorhombic MnRhBi3 as one such compound and present a thorough study of its physical properties. Exfoliation is demonstrated experimentally, and the cleavage energy and electronic structure are examined by density functional theory calculations. It is concluded that MnRhBi3 is a van der Waals layered material that cleaves easily between neighboring Bi layers, and that the Bi atoms have lone pairs extending into the van der Waals gaps. A series of four phase transitions are observed below room temperature, and neutron diffraction shows that at least two of the transitions involve the formation of antiferromagnetic order. Anomalous thermal expansion points to a crystallographic phase transition and/or strong magnetoelastic coupling. This work reveals a complex phase evolution in MnRhBi3 and establishes this cleavable antiferromagnetic metal as an interesting material for studying the interplay of structure, magnetism, and transport in the bulk and ultrathin limits as well as the role of lone pair electrons in interface chemistry and proximity effects in van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2024

Spin Dynamics of the Centrosymmetric Skyrmion Material GdRu2Si2

Magnetic skyrmion crystals are traditionally associated with non-centrosymmetric crystal structures; however, it has been demonstrated that skyrmion crystals can be stabilized by competing interactions in centrosymmetric crystals. To understand and optimize the physical responses associated with topologically-nontrivial skyrmion textures, it is important to quantify their magnetic interactions by comparing theoretical predictions with spectroscopic data. Here, we present neutron diffraction and spectroscopy data on the centrosymmetric skyrmion material GdRu$_2$Si$_2$, and show that the key spectroscopic features can be explained by the magnetic interactions calculated using density-functional theory calculations. We further show that the recently-proposed 2-$\mathbf{q}$ "topological spin stripe" structure yields better agreement with our data than a 1-$\mathbf{q}$ helical structure, and identify how the magnetic structure evolves with temperature.

cond-mat.str-el↗

arXiv2023

Revisiting spin ice physics in the ferromagnetic Ising pyrochlore Pr$_2$Sn$_2$O$_7$

Pyrochlore materials are characterized by their hallmark network of corner-sharing rare-earth tetrahedra, which can produce a wide array of complex magnetic ground states. Ferromagnetic Ising pyrochlores often obey the "two-in-two-out" spin ice rules, which can lead to a highly-degenerate spin structure. Large moment systems, such as Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$, tend to host a classical spin ice state with low-temperature spin freezing and emergent magnetic monopoles. Systems with smaller effective moments, such as Pr$^{3+}$-based pyrochlores, have been proposed as excellent candidates for hosting a "quantum spin ice" characterized by entanglement and a slew of exotic quasiparticle excitations. However, experimental evidence for a quantum spin ice state has remained elusive. Here, we show that the low-temperature magnetic properties of Pr$_2$Sn$_2$O$_7$ satisfy several important criteria for continued consideration as a quantum spin ice. We find that Pr$_2$Sn$_2$O$_7$ exhibits a partially spin-frozen ground state with a large volume fraction of dynamic magnetism. Our comprehensive bulk characterization and neutron scattering measurements enable us to map out the magnetic field-temperature phase diagram, producing results consistent with expectations for a ferromagnetic Ising pyrochlore. We identify key hallmarks of spin ice physics, and show that the application of small magnetic fields ($μ_0 H_c \sim$0.75T) suppresses the spin ice state and induces a long-range ordered magnetic structure. Together, our work clarifies the current state of Pr$_2$Sn$_2$O$_7$ and encourages future studies aimed at exploring the potential for a quantum spin ice ground state in this system.

cond-mat.str-el↗

arXiv2023

Structure, spin correlations and magnetism of the $S = 1/2$ square-lattice antiferromagnet Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ ($0 \leq x \leq 1$)

Quantum spin liquids are highly entangled magnetic states with exotic properties. The $S = 1/2$ square-lattice Heisenberg model is one of the foundational models in frustrated magnetism with a predicted, but never observed, quantum spin liquid state. Isostructural double perovskites Sr$_2$CuTeO$_6$ and Sr$_2$CuWO$_6$ are physical realizations of this model, but have distinctly different types magnetic order and interactions due to a $d^{10}/d^0$ effect. Long-range magnetic order is suppressed in the solid solution Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ in a wide region of $x = 0.05-0.6$, where the ground state has been proposed to be a disorder-induced spin liquid. Here we show that the spin-liquid-like $x = 0.2$ and $x = 0.5$ samples have distinctly different local spin correlations, which suggests they have different ground states. Furthermore, the previously ignored interlayer coupling between the square-planes is likely to play a role in the suppression of magnetic order on the W-rich side at $x \approx 0.6$. These results highlight the complex magnetism of Sr$_2$CuTe$_{1-x}$W$_x$O$_6$ and hint at a new quantum critical point at $x \approx 0.3$.

cond-mat.str-el↗

arXiv2023

Multiple Incommensurate Magnetic States in the Kagome Antiferromagnet Na2Mn3Cl8

The kagome lattice can host exotic magnetic phases arising from frustrated and competing magnetic interactions. However, relatively few insulating kagome materials exhibit incommensurate magnetic ordering. Here, we present a study of the magnetic structures and interactions of antiferromagnetic Na$_2$Mn$_3$Cl$_8$ with an undistorted Mn$^{2+}$ kagome network. Using neutron-diffraction and bulk magnetic measurements, we show that Na$_2$Mn$_3$Cl$_8$ hosts two different incommensurate magnetic states, which develop at $T_{N1} = 1.6$ K and $T_{N2} = 0.6$ K. Magnetic Rietveld refinements indicate magnetic propagation vectors of the form $\mathbf{q} = (q_{x},q_{y},\frac{3}{2})$, and our neutron-diffraction data can be well described by cycloidal magnetic structures. By optimizing exchange parameters against magnetic diffuse-scattering data, we show that the spin Hamiltonian contains ferromagnetic nearest-neighbor and antiferromagnetic third-neighbor Heisenberg interactions, with a significant contribution from long-ranged dipolar coupling. This experimentally-determined interaction model is compared with density-functional-theory simulations. Using classical Monte Carlo simulations, we show that these competing interactions explain the experimental observation of multiple incommensurate magnetic phases and may stabilize multi-$\mathbf{q}$ states. Our results expand the known range of magnetic behavior on the kagome lattice.

cond-mat.str-el↗