arXiv subjects

Stuart Calder

Publications and source records attributed to Stuart Calder.

At least 19 recordsLinked to original sources

arXiv2026

Local magnetic order in vacancy-disrupted spin ice Ho2TiO5

We investigate how local magnetic correlations evolve when the classical pyrochlore spin-ice Ho2Ti2O7 is transformed into the partially disordered stuffed compound Ho2TiO5. Neutron scattering measurements were analyzed using real-space magnetic pair distribution function, reciprocal-space reverse Monte Carlo, and half-polarized neutron powder diffraction methods to connect the average crystal structure with local magnetic correlations. Both compounds retain long-range $Fd-3m symmetry, but in Ho2TiO5 this average structure distorts locally through Ho-O, Ti-O and O-O bond-length disorder associated with partial Ho/Ti occupancy. Despite this disorder, half-polarized neutron powder diffraction shows that the Ho moments retain local <111> rangle Ising anisotropy and form spin-in/spin-out configurations on the tetrahedral network. In Ho2Ti2O7, real- and reciprocal-space analyses reveal a nearly ideal two-in/two-out spin-ice state at 0.3K, with 95% of tetrahedra satisfying the ice rule, followed by progressive thermal disordering on warming. In Ho2TiO5, most tetrahedra are magnetically incomplete because some tetrahedral vertices are occupied by nonmagnetic Ti rather than Ho; nevertheless, the dominant incomplete configurations are 2-in/1-out and 1-in/2-out, which are locally compatible with the ice rule if the missing Ho spin is restored. The single-ion <111> Ising anisotropy is therefore retained throughout, while the collective ice ordering is strongly disrupted: Ho2TiO5 is a vacancy-disrupted spin ice in which a local ice-rule tendency persists on a topologically incomplete magnetic network.

cond-mat.str-el↗

arXiv2026

Correlation-Driven Spin Reorientation via Competing Anisotropy Channels in CrPS4

We identify a correlation-driven mechanism for the temperature-induced spin reorientation in the quasi-one-dimensional van der Waals antiferromagnet CrPS4. Magnetic pair distribution function (mPDF) analysis resolves the local spin direction and shows that ferromagnetic intrachain correlations persist far above TN. Combining these correlations with a DFT-derived spin Hamiltonian reveals competing single-ion and exchange-anisotropy channels, with single-ion anisotropy remaining local while exchange anisotropy is renormalized as intersite correlations decay. This differential renormalization rotates the effective easy axis and captures the ordered-state canting. Above TN, the continued rotation beyond the model prediction delineates the limits of the dominant-chain approximation. These results establish mPDF-derived correlations as direct inputs to microscopic Hamiltonians and show how low-dimensional correlations can control magnetic anisotropy.

cond-mat.str-el↗

arXiv2026

Magnetic order and excitations in Ce$_3$TiBi$_5$ and Ce$_3$ZrBi$_5$

The R3MBi5 rare-earth intermetallics (R = rare earth, M = Ti, Zr, Sc) provide a versatile platform to explore how Kondo hybridization, RKKY exchange, magnetic frustration, and broken inversion symmetry may cooperate to generate unusual magnetic behavior. We present a comprehensive neutron scattering investigation of the magnetic structure, crystal electric field (CEF), and low-energy excitations in the locally noncentrosymmetric Kondo-lattice compounds Ce3TiBi5 and Ce3ZrBi5. Powder and single-crystal neutron diffraction reveals incommensurate cycloidal antiferromagnetic order in Ce3TiBi5 with propagation vector k = (0, 0, 0.388) and a reduced ordered moment of m = 0.53(3)$\mu_{B}$. Ce3ZrBi5 exhibits a qualitatively similar magnetic diffraction profile, with k $\simeq$ (0, 0, 0.37). Inelastic neutron scattering measurements resolve two clear, well-separated CEF excitations in both compounds with nearly the same profile, confirming a well-isolated Kramers doublet ground state. At low energies, a broad, quasi-elastic magnetic response is observed at T $\simeq$ TN, whose momentum-dependence is inconsistent with that expected from conventional collective excitations of localized moments. This discrepancy, along with a Kondo temperature estimate TK ~ 3--5 K -- comparable to TN -- indicates sizable Kondo hybridization, which accounts for the moment reduction and the spiral magnetic order that appears to involve the magnetic hard direction. Our results place these compounds in a regime where local inversion symmetry breaking, anisotropic CEF effects, and competing Kondo and RKKY interactions collectively give rise to unconventional magnetic order.

cond-mat.str-el↗

arXiv2026

A New Layered Kagome Strip Structure Na2Co3(AsO4)2(OH)2: Static and Dynamic Magnetic Properties

One-dimensional kagome strip chains share much of the same frustrated structural motif as two-dimensional kagome antiferromagnets, making them valuable for deepening our understanding of kagome lattice magnetism. In this paper, we report the hydrothermal synthesis and detailed structural and property characterization of Na2Co3(AsO4)2(OH)2, a striped kagome system. The crystal structure was characterized using single crystal X-ray diffraction, which reveals that Na2Co3(AsO4)2(OH)2 crystallizes in the monoclinic crystal system C2/m. The structure features a one-dimensional kagome strip lattice built from Co2+ ions and undergoes an antiferromagnetic transition at TN = 14 K. The magnetic ground state at zero field was characterized using neutron powder diffraction. Below the magnetic transition, Na2Co3(AsO4)2(OH)2 orders into an antiferromagnetic structure with a k-vector (0.5, 0.5, 0.5). In the proposed model, the Co1 moment is predominantly confined to the ac-plane while the Co2 moment is primarily aligned along the b-axis. Two flat bands were observed in the inelastic neutron spectra below the magnetic transition at 5 and 10 meV. Inelastic neutron spectra were modeled with a Heisenberg Hamiltonian including three nearest-neighbor exchange interactions (J1, J2, J3) and strong single-ion anisotropy to stabilize the observed magnetic structure. Our study highlights the complexity of the Co2+-based kagome strip magnetic lattice compound Na2Co3(AsO4)2(OH)2, which provides an excellent platform to broaden our understanding of the frustrated kagome magnetic lattice space.

cond-mat.mtrl-sci↗

arXiv2025

Magnetic dynamics in NiTiO3 honeycomb antiferromagnet using neutron scattering

The ilmenite NiTiO3 consists of a buckled honeycomb lattice, with the Ni spins aligned ferromagnetically in-plane and antiferromagnetically out-of-plane. Using neutron spectroscopy, the magnetic structure and the dynamics were investigated as a function of temperature. Dispersive acoustic bands and nearly dispersionless optical bands at ~3.7 meV are described by a highly anisotropy Heisenberg model with stronger antiferromagnetic (AFM) out-of-plane, weaker ferromagnetic (FM) in-plane interactions and an anisotropy gap of 0.95 meV. The order parameter yields a critical exponent between the Heisenberg and two-dimensional Ising models, consistent with highly anisotropic Heisenberg systems. The frustration parameter ~ 2 supports a weakly frustrated system.

cond-mat.mtrl-sci↗

arXiv2025

Insulating ground state and 2-k magnetic structure of candidate Weyl Hydrogen atom K$_2$Mn$_3$(AsO$_4$)$_3$

The ideal Weyl 'Hydrogen-atom' semi-metal exhibits only a single pair of Weyl nodes and no other trivial states at the Fermi energy. Such a material would be a panacea in the study of Weyl quasi particles allowing direct unambiguous observation of their topological properties. The alluaudite-like K$_2$Mn$_3$(AsO$_4$)$_3$ compound was recently proposed as such a material. Here we use comprehensive experimental work and first principle calculations to assess this prediction. We find K$_2$Mn$_3$(AsO$_4$)$_3$ crystallizes in the $C2/c$ symmetry with a quasi-1D Mn sublattice, growing as small needle-like crystals. Bulk properties measurements reveal magnetic transitions at $\approx$ 8 and $\approx$ 4 K which neutron scattering experiments show correspond to two distinct magnetic orders, first a partially ordered ferrimagnetic $\mathbf{k_1}$= (0, 0, 0) structure at 8 K and a second transition of $\mathbf{k_2}$= (1, 0, 0) at 4 K to a fully ordered state. Below the second transition, both ordering vectors are necessary to describe the complex magnetic structure with modulated spin magnitudes. Both of the best-fit magnetic structures in this work are found to break the symmetry necessary for the generation of the Weyl nodes, though one of the magnetic structures allowed by $\mathbf{k_1}$ does preserve this symmetry. However, the crystals are optically transparent and ellipsometry measurements reveal a large band-gap, undermining expectations of semi-metallic behavior. Density functional theory calculations predict an insulating antiferromagnetic ground state, in contrast to previous reports, and suggest potential frustration on the magnetic sublattice. Given the wide tunability of the alluaudite structure we consider ways to push the system closer to semi-metallic state.

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

Tuning the magnetic properties of the spin-split antiferromagnet MnTe through pressure

The hexagonal antiferromagnet MnTe has attracted enormous interest as a prototypical example of a spin-compensated magnet in which the combination of crystal and spin symmetries lifts the spin degeneracy of the electron bands without the need for spin-orbit coupling, a phenomenon called non-relativistic spin splitting (NRSS). Subgroups of NRSS are determined by the specific spin-interconverting symmetry that connects the two opposite-spin sublattices. In MnTe, this symmetry is rotation, leading to the subgroup with spin splitting away from the Brillouin zone center, often called altermagnetism. MnTe also has the largest spontaneous magnetovolume effect of any known antiferromagnet, implying strong coupling between the magnetic moment and volume. This magnetostructural coupling offers a potential knob for tuning the spin-splitting properties of MnTe. Here, we use neutron diffraction with $\textit{in situ}$ applied pressure to determine the effects of pressure on the magnetic properties of MnTe and further explore this magnetostructural coupling. We find that applying pressure significantly increases the N\'eel temperature but decreases the ordered magnetic moment. We explain this as a consequence of strengthened magnetic exchange interactions under pressure, resulting in higher $T_\mathrm{N}$, with a simultaneous reduction of the local moment of individual Mn atoms, described here via density functional theory. This reflects the increased orbital hybridization and electron delocalization with pressure. These results show that the magnetic properties of MnTe can be controlled by pressure, opening the door to improved properties for spintronic applications through tuning via physical or chemical pressure.

cond-mat.mtrl-sci↗

arXiv2025

Magnetic Pair Distribution Function and Half Polarized Neutron Powder Diffraction at the HB-2A Powder Diffractometer

Local magnetic order and anisotropy are often central for understanding fundamental behavior and emergent functional properties in quantum materials and beyond. Advances in neutron powder diffraction experiments and analysis tools now allow for quantitative determination. We demonstrate this here with complementary total neutron scattering and polarized neutron measurements on the HB-2A neutron powder diffractometer at the High Flux Isotope Reactor (HFIR). In recent years, magnetic pair distribution function (mPDF) analysis has emerged as a powerful technique for probing local magnetic spin ordering of magnetic materials. This method can be broadly applied to any magnetic material but is particularly effective for studying systems with short-range magnetic order, such as materials with reduced dimensionality, geometrically frustrated magnets, thermoelectrics, multiferroics, and correlated paramagnets. Magnetic anisotropy often underpins the short-range order adopted. Half-polarized neutron powder diffraction (pNPD) can be used to determine the local susceptibility tensor on the magnetic sites to quantify the magnetic anisotropy. Combining the techniques of mPDF and pNPD can therefore provide valuable insights into local magnetic behavior. A series of measurements optimized for these techniques are presented as exemplar cases focused on frustrated materials where short-range order dominates, these include measurements to ultra-low temperature (<100 mK) not typically accessible for such experiments.

cond-mat.str-el↗

arXiv2025

Short-range magnetic order and planar anisotropy in the topological ferrimagnet Mn3Si2Te6

Mn3Si2Te6 is a ferrimagnetic topological nodal-line semiconductor that exhibits unconventional colossal magnetoresitance (CMR) behavior, with short-range spin fluctuations being potentially intimately linked to the emergent properties. In this work, we determine the short range magnetic order and quantify the local magnetic anisotropy through total neutron scattering and polarized neutron powder diffraction (pNPD) measurements on polycrystalline Mn3Si2Te6. The real space local and long range spin structure was determined through the application of magnetic pair distribution function (mPDF) analysis, with measurements from the low temperature ordered phase to the high temperature paramagnetic state. Short-range order over a frustrated trimer of three nearest neighbors was found to exist well above the long range ferrimagnetic transition. pNPD measurements in the spin polarized paramagnetic state were used to extract the local site susceptibility tensor of the Mn ions to quantify the magnetic anisotropy. Our combined mPDF and pNPD results provide quantitative information on the short-range order intrinsic to Mn3Si2Te6, showing strong in-plane anisotropy with the spins largely confined to the ab-plane in zero field and remain stable with increasing temperature through the long-range to short-range ordered transition.

cond-mat.str-el↗

arXiv2025

Jeff = 1/2 Diamond Magnet CaCo2TeO6: A Pathway toward New Spin Physics and Quantum Functions

Diamond lattice magnets, formed by a framework of corner-sharing tetrahedra of magnetic cations, offer unique opportunities to realize novel states of matter for potential utility in information technology. However, research has mostly focused on AB2X4 spinels with Td magnetic ions. This hinders the atomically enabled tunability of competing interactions at different energy scales and the ability to harness many-body electronic states in quantum materials, making the discovery of quantum fluctuations and spin dynamics less accessible. We discover a new material CaCo2TeO6 featuring a diamond lattice of two distinct Oh-Co2+ sites. This material displays strong quantum fluctuations, increased competing magnetic exchange interactions, and field-induced tunability of magnetic structures. The results demonstrate how simple, fundamental refinements in ligand fields can profoundly influence the phase space of quantum matter.

cond-mat.mtrl-sci↗

arXiv2025

Applied-field magnetic structure and spectroscopy shifts of the effective spin-$\frac{1}{2}$, $XY$-like magnet Li$_2$CoCl$_4$

Insulators containing chains of magnetic transition metal cations provide platforms for probing spin-$\frac{1}{2}$ dynamics and quantum critical behavior. Li$_2$CoCl$_4$ contains edge-sharing CoCl$_6$ octahedra that form chains along the crystallographic $c$ axis and orders antiferromagnetically at zero field, but questions remain about its applied-field magnetic structure and the Co$^{2+}$ spin state. Here, we show with neutron diffraction on a polycrystalline sample how the anti-aligned chains of cobalt moments begin to transition to a ferromagnetic state above 1.6 T. Further, using magnetic resonance absorption measurements and noninteracting spin models, we reveal the strongly anisotropic nature of the Co$^{2+}$ ion's $XY$-like magnetic behavior ($g_{\parallel}=2.77$ and $g_{\perp}=5.23$) and its $J=\frac{1}{2}$ ground state. We, therefore, supply the magnetic structures and anisotropic description needed to explore the dynamics of the field-driven magnetic phases, laying the foundation for further experimental and theoretical studies.

cond-mat.str-el↗

arXiv2024

Cluster spin glass correlations and dynamics in Zn$_{0.5}$Mn$_{0.5}$Te

We present a magnetometry, muon spin relaxation ($\mu$SR), and neutron scattering study of the insulating face-centered-cubic spin glass Zn$_{0.5}$Mn$_{0.5}$Te. The magnetometry and $\mu$SR results confirm a spin freezing transition around $T_f \approx 23$ K, with the spin fluctuation rate decreasing gradually and somewhat inhomogeneously through the sample volume as the temperature decreases toward $T_f$. Characteristic spin correlation times well above $T_f$ are on the order of 10$^{-10}$ s, in line with expectations for a cluster spin glass. Using magnetic pair distribution function (mPDF) analysis and reverse Monte Carlo (RMC) modeling of the magnetic diffuse neutron scattering data, we show that the spin-glass ground state consists of clusters of spins exhibiting short-range-ordered type-III antiferromagnetic correlations, with a locally ordered moment of 3.1(1) $\mu_{\mathrm{B}}$ between nearest-neighbor spins. The type-III correlations decay exponentially as a function of spin separation distance with a correlation length of approximately 5 \AA. The diffuse magnetic scattering and corresponding mPDF show no significant changes across $T_f$, indicating that the dynamically fluctuating short-range spin correlations in the paramagnetic state retain the same basic type-III configuration; the only change apparent from the neutron scattering data is a gradual reduction of the correlation length and locally ordered moment with increasing temperature. Taken together, these results paint a unique and detailed picture of the local magnetic structure and dynamics in Zn$_{0.5}$Mn$_{0.5}$Te and show that this material is best described as a cluster spin glass. In addition, this work showcases a statistical method for extracting diffuse scattering signals from neutron powder diffraction data.

cond-mat.mtrl-sci↗

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

Chemical versus physical pressure effects on the structure transition of bilayer nickelates

The observation of high-$T_c$ superconductivity (HTSC) in concomitant with pressure-induced orthorhombic-tetragonal structural transition in the bilayer La$_{3}$Ni$_2$O$_7$ has sparked hopes of achieving HTSC by stabilizing the tetragonal phase at ambient pressure. To mimic the effect of external physical pressures, the application of chemical pressure via replacing La$^3$$^+$ with smaller rare-earth R$^3$$^+$ has been considered as a potential route. Here we clarify the distinct effects of chemical and physical pressures on the structural transition of bilayer nickelates through a combined experimental and theoretical investigation. Contrary to general expectations, we find that substitutions of smaller R$^3$$^+$ for La$^3$$^+$ in La$_{3-x}$R$_x$Ni$_2$O$_{7-\delta}$, despite of an overall lattice contraction, produce stronger orthorhombic structural distortions and thus require higher pressures to induce the structural transition. We established a quantitative relationship between the critical pressure $P_c$ for structural transition and the average size of $A$-site cations. A linear extrapolation of $P_c$ versus <$r_A$> yields a putative critical value of <$r_A$>$_c$ ~ 1.23 angstrom for $P_c$ ~ 1 bar. The negative correlation between $P_c$ and <$r_A$> indicates that it is unlikely to reduce $P_c$ to ambient by replacing La$^3$$^+$ with smaller R$^3$$^+$ ions. Instead, partial substitution of La$^3$$^+$ with larger cations such as alkaline-earth Sr$^2$$^+$ or Ba$^2$$^+$ might be a feasible approach. Our results provide valuable guidelines in the quest of ambient-pressure HTSC in bilayer nickelates.

cond-mat.str-el↗

arXiv2024

Magnetic properties of RE2O2CO3 (RE = Pr, Nd, Gd, Tb, Dy, Ho, Er, Yb) with a rare earth-bilayer of triangular lattice

Polycrystalline samples of RE2O2CO3 (RE = Pr, Nd, Gd, Tb, Dy, Ho, Er, and Yb) with a unique rare-earth bilayer of triangular lattice were synthesized and studied by DC and AC magnetic susceptibility. Data reveals various magnetic ground states including (i) a nonmagnetic ground state for the Pr sample; (ii) long range magnetic ordering for the Nd, Gd, Tb, Dy, Ho, and Er samples. Besides the Gd sample, they exhibit field-induced spin state transitions. More interestingly, the series spin state transitions in the Nd and Dy samples could be attributed to the field-induced up-up-down (UUD) spin structure. Neutron powder diffraction (NPD) measurements of the Er sample suggest a spiral spin structure below its TN; and (iii) a short-range ordering for the Yb sample. The disrupted inter-layer interaction due to the shift of Yb3+ ions within the bilayer prevents long range magnetic ordering down to 30 mK and makes it another Yb-related triangular lattice antiferromagnet that has the potential to realize a quantum spin liquid state.

cond-mat.str-el↗

arXiv2024

Bulk high-temperature superconductivity in the high-pressure tetragonal phase of bilayer La2PrNi2O7

The Ruddlesden-Popper (R-P) bilayer nickelate, La3Ni2O7, was recently found to show signatures of high-temperature superconductivity (HTSC) at pressures above 14 GPa. Subsequent investigations achieved zero resistance in single- and poly-crystalline samples under hydrostatic pressure conditions. Yet, obvious diamagnetic signals, the other hallmark of superconductors, are still lacking owing to the filamentary nature with low superconducting volume fraction. The presence of a novel "1313" polymorph and competing R-P phases obscured proper identification of the phase for HTSC. Thus, achieving bulk HTSC and identifying the phase at play are the most prominent tasks at present. Here, we address these issues in the praseodymium (Pr)-doped La2PrNi2O7 polycrystalline samples. We find that the substitutions of Pr for La effectively inhibits the intergrowth of different R-P phases, resulting in nearly pure bilayer structure. For La2PrNi2O7, pressure-induced orthorhombic-to-tetragonal structural transition takes place at Pc ~ 11 GPa, above which HTSC emerges gradually upon further compression. The superconducting transition temperatures at 18-20 GPa reach Tconset = 82.5 K and Tczero = 60 K, which are the highest values among known nickelate superconductors. More importantly, bulk HTSC was testified by detecting clear diamagnetic signals below ~75 K corresponding to an estimated superconducting volume fraction ~ 57(5)% at 20 GPa. Our results not only resolve the existing controversies but also illuminate directions for exploring bulk HTSC in the bilayer nickelates.

cond-mat.supr-con↗

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↗