arXiv subjects

J. Ross Stewart

Publications and source records attributed to J. Ross Stewart.

At least 19 recordsLinked to original sources

arXiv2026

Zeeman Ladders in Frustrated XYZ Spin Chains

We investigate the nature of the excitations captured by the dynamical response of XYZ triangular spin-1/2 ladders. We complement experimental inelastic neutron scattering results on the compound $\text{Cs}_\text{2}\text{CoBr}_\text{4}$ with numerically exact simulations based on time-dependent matrix product state methods. Our results show that bound states of spinon excitations can arise in XYZ beyond the requirement of strong Ising anisotropies. We analyze the role of the frustrated triangular couplings on the excitations giving rise to the spin dynamical structure factor and show how the features of the bound states manifest themselves in the different polarization channels.

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

Quasi-one-dimensional spin excitations in the iron pnictide NaFe$_{0.53}$Cu$_{0.47}$As

Spectroscopic measurements in model one-dimensional (1D) correlated systems offer insights for understanding their two-dimensional counterparts, which include the cuprate and iron pnictide/chalcogenide superconductors. A major challenge is the identification of such correlated systems with dominantly 1D physics. In this work, inelastic neutron scattering measurements on NaFe$_{0.53}$Cu$_{0.47}$As single crystal directly reveal quasi-1D spin excitations, resulting from atomic order that lead to magnetic Fe and nonmagnetic Cu chains. The dominant exchange interaction is antiferromagnetic along the chain ($SJ_{\rm \parallel}\approx90.1(3)$~meV), whereas the inter-chain couplings are much weaker ($SJ_{\rm \perp}\approx-2.4(1)$~meV and $SJ_{\rm c}\approx0.15(5)$~meV). The quasi-1D spin excitations in NaFe$_{0.53}$Cu$_{0.47}$As stem from both the Néel and stripe vectors, with Néel excitations sensitive to Fe impurities on the Cu site. The spin excitations in quasi-1D NaFe$_{0.53}$Cu$_{0.47}$As and quasi-2D FeSe exhibit a striking resemblance, suggesting a common origin for their coexistent stripe and Néel excitations. Our findings demonstrate magnetic dilution in NaFeAs leads to dimension reduction of its magnetic degree of freedom, presenting a strategy for discovering low-dimensional quantum materials.

cond-mat.str-el↗

arXiv2025

Critical spin fluctuations across the superconducting dome in La$_{2-x}$Sr$_{x}$CuO$_4$

Overdoped cuprate superconductors are strange metals above their superconducting transition temperature. In such materials, the electrical resistivity has a strong linear dependence on temperature ($T$) and electrical current is not carried by electron quasiparticles as in conventional metals. Here we demonstrate that the strange metal behaviour co-exists with strongly temperature-dependent critical spin fluctuations showing dynamical scaling across the cuprate phase diagram. Our neutron scattering observations and the strange metal behaviour are consistent with a spin density wave quantum phase transition in a metal with spatial disorder in the tuning parameter. Numerical computations using a theory of spin density waves in a disordered metal yield an extended `Griffiths phase' with scaling properties in agreement with experimental observations. Thus we establish that low-energy spin excitations and spatial disorder are central to the strange metal behaviour.

cond-mat.supr-con↗

arXiv2025

From continuum excitations to sharp magnons via transverse magnetic field in the spin-1/2 Ising-like triangular lattice antiferromagnet Na2BaCo(PO4)2

We report high-resolution inelastic neutron scattering measurements of the excitation spectrum in large single crystals of the spin-1/2 triangular lattice Ising-like antiferromagnet Na2BaCo(PO4)2 in magnetic fields applied transverse to the Ising axis. In the high-field polarized phase above a critical field $B_{C}$ we observe sharp magnons, as expected in the case of no exchange disorder. Through simultaneous fits to the dispersions including data in polarizing field along the Ising axis, we obtain an excellent match to an Ising-like XXZ Hamiltonian and rule out previously proposed Kitaev exchanges. In the intermediate-field phase below $B_{C}$, we observe three dispersive modes, out of which only the lowest energy one is sharp and the others are broad and overlap with continuum scattering. We propose that the broadening effects are due to magnon decays into two-magnon excitations and confirm that such processes are kinematically allowed. The continuum scattering becomes progressively stronger upon lowering field and, at 0.25 T and zero field, it dominates the complete spectrum with no clear evidence for even broadened magnon modes. We discuss the relevance of the continuous manifold of mean-field degenerate ground states of the refined Hamiltonian for capturing the observed spectrum in zero field, and compare the data with the one- and two-magnon spectrum averaged over this manifold. We also propose a model of the interlayer couplings to explain the observed finite interlayer magnetic propagation vector of the zero-field magnetic order; this requires the breaking of the mirror symmetry in the nominal P-3m1 space group and through refinement of x-ray diffraction data on an untwinned single crystal, we indeed confirm a rotation of the CoO6 octahedra around the c-axis, which lowers the symmetry to P-3.

cond-mat.str-el↗

arXiv2025

Single-ion anisotropy driven chiral magnetic order in a spin-1 antiferromagnetic chain

Chirality in magnetic systems gives rise to a wide range of exotic phenomena, yet its influence in $S=1$ chains remains largely unexplored. Here, we present a comprehensive experimental study of a chiral antiferromagnetic (AFM) $S=1$ chain, [Ni(pym)(H$_{2}$O)$_{4}$]SO$_{4} \cdot$ H$_{2}$O (pym = pyrimidine), where the Ni(II) octahedral orientation exhibits a four-fold chiral periodicity. Muon spin rotation measurements indicate the onset of long-range magnetic order below $T_{\rm N} = 1.82(2)\,\mathrm{K}$. Neutron diffraction measurements reveal a chiral AFM order driven by a chiral modulation of the easy-axis anisotropy direction, rather than the typical scenario of Dzyaloshinskii-Moriya interactions, geometrical frustration or higher-order interactions. Inelastic neutron scattering (INS) measurements reveal dispersive spin-wave excitations well described by linear spin-wave theory, with Hamiltonian parameters $J_{0} = 6.81(1)\,\mathrm{K}$ (intrachain exchange), $J'_{1\rm a} = -0.091(1)\,\mathrm{K}$ (interchain exchange), and $D = -3.02(1)\,\mathrm{K}$ (easy-axis single-ion anisotropy). These parameters are further validated by Monte Carlo simulations of the magnetisation. Additionally, the INS data reveal multiple dispersionless bands, suggesting the presence of further excitations beyond the scope of our linear spin-wave theory.

cond-mat.str-el↗

arXiv2024

Magnetic properties of a staggered $S=1$ chain Ni(pym)(H$_{2}$O)$_{2}$(NO$_{3}$)$_{2}$ with an alternating single-ion anisotropy direction

Materials composed of spin-1 antiferromagnetic (AFM) chains are known to adopt complex ground states which are sensitive to the single-ion-anisotropy (SIA) energy ($D$), and intrachain ($J_{0}$) and interchain ($J'_{i}$) exchange energy scales. While theoretical and experimental studies have extended this model to include various other energy scales, the effect of the lack of a common SIA axis is not well explored. Here we investigate the magnetic properties of Ni(pyrimidine)(H$_{2}$O)$_{2}$(NO$_{3}$)$_{2}$, a chain compound where the tilting of Ni octahedra leads to a 2-fold alternation of the easy-axis directions along the chain. Muon-spin relaxation measurements indicate a transition to long-range order at $T_{\text{N}}=2.3$\,K and the magnetic structure is initially determined to be antiferromagnetic and collinear using elastic neutron diffraction experiments. Inelastic neutron scattering measurements were used to find $J_{0} = 5.107(7)$\,K, $D = 2.79(1)$\,K, $J'_{2}=0.18(3)$\,K and a rhombic anisotropy energy $E=0.19(9)$\,K. Mean-field modelling reveals that the ground state structure hosts spin canting of $ϕ\approx6.5^{\circ}$, which is not detectable above the noise floor of the elastic neutron diffraction data. Monte-Carlo simulation of the powder-averaged magnetization, $M(H)$, is then used to confirm these Hamiltonian parameters, while single-crystal $M(H)$ simulations provide insight into features observed in the data.

cond-mat.str-el↗

arXiv2024

Magnetic Phase Diagram of Rouaite, Cu$_2$(OH)$_3$NO$_3$

Spinon-magnon mixing was recently reported in botallackite Cu$_2$(OH)$_3$Br with a uniaxially compressed triangular lattice of Cu$^{2+}$ quantum spins [Zhang et al., Phys. Rev. Lett. 125, 037204 (2020)]. Its nitrate counterpart rouaite, Cu$_2$(OH)$_3$NO$_3$, has a highly analogous structure and might be expected to exhibit similar physics. To lay a foundation for research on this material, we clarify rouaite's magnetic phase diagram and identify both low-field phases. The low-temperature magnetic state consists of alternating ferro- and antiferromagnetic chains, as in botallackite, but with additional canting, leading to net moments on all chains which rotate from one chain to another to form a 90$^\circ$ cycloidal pattern. The higher-temperature phase is a helical modulation of this order, wherein the spins rotate from one Cu plane to the next. This extends to zero temperature for fields perpendicular to the chains, leading to a set of low-temperature field-induced phase transitions. Rouaite may offer another platform for spinon-magnon mixing, while our results suggest a delicate balance of interactions and high tunability of the magnetism.

cond-mat.str-el↗

arXiv2022

Magnetic ground state of the Kitaev Na$_2$Co$_2$TeO$_6$ spin liquid candidate

As a candidate Kitaev material, Na$_2$Co$_2$TeO$_6$ exhibits intriguing magnetism on a honeycomb lattice that is believed to be $C_3$-symmetric. Here we report a neutron diffraction study of high quality single crystals under $a$-axis magnetic fields. Our data support the less common notion of a magnetic ground state that corresponds to a triple-$\mathbf{q}$ magnetic structure with $C_3$ symmetry, rather than the multi-domain zigzag structure typically assumed in prototype Kitaev spin liquid candidates. In particular, we find that the field is unable to repopulate the supposed zigzag domains, where the only alternative explanation is that the domains are strongly pinned by hitherto unidentified structural reasons. If the triple-$\mathbf{q}$ structure is correct then this requires reevaluation of many candidate Kitaev materials. We also find that fields beyond about 10 Tesla suppress the long range antiferromagnetic order, allowing new magnetic behavior to emerge different from that expected for a spin liquid.

cond-mat.str-el↗

arXiv2022

Upgrade of the MARI spectrometer at ISIS

The MARI direct geometry time-of-flight neutron spectrometer at ISIS has been upgraded with an $m=3$ supermirror guide and new detector electronics. This has resulted in a flux gain of ${\approx}6{\times}$ at $λ=1.8$ Å, and improvements on discriminating electrical noise, allowing MARI to continue to deliver a high quality science program well into its fourth decade of life.

physics.ins-det↗

arXiv2022

Magnetic field effects in an octupolar quantum spin liquid candidate

Quantum spin liquid (QSL) is a disordered state of quantum-mechanically entangled spins commonly arising from frustrated magnetic dipolar interactions. However, QSL in some pyrochlore magnets can also come from frustrated magnetic octupolar interactions. Although the key signature for both dipolar and octupolar interaction-driven QSL is the presence of a spin excitation continuum (spinons) arising from the spin quantum number fractionalization, an external magnetic field-induced ferromagnetic order will transform the spinons into conventional spin waves in a dipolar QSL. By contrast, in an octupole QSL, the spin waves carry octupole moments that do not couple, in the leading order, to the external magnetic field or to neutron moments but will contribute to the field dependence of the heat capacity. Here we use neutron scattering to show that the application of a large external magnetic field to Ce2Zr2O7, an octupolar QSL candidate, induces an Anderson-Higgs transition by condensing the spinons into a static ferromagnetic ordered state with octupolar spin waves invisible to neutrons but contributing to the heat capacity. Our theoretical calculations also provide a microscopic, qualitative understanding for the presence of octupole scattering at large wavevectors in Ce2Sn2O7 pyrochlore, and its absence in Ce2Zr2O7. Therefore, our results identify Ce2Zr2O7 as a strong candidate for an octupolar U (1) QSL, establishing that frustrated magnetic octupolar interactions are responsible for QSL properties in Ce-based pyrochlore magnets.

cond-mat.str-el↗

arXiv2021

Spin excitations in metallic kagome lattice FeSn and CoSn

In two-dimensional (2D) metallic kagome lattice materials, destructive interference of electronic hopping pathways around the kagome bracket can produce nearly localized electrons, and thus electronic bands that are flat in momentum space. When ferromagnetic order breaks the degeneracy of the electronic bands and splits them into the spin-up majority and spin-down minority electronic bands, quasiparticle excitations between the spin-up and spin-down flat bands should form a narrow localized spin-excitation Stoner continuum coexisting with well-defined spin waves in the long wavelengths. Here we report inelastic neutron scattering studies of spin excitations in 2D metallic Kagome lattice antiferromagnetic FeSn and paramagnetic CoSn, where angle resolved photoemission spectroscopy experiments found spin-polarized and nonpolarized flat bands, respectively, below the Fermi level. Although our initial measurements on FeSn indeed reveal well-defined spin waves extending well above 140 meV coexisting with a flat excitation at 170 meV, subsequent experiments on CoSn indicate that the flat mode actually arises mostly from hydrocarbon scattering of the CYTOP-M commonly used to glue the samples to aluminum holder. Therefore, our results established the evolution of spin excitations in FeSn and CoSn, and identified an anomalous flat mode that has been overlooked by the neutron scattering community for the past 20 years.

cond-mat.str-el↗

arXiv2020

Nature of Partial Magnetic Order in the Frustrated Antiferromagnet Gd2Ti2O7

Partially-ordered magnets are distinct from both spin liquids and conventional ordered magnets because order and disorder coexist in the same magnetic phase. Here, we determine the nature of partial order in the canonical frustrated pyrochlore antiferromagnet Gd$_2$Ti$_{2}$O$_{7}$. Using single-crystal neutron-diffraction measurements in applied magnetic field, magnetic symmetry analysis, inelastic neutron-scattering measurements, and spin-wave modeling, we show that its low-temperature magnetic structure involves two propagation vectors (2-$\mathbf{k}$ structure) with suppressed ordered magnetic moments and enhanced spin-wave fluctuations. Our experimental results support theoretical predictions of thermal fluctuation-driven order in Gd$_{2}$Ti$_{2}$O$_{7}$.

cond-mat.str-el↗

arXiv2016

Spin Correlations in the Dipolar Pyrochlore Antiferromagnet Gd2Sn2O7

We investigate spin correlations in the dipolar Heisenberg antiferromagnet Gd2Sn2O7 using polarised neutron-scattering measurements in the correlated paramagnetic regime. Using Monte Carlo methods, we show that our data are sensitive to weak further-neighbour exchange interactions of magnitude ~0.5% of the nearest-neighbour interaction, and are compatible with either antiferromagnetic next-nearest neighbour interactions, or ferromagnetic third-neighbour interactions that connect spins across hexagonal loops. Calculations of the magnetic scattering intensity reveal rods of diffuse scattering along [111] reciprocal-space directions, which we explain in terms of strong antiferromagnetic correlations parallel to the set of <110> directions that connect a given spin with its nearest neighbours. Finally, we demonstrate that the spin correlations in Gd2Sn2O7 are highly anisotropic, and correlations parallel to third-neighbour separations are particularly sensitive to critical fluctuations associated with incipient long-range order.

cond-mat.str-el↗

arXiv2016

The Magnetic Structure of Paramagnetic MnO

Using a combination of single-crystal neutron scattering and reverse Monte Carlo refinements, we study the magnetic structure of paramagnetic MnO at a temperature (160\,K) substantially below the Curie-Weiss temperature $|θ|\sim550$\,K. The microscopic picture we develop reveals a locally-ordered domain structure that persists over distances many times larger than the correlation length implied by direct analysis of the spin correlation function. Moreover, the directional dependence of paramagnetic spin correlations in paramagnetic MnO differs in some important respects from that of its incipient ordered antiferromagnetic state. Our results have implications for the understanding of paramagnetic states in weakly-frustrated systems, including high-temperature superconductors.

cond-mat.mtrl-sci↗

arXiv2016

From 3D static order to 2D dynamic correlations in the tetragonal double perovskite Sr2CuWO6

\SCWO is a tetragonal ($I4/m$) double perovskite with diamagnetic W$^{6+}$ (5d$^0$) and (Jahn-Teller-active) Cu$^{2+}$ (3$d^9$) in a rocksalt-ordered arrangement on the B sites, modelling an anisotropic fcc-lattice antiferromagnet with $S=1/2$. We have studied the magnetic structure, dynamics and thermodynamic properties of this material above and below the \Neel{}-ordering transition at $T_{\textrm{N}} = 24$~K. Muon spin relaxation spectroscopy, neutron diffraction and neutron spectroscopy experiments show that the transition at $T_{\textrm{N}}$ on heating is from static 3D type-2 antiferromagnetism to 2D dynamic correlations that remain detectable up to 100~K. Above $T_{\textrm{N}}$ the muon relaxation is described by a compressed exponential decay, revealing a strong correlation between the spin fluctuation rate and the 2D correlation length. The low-temperature muon data and the entropy release around $T_{\textrm{N}}$ as obtained from the heat capacity data point to small magnetic domains, probably of the order of 60~Å. We note that the material behaves more like a quasi-2D square lattice antiferromagnet than could be expected considering its structure only. A possible explanation might lie in the unusual strong spin-orbit-coupled magnetism of the W 5$d$ levels, as the dominant exchange interaction is via the Cu-O-W-O-Cu pathway.

cond-mat.str-el↗

arXiv2015

Nature of Partial Magnetic Order in the Frustrated Antiferromagnet Gd2Ti2O7

The frustrated pyrochlore antiferromagnet Gd$_{2}$Ti$_{2}$O$_{7}$ has an unusual partially-ordered magnetic structure at the lowest measurable temperatures. This structure is currently believed to involve four magnetic propagation vectors $\mathbf{k}\in \langle \frac{1}{2} \frac{1}{2} \frac{1}{2} \rangle^*$ in a cubic 4-$\mathbf{k}$ structure, based on analysis of magnetic diffuse-scattering data [J. Phys.: Condens. Matter 16, L321 (2004)]. Here, we present three pieces of evidence against the 4-$\mathbf{k}$ structure. First, we report single-crystal neutron-diffraction measurements as a function of applied magnetic field, which are consistent with the selective field-induced population of non-cubic magnetic domains. Second, we present evidence from high-resolution powder neutron-diffraction measurements that rhombohedral strains exist within magnetic domains, which may be generated by magneto-elastic coupling only for the alternative 1-$\mathbf{k}$ structure. Finally, we show that the argument previously used to rule out the 1-$\mathbf{k}$ structure is flawed, and demonstrate that magnetic diffuse-scattering data can actually be fitted quantitatively by a 1-$\mathbf{k}$ structure in which spin fluctuations on ordered and disordered magnetic sites are strongly coupled. Our results provide an experimental foundation on which to base theoretical descriptions of partially-ordered states.

cond-mat.str-el↗

arXiv2013

Spin correlations in Ca3Co2O6: A polarised-neutron diffraction and Monte Carlo study

We present polarised-neutron diffraction measurements of the Ising-like spin-chain compound Ca3Co2O6 above and below the magnetic ordering temperature TN. Below TN, a clear evolution from a single-phase spin-density wave (SDW) structure to a mixture of SDW and commensurate antiferromagnet (CAFM) structures is observed on cooling. For a rapidly-cooled sample, the majority phase at low temperature is the SDW, while if the cooling is performed sufficiently slowly, then the SDW and the CAFM structure coexist between 1.5 and 10 K. Above TN, we use Monte Carlo methods to analyse the magnetic diffuse scattering data. We show that both intra- and inter-chain correlations persist above TN, but are essentially decoupled. Intra-chain correlations resemble the ferromagnetic Ising model, while inter-chain correlations resemble the frustrated triangular-lattice antiferromagnet. Using previously-published bulk property measurements and our neutron diffraction data, we obtain values of the ferromagnetic and antiferromagnetic exchange interactions and the single-ion anisotropy.

cond-mat.str-el↗