arXiv subjects

S. E. Dutton

Publications and source records attributed to S. E. Dutton.

16 recordsLinked to original sources

arXiv2025

Intrinsic disorder in the candidate quantum spin ice Pr$_2$Zr$_2$O$_7$

Quantum spin liquids with long-range entanglement are of great interest for applications in quantum technology. The quantum spin ice Pr$_2$Zr$_2$O$_7$ is a promising example, where it is believed that structural disorder plays a key role in enhancing quantum mechanical effects by introducing strains that split the ground state doublet akin to the effect of a local disordered transverse field. However, the precise defect structure responsible for this behaviour is unknown. Here we have determined the intrinsic defect structure of Pr$_2$Zr$_2$O$_7$ using neutron and x-ray scattering techniques supported by density functional theory. We find the main defect is the stuffing of Zr$^{4+}$ sites by Pr$^{3+}$ ions, accompanied by charge compensating O$^{2-}$ vacancies, and the relaxation of a neighbouring O$^{2-}$ ion to an interstitial site. Our results explain the single-ion magnetism by considering the non-magnetic singlets that arise on neighbouring sites as a result of the defect structure. These singlets account for additional features in the crystal electric field excitations. The effects caused by this low level of structural disorder are magnified since several neighbouring Pr sites are affected. This makes a significant contribution towards the observed broadening of pinch points in the magnetic diffuse scattering, which was previously attributed purely to quantum effects.

cond-mat.str-el↗

arXiv2023

Spin-glass states generated in a van der Waals magnet by alkali-ion intercalation

Tuning magnetic properties in layered van der Waals (vdW) materials has captured a significant attention due to the efficient control of ground-states by heterostructuring and external stimuli. Electron doping by electrostatic gating, interfacial charge transfer and intercalation is particularly effective in manipulating the exchange and spin-orbit properties, resulting in a control of Curie temperature ($T_{\text{C}}$) and magnetic anisotropy. Here, we discover an uncharted role of intercalation to generate magnetic frustration. As a model study, we intercalate Na atoms into the vdW gaps of pristine Cr$_2$Ge$_2$Te$_6$ (CGT) where generated magnetic frustration leads to emerging spin-glass states coexisting with a ferromagnetic order. A series of dynamic magnetic susceptibility measurements/analysis confirms the formation of magnetic clusters representing slow dynamics with a distribution of relaxation times. The intercalation also modifies other macroscopic physical parameters including the significant enhancement of $T_{\text{C}}$ from 66\,K to 240\,K and the switching of magnetic easy-hard axis direction. Our study identifies intercalation as a unique route to generate emerging frustrated spin states in simple vdW crystals.

cond-mat.mtrl-sci↗

arXiv2022

Valence bond glass state in the 4$d^1$ fcc antiferromagnet Ba$_2$LuMoO$_6$

$B$-site ordered 4$d^1$ and 5$d^1$ double perovskites have a number of potential novel ground states including multipolar order, quantum spin liquids and valence bond glass states. These arise from the complex interactions of spin-orbital entangled $J_{eff}$ = 3/2 pseudospins on the geometrically frustrated fcc lattice. The 4$d^1$ Mo$^{5+}$ perovskite Ba$_2$YMoO$_6$ has been suggested to have a valence bond glass ground state. Here we report on the low temperature properties of powder samples of isostructural Ba$_2$LuMoO$_6$: the only other known cubic 4$d^1$ perovskite with one magnetic cation. Our muon spectroscopy experiments show that magnetism in this material remains dynamic down to 60 mK without any spin freezing or magnetic order. A singlet-triplet excitation with a gap of $Δ$ = 28 meV is observed in inelastic neutron scattering. These results are interpreted as a disordered valence bond glass ground state similar to Ba$_2$YMoO$_6$. Our results highlight the differences of the 4$d^1$ double perovskites in comparison to cubic 5$d^1$ analogues, which have both magnetic and multipolar order.

cond-mat.str-el↗

arXiv2020

Sample Dependence of Magnetism in the Next Generation Cathode Material LiNi$_{0.8}$Mn$_{0.1}$Co$_{0.1}$O$_2$

We present a structural and magnetic study on two batches of polycrystalline LiNi$_{0.8}$Mn$_{0.1}$Co$_{0.1}$O$_2$ (commonly known as Li NMC 811), a Ni-rich Li ion battery cathode material, using elemental analysis, X-ray and neutron diffraction, magnetometry, and polarised neutron scattering measurements. We find that the samples, labelled S1 and S2, have the composition Li$_{1-x}$Ni$_{0.9+x-y}$Mn$_y$Co$_{0.1}$O$_2$, with $x = 0.025(2)$, $y = 0.120(2)$ for S1 and $x = 0.002(2)$, $y = 0.094(2)$ for S2, corresponding to different concentrations of magnetic ions and excess Ni$^{2+}$ in the Li$^+$layers. Both samples show a peak in the zero-field cooled (ZFC) dc susceptibility at 8.0(2) K but the temperature at which the ZFC and FC (field-cooled) curves deviate is substantially different: 64(2) K for S1 and 122(2) K for S2. Ac susceptibility measurements show that the transition for S1 shifts with frequency whereas no such shift is observed for S2 within the resolution of our measurements. Our results demonstrate the sample dependence of magnetic properties in Li NMC 811, consistent with previous reports on the parent material LiNiO$_2$. We further establish that a combination of experimental techniques are necessary to accurately determine the chemical composition of next generation battery materials with multiple cations.

cond-mat.mtrl-sci↗

arXiv2018

Magnetic excitations of the classical spin liquid MgCr2O4

We report a comprehensive inelastic neutron-scattering study of the frustrated pyrochlore antiferromagnet MgCr2O4 in its cooperative paramagnetic regime. Theoretical modeling yields a microscopic Heisenberg model with exchange interactions up to third-nearest neighbors, which quantitatively explains all the details of the dynamic magnetic response. Our work demonstrates that the magnetic excitations in paramagnetic MgCr2O4 are faithfully represented in the entire Brillouin zone by a theory of magnons propagating in a highly-correlated paramagnetic background. Our results also suggest that MgCr2O4 is proximate to a spiral spin-liquid phase distinct from the Coulomb phase, which has implications for the magneto-structural phase transition in MgCr2O4 .

cond-mat.str-el↗

arXiv2017

Relieving the frustration through Mn$^{3+}$ substitution in Holmium Gallium Garnet

We present a study on the impact of Mn$^{3+}$ substitution in the geometrically frustrated Ising garnet Ho$_3$Ga$_5$O$_{12}$ using bulk magnetic measurements and low temperature powder neutron diffraction. We find that the transition temperature, $T_N$ = 5.8 K, for Ho$_3$MnGa$_4$O$_{12}$ is raised by almost 20 when compared to Ho$_3$Ga$_5$O$_{12}$. Powder neutron diffraction on Ho$_3$Mn$_x$Ga$_{5-x}$O$_{12}$ ($x$ = 0.5, 1) below $T_N$ shows the formation of a long range ordered ordered state with $\mathbf{k}$ = (0,0,0). Ho$^{3+}$ spins are aligned antiferromagnetically along the six crystallographic axes with no resultant moment while the Mn$^{3+}$ spins are oriented along the body diagonals, such that there is a net moment along [111]. The magnetic structure can be visualised as ten-membered rings of corner-sharing triangles of Ho$^{3+}$ spins with the Mn$^{3+}$ spins ferromagnetically coupled to each individual Ho$^{3+}$ spin in the triangle. Substitution of Mn$^{3+}$ completely relieves the magnetic frustration with $f = θ_{CW}/T_N \approx 1.1$ for Ho$_3$MnGa$_4$O$_{12}$.

cond-mat.str-el↗

arXiv2017

Sensitivity of magnetic properties to chemical pressure in lanthanide garnets $Ln_3A_2X_3\text{O}_{12}$, $Ln$ = Gd, Tb, Dy, Ho, $A$ = Ga, Sc, In, Te, $X$ = Ga, Al, Li

A systematic study of the structural and magnetic properties of three-dimensionally frustrated lanthanide garnets $Ln_3A_2X_3\text{O}_{12}$, $Ln$ = Gd, Tb, Dy, Ho, $A$ = Ga, Sc, In, Te, $X$ = Ga, Al, Li is presented. Garnets with $Ln$ = Gd show magnetic behaviour consistent with isotropic Gd$^{3+}$ spins; no magnetic ordering is observed for T $\geq$ 0.4 K. Magnetic ordering features are seen for garnets with $Ln$ = Tb, Dy, Ho in the temperature range 0.4 < T < 2.5 K, however the nature of the magnetic ordering varies for the different $Ln$ as well as for different combinations of $A$ and $X$. The changes in magnetic behaviour can be explained by tuning of the magnetic interactions and changes in the single-ion anisotropy. The change in magnetic entropy is evaluated from isothermal magnetisation measurements to characterise the magnetocaloric effect in these materials. Among the Gd garnets, the maximum change in magnetic entropy per mole (15.45 J K$^{-1}$ mol$_{\text{Gd}}^{-1}$) is observed for Gd$_3$Sc$_2$Ga$_3$O$_{12}$ at 2 K, in a field of 9 T. The performance of Dy$_3$Ga$_5$O$_{12}$ as a magnetocaloric material surpasses the other garnets with $Ln$ = Tb, Dy, Ho.

cond-mat.str-el↗

arXiv2016

Emergent Order in the Kagome Ising Magnet Dy3Mg2Sb3O14

The kagome lattice -- a two-dimensional (2D) arrangement of corner-sharing triangles -- is at the forefront of the search for exotic states generated by magnetic frustration. Such states have been observed experimentally for Heisenberg and planar spins. In contrast, frustration of Ising spins on the kagome lattice has previously been restricted to nano-fabricated systems and spin-ice materials under applied magnetic field. Here, we show that the layered Ising magnet Dy3Mg2Sb3O14 hosts an emergent order predicted theoretically for individual kagome layers of in-plane Ising spins. Neutron-scattering and bulk thermomagnetic measurements, supported by Monte Carlo simulations, reveal a phase transition at T* = 0.3 K from a disordered spin-ice like regime to an "emergent charge ordered" state in which emergent charge degrees of freedom exhibit three-dimensional order while spins remain partially disordered. Our results establish Dy3Mg2Sb3O14 as a tuneable system to study interacting emergent charges arising from kagome Ising frustration.

cond-mat.str-el↗

arXiv2014

Enhancement of the magnetocaloric effect driven by changes in the crystal structure of Al doped GGG, Gd3Ga5-xAlxO12 (0 < x < 5)

The Gd3Ga5-xAlxO12 (0 < x < 5) solid solution has been prepared using ceramic synthesis routes and the structural and magnetic properties investigated using X-ray diffraction, magnetic susceptibility, chi, and isothermal magnetisation, M(H), measurements. Our results indicate a contraction of the unit cell and more significant antiferromagnetic interactions as x increases. Despite the decrease in the magnetic polarisation on application of a field and the corresponding decrease in the change in the magnetic entropy we find that Gd3Al5O12 has a significantly higher observed (17%) and theoretical (14%) DS per unit mass than Gd3Ga5O12. Per unit volume the theoretical increase in DS (7%) is offset by the increased antiferromagnetic interactions in Gd3Al5O12. The differences in DS are driven by a decrease in both the mass and density as Al ions replace Ga ions. These results highlight the importance of changes to the crystal structure when considering materials for solid state magnetic cooling.

cond-mat.mtrl-sci↗

arXiv2013

Spin-flop and antiferromagnetic phases of the ferromagnetic half-twist ladder compounds Ba3Cu3In4O12 and Ba3Cu3Sc4O12

The title compounds have dominant ferromagnetic (FM) exchange interactions within one-dimensional (1D) half-twist ladders of s =1/2 Cu2^{+} ions and antiferromagnetic(AFM) interactions between ladders, leading to ordered 3D phases at temperatures below 20K. Here we show that a microscopic 1D model of the paramagnetic (PM) phase combined with a phenomenological model based on sublattice magnetization describes the observed temperature and field dependent magnetism. The model identifies AFM, spin-flop (SF) and PM phases whose boundaries have sharp features in the experimental magnetization M(T,H) and specific heat CP(T,H). Exact diagonalization (ED) of the 1D model, possible for 24 spins due to special structural features of half-twist ladders, yields the magnetization and spin susceptibility of the PM phase. AFM interactions between ladders are included at the mean-field level using the field, HAF, obtained from modeling the ordered phases. Isotropic exchange J1 = -135K and g-tensor g = 2.1 within ladders, plus exchange and anisotropy fields HAF and HA, describe the ordered phases, and are almost quantitative for the PM phase.

cond-mat.str-el↗

arXiv2012

Quantum spin liquid in frustrated one dimensional LiCuSbO4

A quantum magnet, LiCuSbO4, with chains of edge-sharing S = 1/2 CuO6 octahedra is reported. While the Curie-Weiss constant is ferromagnetic, θ= 30 K, no phase transition or spin freezing occurs down to 100 mK. Specific heat indicates a distinct high field phase near the 12 T saturation field. Neutron scattering shows incommensurate spin correlations with q = 0.47\pm0.01π/a and places an upper limit of 70 \mueV on a potential spin gap. Exact diagonalization of easy plane S = 1/2 chains with competing ferro- and antiferromagnetic interactions (J1 = - 75 K, J2 = 34 K) accounts for the T > 2 K data.

cond-mat.str-el↗

arXiv2012

Dominant ferromagnetism in the spin-1/2 half-twist ladder 334 compounds, Ba3Cu3In4O12 and Ba3Cu3Sc4O12

The magnetic properties of polycrystalline samples of Ba3Cu3In4O12 (In-334) and Ba3Cu3Sc4O12 (Sc-334) are reported. Both 334 phases have a structure derived from perovskite, with CuO4 squares interconnected to form half-twist ladders along the c-axis. The Cu-O-Cu angles, ~ 90o, and the positive Weiss temperatures indicate the presence of significant ferromagnetic (FM) interactions along the Cu ladders. At low temperatures, T < 20 K, sharp transitions in the magnetic susceptibility and heat capacity measurements indicate three-dimensional (3D) antiferromagnetic (AFM) ordering at TN. TN is suppressed on application of a field and a complex magnetic phase diagram with three distinct magnetic regimes below the upper critical field can be inferred from our measurements. The magnetic interactions are discussed in relation to a modified spin-1/2 FM-AFM model and the 334 half-twist ladder is compared to other 2-rung ladder spin-1/2 systems.

cond-mat.str-el↗

arXiv2011

NaIrO3 - A pentavalent post-perovskite

Sodium iridium(V) oxide, NaIrO3, was synthesized by a high pressure solid state method and recovered to ambient conditions. It is found to be isostructural with CaIrO3, the much-studied structural analogue of the high-pressure post-perovskite phase of MgSiO3. Among the oxide post-perovskites, NaIrO3 is the first example with a pentavalent cation. The structure consists of layers of corner- and edge-sharing IrO6 octahedra separated by layers of NaO8 bicapped trigonal prisms. NaIrO3 shows no magnetic ordering and resistivity measurements show non-metallic behavior. The crystal structure, electrical and magnetic properties are discussed and compared to known post-perovskites and pentavalent perovskite metal oxides.

cond-mat.mtrl-sci↗

arXiv2011

The Sensitivity of the Magnetic Properties of the ZnCr2O4 and MgCr2O4 Spinels to Non-stoichiometry

We report that small amounts of metal atom non-stoichiometry are possible in the ZnCr2O4 and MgCr2O4 spinels. The non-stoichiometry, though less than 2%, significantly impacts TN and the nature of the magnetic correlations above TN. The Zn1+xCr2-xO4 spinel is particularly sensitive. While stoichiometric ZnCr2O4 displays antiferromagnetic short range correlations in the susceptibility above TN, ferromagnetic correlations are observed in non-stoichiometric, hole doped Zn1+xCr2-xO4. The Mg1+xCr2-xO4 spinels are less profoundly affected by non-stoichiometry, though significant changes are also observed. We contrast the magnetic properties of Zn1+xCr2-xO4 and Mg1+xCr2-xO4 (x=0, 0.02, 0.04) with those of materials with the equivalent amounts of isovalent non-magnetic Ga3+ substituted on the Cr3+ site to separate the effects of static site disorder and hole doping.

cond-mat.mtrl-sci↗

arXiv2010

Superconductivity at 2.3 K in the misfit compound (PbSe)1.16(TiSe2)2

The structural misfit compound (PbSe)1.16(TiSe2)2 is reported. It is a superconductor with a Tc of 2.3 K. (PbSe)1.16(TiSe2)2 derives from a parent compound, TiSe2, which shows a charge density wave transition and no superconductivity. The crystal structure, characterized by high resolution electron microscopy and powder x-ray diffraction, consists of two layers of 1T-TiSe2 alternating with a double layer of (100) PbSe. Transport measurements suggest that the superconductivity is induced by charge transfer from the PbSe layers to the TiSe2 layers.

cond-mat.supr-con↗

arXiv2010

Divergent effects of static disorder and hole doping in geometrically frustrated b-CaCr2O4

The gallium substituted and calcium deficient variants of geometrically frustrated b-CaCr2O4, b-CaCr2-2xGa2xO4 (0.02<= x<= 0.25) and b-Ca1-yCr2O4 (0.075<= y<= 0.15), have been investigated by x-ray powder diffraction, magnetization and specific heat measurements. This allows for a direct comparison of the effects, in a geometrically frustrated magnet, of the static disorder that arises from non-magnetic substitution and the dynamic disorder that arises from hole doping. In both cases, disturbing the Cr3+ lattice results in a reduction in the degree of magnetic frustration. On substitution of Ga, which introduces disorder without creating holes, a gradual release of spins from ordered antiferromagnetic states is observed. In contrast, in the calcium deficient compounds the introduction of holes induces static ferrimagnetic ordering and much stronger perturbations of the b-CaCr2O4 host.

cond-mat.mtrl-sci↗