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Helen C. Walker

Publications and source records attributed to Helen C. Walker.

33 records · Page 2Linked to original sources

Neutron diffraction evidence of the 3-dimensional structure of Ba2MnTeO6 and misidentification of the triangular layers within the face-centred cubic lattice

Ba2MnTeO6 was first characterised using X-ray diffraction and reported to show a small distortion1 from the idealised cubic perovskite which displays face-centred cubic arrangement of Mn2+. A recent report has asserted that this leads to a layered configuration of Mn2+ that serves as an example of a triangular lattice, i.e. a 2D structure containing discreet layers.2 Here we show how neutron scattering gives great confidence in establishing the crystal structure being an undistorted cubic phase and how this can be mis-assigned as a triangular layered structure. This has profound implications for the understanding of the magnetic properties of the system.

cond-mat.str-el↗

Pressure dependence of atomic dynamics in barocaloric ammonium sulfate: I. Rotations

Solid-state cooling using barocaloric materials is a promising avenue for eco-friendly, inexpensive and highly efficient cooling. To design barocaloric compounds ready for deployment, it is essential to understand their thermodynamic behaviour under working conditions. To this end, we have studied the rotational dynamics in the molecular-ionic crystal ammonium sulfate under pressure, providing detailed insight into the origin of its large barocaloric effect. Using quasielastic neutron scattering experiments, we show that rotation of the ammonium cations is facilitated by pressure in the low-entropy phase, with the rotational "hopping" motion increasing in frequency as the pressure-induced phase transition is approached. We explain this unusual behaviour in terms of the competing hydrogen-bond networks represented by the two phases. This work includes the first results of a recently developed low-background, high-pressure gas cell for neutron scattering, showcasing its power in obtaining high-precision measurements of molecular dynamics under pressure.

cond-mat.mtrl-sci↗

Neutron Scattering Studies of the Breathing Pyrochlore Antiferromagnet LiGaCr$_{4}$O$_{8}$

We report neutron scattering measurements of the spinel oxide LiGaCr$_{4}$O$_{8}$, in which magnetic ions Cr$^{3+}$ form a breathing pyrochlore lattice. Our experiments reveal the coexistence of a nearly dispersionless resonance mode and dispersive spin wave excitations in the magnetically ordered state, which can be quantitatively described by a quantum spin model of hexagonal loops and linear spin wave theory with the same set of exchange parameters, respectively. Comparison to other Cr spinel oxides reveals a linear relationship between the resonance energy and lattice constant across all these materials, which is in agreement with our hexagonal loop calculations. Our results suggest a unified picture for spin resonances in Cr spinel oxides.

cond-mat.str-el↗

Field-Tuned Quantum Effects in a Triangular-Lattice Ising Magnet

We report thermodynamic and neutron scattering measurements of the triangular-lattice quantum Ising magnet TmMgGaO 4 in longitudinal magnetic fields. Our experiments reveal a quasi-plateau state induced by quantum fluctuations. This state exhibits an unconventional non-monotonic field and temperature dependence of the magnetic order and excitation gap. In the high field regime where the quantum fluctuations are largely suppressed, we observed a disordered state with coherent magnon-like excitations despite the suppression of the spin excitation intensity. Through detailed semi-classical calculations, we are able to understand these behaviors quantitatively from the subtle competition between quantum fluctuations and frustrated Ising interactions.

cond-mat.str-el↗

Diamagnetic d-orbitals Drive Magnetic Structure Selection in the Double Perovskite Ba$_2$MnTeO$_6$

B-site ordered A$_2$B'B''O$_6$ double perovskites have a variety of applications as magnetic materials. Here we show that diamagnetic $d^{10}$ and $d^0$ B'' cations have a significant effect on the magnetic interactions in these materials. We present a neutron scattering and theoretical study of the Mn$^{2+}$ double perovskite Ba$_2$MnTeO$_6$ with a $4d^{10}$ Te$^{6+}$ cation on the B''-site. It is found to be a Type I antiferromagnet with a dominant nearest-neighbor $J_1$ interaction. In contrast, the $5d^0$ W$^{6+}$ analogue Ba$_2$MnWO$_6$ is a Type II antiferromagnet with a significant next-nearest-neighbor $J_2$ interaction. This is due to a $d^{10}$/$d^0$ effect, where the different orbital hybridization with oxygen 2p results in different superexchange pathways. We show that $d^{10}$ B'' cations promote nearest neighbor and $d^0$ cations promote next-nearest-neighbor interactions. The $d^{10}$/$d^0$ effect could be used to tune magnetic interactions in double perovskites.

cond-mat.str-el↗

Large Easy Axis Anisotropy in the One-Dimensional Magnet BaMo(PO$_4$)$_2$

We present an extensive experimental and theoretical study on the low-temperature magnetic properties of the monoclinic anhydrous alum compound BaMo(PO$_4$)$_2$. The magnetic susceptibility reveals strong antiferromagnetic interactions $θ_{CW} = -167$~K and long-range magnetic order at $T_N=22$~K, in agreement with a recent report. Powder neutron diffraction furthermore shows that the order is collinear, with the moments near the $ac$ plane. Neutron spectroscopy reveals a large excitation gap $Δ= 15$~meV in the low-temperature ordered phase, suggesting a much larger easy-axis spin anisotropy than anticipated. However, the large anisotropy justifies the relatively high ordered moment, Néel temperature, and collinear order observed experimentally, and is furthermore reproduced in a first principles calculations using a new computational scheme. We therefore propose BaMo(PO$_4$)$_2$ to host $S=1$ antiferromagnetic chains with large easy-axis anisotropy, which has been theoretically predicted to realize novel excitation continua.

cond-mat.str-el↗

Long and short range magnetism in the frustrated double perovskite Ba2MnWO6

The structural and magnetic properties of the face-centered cubic double perovskite Ba2MnWO6 were investigated using neutron powder diffraction, DC-magnetometry, muon spin relaxation and inelastic neutron scattering. Ba2MnWO6 undergoes Type II long-range antiferromagnetic ordering at a Neel temperature of 8(1) K with a frustration index, f = 8. Inelastic neutron scattering was used to identify the magnetic coupling constants J1 and J2, which were found to equal -0.080 meV and -0.076 meV respectively. This indicated that both of the magnetic coupling constants were antiferromagnetic with similar magnitudes, which is in contrast to other known 3d metal double perovskites Ba2MWO6. Above the Neel temperature, muon spin relaxation measurements and inelastic neutron scattering techniques identify a short-range correlated magnetic state that is similar to that observed in the archetypical face-centered cubic lattice antiferromagnet MnO.

cond-mat.mtrl-sci↗

Gapless spin-liquid state in the structurally disorder-free triangular antiferromagnet NaYbO$_2$

We present the structural characterization and low-temperature magnetism of the triangular-lattice delafossite NaYbO$_2$. Synchrotron x-ray diffraction and neutron scattering exclude both structural disorder and crystal-electric-field randomness, whereas heat-capacity measurements and muon spectroscopy reveal the absence of magnetic order and persistent spin dynamics down to at least 70\,mK. Continuous magnetic excitations with the low-energy spectral weight accumulating at the $K$-point of the Brillouin zone indicate the formation of a novel spin-liquid phase in a triangular antiferromagnet. This phase is gapless and shows a non-trivial evolution of the low-temperature specific heat. Our work demonstrates that NaYbO$_2$ practically gives the most direct experimental access to the spin-liquid physics of triangular antiferromagnets.

cond-mat.str-el↗

Intermultiplet transitions and magnetic long-range order in Sm-based pyrochlores

We present bulk and neutron scattering measurements performed on the isotopically enriched $^{154}\mathrm{Sm_2Ti_2O_7}$ and $^{154}\mathrm{Sm_2Sn_2O_7}$ samples. Both compounds display sharp heat capacity anomalies, at 350 mK and 440 mK, respectively. Inelastic neutron scattering measurements are employed to determine the crystalline electric field (CEF) level scheme, which includes transitions between the ground-state and first excited $J$ multiplets of the $\mathrm{Sm}^{3+}$ ion. To further validate those results, the single-ion magnetic susceptibility of the compounds is calculated and compared with the experimental DC-susceptibility measured in low applied magnetic fields. It is demonstrated that the inclusion of intermultiplet transitions in the CEF analysis is fundamental to the understanding of the intermediate and, more importantly, low temperature magnetic behaviour of the Sm-based pyrochlores. Finally, the heat capacity anomaly is shown to correspond to the onset of an all-in-all-out long-range order in the stannate sample, while in the titanate a dipolar long-range order can be only indirectly inferred.

cond-mat.str-el↗

Spin dynamics of coupled spin ladders near quantum criticality in Ba2CuTeO6

We report inelastic neutron scattering measurements of the magnetic excitations in Ba2CuTeO6, proposed by ab initio calculations to magnetically realize weakly coupled antiferromagnetic two-leg spin-1/2 ladders. Isolated ladders are expected to have a singlet ground state protected by a spin gap. Ba2CuTeO6 orders magnetically, but with a small Neel temperature relative to the exchange strength, suggesting that the interladder couplings are relatively small and only just able to stabilize magnetic order, placing Ba2CuTeO6 close in parameter space to the critical point separating the gapped phase and Neel order. Through comparison of the observed spin dynamics with linear spin wave theory and quantum Monte Carlo calculations, we propose values for all relevant intra- and interladder exchange parameters, which place the system on the ordered side of the phase diagram in proximity to the critical point. We also compare high field magnetization data with quantum Monte Carlo predictions for the proposed model of coupled ladders.

cond-mat.str-el↗

Magnetic Excitations in Non-Collinear Antiferromagnetic Weyl Semimetal $\mathsf{Mn_{3}Sn}$

$\mathsf{Mn_{3}Sn}$ has recently attracted considerable attention as a magnetic Weyl semimetal exhibiting concomitant transport anomalies at room temperature. The topology of the electronic bands, their relation to the magnetic ground state and their nonzero Berry curvature lie at the heart of the problem. The examination of the full magnetic Hamiltonian reveals otherwise hidden aspects of these unusual physical properties. Here, we report the full spin wave spectra of $\mathsf{Mn_{3}Sn}$ measured over a wide momentum - energy range by the inelastic neutron scattering technique. Using a linear spin wave theory, we determine a suitable magnetic Hamiltonian which not only explains the experimental results but also stabilizes the low-temperature helical phase, consistent with our DFT calculations. The effect of this helical ordering on topological band structures is further examined using a tight-binding method, which confirms the elimination of Weyl points in the helical phase. Our work provides a rare example of the intimate coupling between the electronic and spin degrees of freedom for a magnetic Weyl semimetal system.

cond-mat.str-el↗

Coexistence of magnetic fluctuations and long-range orders in the one-dimensional $J_1-J_2$ zigzag chains materials BaDy$_2$O$_4$ and BaHo$_2$O$_4$

The compounds BaDy$_2$O$_4$ and BaHo$_2$O$_4$ are part of a family of frustrated systems exhibiting interesting properties, including spin liquid-type ground states, magnetic field-induced phases, and the coexistence of short- and long-range magnetic orders, with dominant one-dimensional correlations, which can be described as Ising $J_1-J_2$ zigzag chains along the $c$-axis. We have investigated polycrystalline samples of BaDy$_2$O$_4$ and BaHo$_2$O$_4$ with both neutron diffraction and neutron spectroscopy, coupled to detailed crystalline electric field calculations. The latter points to site-dependent anisotropic magnetism in both materials, which is corroborated by the magnetic structures we determined. The two systems show the coexistence of two different long-range orders --- two double Néel $\uparrow\uparrow\downarrow\downarrow$ orders in the $ab$-plane with propagation vectors $\mathbf{k}_1$ = ($\frac{1}{2}$,0,$\frac{1}{2}$) and $\mathbf{k}_2$ = ($\frac{1}{2}$,$\frac{1}{2}$,$\frac{1}{2}$) for BaDy$_2$O$_4$, and two distinct arrangements of simple Néel $\uparrow\downarrow\uparrow\downarrow$ orders along the $c$-axis, both with the propagation vector $\mathbf{k}_0$ = (0,0,0) for BaHo$_2$O$_4$. The order for both wave vectors in BaDy$_2$O$_4$ occurs at $T_\mathrm{N}$ = 0.48 K, while in BaHo$_2$O$_4$, the first order sets in at $T_\mathrm{N}\sim$ 1.3 K and the second one has a lower ordering temperature of 0.84 K. Both compounds show extensive diffuse scattering which we successfully modeled with a one-dimensional axial next-nearest neighbor Ising (ANNNI) model. In both materials, strong diffusive scattering persists to temperatures well below where the magnetic order is fully saturated. The ANNNI model fits indicate the presence of sites which do not order with moments in the $ab$-plane.

cond-mat.str-el↗

Coulomb spin liquid in anion-disordered pyrochlore Tb$_2$Hf$_2$O$_7$

The charge ordered structure of ions and vacancies characterizing rare-earth pyrochlore oxides serves as a model for the study of geometrically frustrated magnetism. The organization of magnetic ions into networks of corner-sharing tetrahedra gives rise to highly correlated magnetic phases with strong fluctuations, including spin liquids and spin ices. It is an open question how these ground states governed by local rules are affected by disorder. In the pyrochlore Tb$_2$Hf$_2$O$_7$, we demonstrate that the vicinity of the disordering transition towards a defective fluorite structure translates into a tunable density of anion Frenkel disorder while cations remain ordered. Quenched random crystal fields and disordered exchange interactions can therefore be introduced into otherwise perfect pyrochlore lattices of magnetic ions. We show that disorder can play a crucial role in preventing long-range magnetic order at low temperatures, and instead induces a strongly-fluctuating Coulomb spin liquid with defect-induced frozen magnetic degrees of freedom.

cond-mat.str-el↗

Long range antiferromagnetic order of formally non-magnetic Eu$^{3+}$ Van Vleck ions observed in multiferroic Eu$_{1-x}$Y$_{x}$MnO$_3$

We report on resonant magnetic x-ray scattering and absorption spectroscopy studies of exchange-coupled antiferromagnetic ordering of Eu$^{3+}$ magnetic moments in multiferroic Eu$_{1-x}$Y$_{x}$MnO$_3$ in the absence of an external magnetic field. The observed resonant spectrum is characteristic of a magnetically ordered $^7F_1$ state that mirrors the Mn magnetic ordering, due to exchange coupling between the Eu $4f$ and Mn $3d$ spins. This is the first observation of long range magnetic order generated by exchange coupling of magnetic moments of formally non-magnetic Van Vleck ions, which is a step further towards the realization of exotic phases induced by exchange coupling in systems entirely composed of non-magnetic ions.

cond-mat.str-el↗

On the role of intrinsic disorder in the structural phase transition of magnetoelectric EuTiO3

Up to now the crystallographic structure of the magnetoelectric perovskite EuTiO3 was considered to remain cubic down to low temperature. Here we present high resolution synchrotron X-ray powder diffraction data showing the existence of a structural phase transition, from cubic Pm-3m to tetragonal I4/mcm, involving TiO6 octahedra tilting, in analogy to the case of SrTiO3. The temperature evolution of the tilting angle indicates a second-order phase transition with an estimated Tc=235K. This critical temperature is well below the recent anomaly reported by specific heat measurement at TA\sim282K. By performing atomic pair distribution function analysis on diffraction data we provide evidence of a mismatch between the local (short-range) and the average crystallographic structures in this material. Below the estimated Tc, the average model symmetry is fully compatible with the local environment distortion but the former is characterized by a reduced value of the tilting angle compared to the latter. At T=240K data show the presence of local octahedra tilting identical to the low temperature one, while the average crystallographic structure remains cubic. On this basis, we propose intrinsic lattice disorder to be of fundamental importance in the understanding of EuTiO3 properties.

cond-mat.str-el↗