Correlating electromechanical and dielectric properties with nanometre-scale order is the definin... more Correlating electromechanical and dielectric properties with nanometre-scale order is the defining challenge for the development of piezoelectric oxides. Current lead (Pb)-based relaxor ferroelectrics can serve as model systems with which to unravel these correlations, but the nature of the local order and its relation to material properties remains controversial. Here we employ recent advances in diffuse scattering instrumentation to investigate crystals that span the phase diagram of PbMgNbO-xPbTiO (PMN-xPT) and identify four forms of local order. From the compositional dependence, we resolve the coupling of each form to the dielectric and electromechanical properties observed. We show that relaxor behaviour does not correlate simply with ferroic diffuse scattering; instead, it results from a competition between local antiferroelectric correlations, seeded by chemical short-range order, and local ferroic order. The ferroic diffuse scattering is strongest where piezoelectricity is ...
Most of the searches for Kitaev materials deal with $4d/5d$ magnets with spin-orbit-coupled ${J=1... more Most of the searches for Kitaev materials deal with $4d/5d$ magnets with spin-orbit-coupled ${J=1/2}$ local moments such as iridates and $\alpha$-RuCl$_3$. Here we propose a new Kitaev material candidate YbCl$_3$. We perform thermodynamic, $ac$ susceptibility, angle-dependent magnetic torque measurements and neutron diffraction on YbCl$_3$ single crystal. We find that the Yb$^{3+}$ ion exhibits a Kramers doublet ground state that gives rise to an effective spin ${J_{\text{eff}}=1/2}$ local moment with likely strong anisotropic exchange interactions. The compound exhibits short-range magnetic order below 1.20 K followed by a N\'eel-type antiferromagnetic long-range order at 0.60 K, which is proved by single crystal neutron diffraction. These orders can be suppressed by in-plane and out-of-plane magnetic fields at around 6 and 10 T, respectively. Moreover, N\'eel temperature varies non-monotonically under the out-of-plane magnetic fields. The in-plane magnetic anisotropy and t...
This study investigates magnetic ordering temperature in nano- and mesoscale structural features ... more This study investigates magnetic ordering temperature in nano- and mesoscale structural features in an iron arsenide. Although magnetic ground states in quantum materials can be theoretically predicted from known crystal structures and chemical compositions, the ordering temperature is harder to pinpoint due to potential local lattice variations that calculations may not account for. In this work we find surprisingly that a locally disordered material can exhibit a significantly larger Néel temperature (TN) than an ordered material of precisely the same chemical stoichiometry. Here, a EuFe2As2 crystal, which is a ‘122’ parent of iron arsenide superconductors, is found through synthesis to have ordering below TN = 195 K (for the locally disordered crystal) or TN = 175 K (for the ordered crystal). In the higher TN crystals, there are shorter planar Fe-Fe bonds [2.7692(2) Å vs. 2.7745(3) Å], a randomized in-plane defect structure, and diffuse scattering along the [00 L] crystallographi...
The presence of a large applied magnetic field removes the degeneracy of the vacuum energy states... more The presence of a large applied magnetic field removes the degeneracy of the vacuum energy states for spin-up and spin-down neutrons. For polarized neutron reflectometry, this must be included in the reference potential energy of the Schrödinger equation that is used to calculate the expected scattering from a magnetic layered structure. For samples with magnetization that is purely parallel or antiparallel to the applied field which defines the quantization axis, there is no mixing of the spin states (no spin-flip scattering) and so this additional potential is constant throughout the scattering region. When there is non-collinear magnetization in the sample, however, there will be significant scattering from one spin state into the other, and the reference potentials will differ between the incoming and outgoing wavefunctions, changing the angle and intensities of the scattering. The theory of the scattering and recommended experimental practices for this type of measurement are p...
Correlating electromechanical and dielectric properties with nanometre-scale order is the definin... more Correlating electromechanical and dielectric properties with nanometre-scale order is the defining challenge for the development of piezoelectric oxides. Current lead (Pb)-based relaxor ferroelectrics can serve as model systems with which to unravel these correlations, but the nature of the local order and its relation to material properties remains controversial. Here we employ recent advances in diffuse scattering instrumentation to investigate crystals that span the phase diagram of PbMgNbO-xPbTiO (PMN-xPT) and identify four forms of local order. From the compositional dependence, we resolve the coupling of each form to the dielectric and electromechanical properties observed. We show that relaxor behaviour does not correlate simply with ferroic diffuse scattering; instead, it results from a competition between local antiferroelectric correlations, seeded by chemical short-range order, and local ferroic order. The ferroic diffuse scattering is strongest where piezoelectricity is ...
Most of the searches for Kitaev materials deal with $4d/5d$ magnets with spin-orbit-coupled ${J=1... more Most of the searches for Kitaev materials deal with $4d/5d$ magnets with spin-orbit-coupled ${J=1/2}$ local moments such as iridates and $\alpha$-RuCl$_3$. Here we propose a new Kitaev material candidate YbCl$_3$. We perform thermodynamic, $ac$ susceptibility, angle-dependent magnetic torque measurements and neutron diffraction on YbCl$_3$ single crystal. We find that the Yb$^{3+}$ ion exhibits a Kramers doublet ground state that gives rise to an effective spin ${J_{\text{eff}}=1/2}$ local moment with likely strong anisotropic exchange interactions. The compound exhibits short-range magnetic order below 1.20 K followed by a N\'eel-type antiferromagnetic long-range order at 0.60 K, which is proved by single crystal neutron diffraction. These orders can be suppressed by in-plane and out-of-plane magnetic fields at around 6 and 10 T, respectively. Moreover, N\'eel temperature varies non-monotonically under the out-of-plane magnetic fields. The in-plane magnetic anisotropy and t...
This study investigates magnetic ordering temperature in nano- and mesoscale structural features ... more This study investigates magnetic ordering temperature in nano- and mesoscale structural features in an iron arsenide. Although magnetic ground states in quantum materials can be theoretically predicted from known crystal structures and chemical compositions, the ordering temperature is harder to pinpoint due to potential local lattice variations that calculations may not account for. In this work we find surprisingly that a locally disordered material can exhibit a significantly larger Néel temperature (TN) than an ordered material of precisely the same chemical stoichiometry. Here, a EuFe2As2 crystal, which is a ‘122’ parent of iron arsenide superconductors, is found through synthesis to have ordering below TN = 195 K (for the locally disordered crystal) or TN = 175 K (for the ordered crystal). In the higher TN crystals, there are shorter planar Fe-Fe bonds [2.7692(2) Å vs. 2.7745(3) Å], a randomized in-plane defect structure, and diffuse scattering along the [00 L] crystallographi...
The presence of a large applied magnetic field removes the degeneracy of the vacuum energy states... more The presence of a large applied magnetic field removes the degeneracy of the vacuum energy states for spin-up and spin-down neutrons. For polarized neutron reflectometry, this must be included in the reference potential energy of the Schrödinger equation that is used to calculate the expected scattering from a magnetic layered structure. For samples with magnetization that is purely parallel or antiparallel to the applied field which defines the quantization axis, there is no mixing of the spin states (no spin-flip scattering) and so this additional potential is constant throughout the scattering region. When there is non-collinear magnetization in the sample, however, there will be significant scattering from one spin state into the other, and the reference potentials will differ between the incoming and outgoing wavefunctions, changing the angle and intensities of the scattering. The theory of the scattering and recommended experimental practices for this type of measurement are p...
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