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We have investigated the magnetic ground state of the antiferromagnetic Kondo-lattice compounds CeMAl$_{4}$Si$_{2}$ (M = Rh, Ir) using neutron powder diffraction. Although both of these compounds show two magnetic transitions $T_{N1}$ and $T_{N2}$ in the bulk properties measurements, evidence for magnetic long-range order was only found below the lower transition $T_{N2}$. Analysis of the diffraction profiles reveals a commensurate antiferromagnetic structure with a propagation vector $mathbf{k}$= (0, 0, 1/2). The magnetic moment in the ordered state of CeRhAl$_{4}$Si$_{2}$ and CeIrAl$_{4}$Si$_{2}$ were determined to be 1.14(2) and 1.41(3) $mu_{B}$/Ce, respectively, and are parallel to the crystallographic $c$-axis in agreement with magnetic susceptibility measurements.
Enhanced coupling of material properties offers new fundamental insights and routes to multifunctional devices. In this context 5d oxides provide new paradigms of cooperative interactions driving novel emergent behavior. This is exemplified in 5d osm ates that host a metal-insulator transition (MIT) driven by magnetic order. Here we consider the most robust case, the 5d perovskite NaOsO3, and reveal a giant coupling between spin and phonon through a frequency shift of {Delta}{omega}=40 cm-1, the largest measured in any material. We identify the dominant octahedral breathing mode and show isosymmetry with spin ordering which induces dynamic charge disproportionation that sheds new light on the MIT. The occurrence of the dramatic spin-phonon-electronic coupling in NaOsO3 is due to a property common to all 5d materials: the large spatial extent of the 5d ion. This allows magnetism to couple to phonons on an unprecedented scale and consequently offers multiple new routes to enhanced coupled phenomena.
The layered 5d transition metal oxide Sr2IrO4 has been shown to host a novel Jeff=1/2 Mott spin orbit insulating state with antiferromagnetic ordering, leading to comparisons with the layered cuprates. Here we study the effect of substituting Mn for Ir in single crystals of Sr2Ir0.9Mn0.1O4 through an investigation involving bulk measurements and resonant x-ray and neutron scattering. We observe a new long range magnetic structure emerge upon doping through a reordering of the spins from the basal plane to the c-axis with a reduced ordering temperature compared to Sr2IrO4. The strong enhancement of the magnetic x-ray scattering intensity at the L3 edge relative to the L2 edge indicates that the Jeff=1/2 state is robust and capable of hosting a variety of ground states.
The metal-insulator transition (MIT) is one of the most dramatic manifestations of electron correlations in materials. Various mechanisms producing MITs have been extensively considered, including the Mott (electron localization via Coulomb repulsion ), Anderson (localization via disorder) and Peierls (localization via distortion of a periodic 1D lattice). One additional route to a MIT proposed by Slater, in which long-range magnetic order in a three dimensional system drives the MIT, has received relatively little attention. Using neutron and X-ray scattering we show that the MIT in NaOsO3 is coincident with the onset of long-range commensurate three dimensional magnetic order. Whilst candidate materials have been suggested, our experimental methodology allows the first definitive demonstration of the long predicted Slater MIT. We discuss our results in the light of recent reports of a Mott spin-orbit insulating state in other 5d oxides.
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