Magnetic structure of Ba(TiO)Cu4_4(PO4_4)4_4 probed using spherical neutron polarimetry

The antiferromagnetic compound Ba(TiO)Cu$_4$(PO$_4$)$_4$ contains square cupola of corner-sharing CuO$_4$ plaquettes, which were proposed to form effective quadrupolar order. To identify the magnetic structure, we have performed spherical neutron polarimetry measurements. Based on symmetry analysis and careful measurements we conclude that the orientation of the Cu$^{2+}$ spins form a non-collinear in-out structure with spins approximately perpendicular to the CuO$_4$ motif. Strong Dzyaloshinskii-Moriya interaction naturally lends itself to explain this phenomenon. The identification of the ground state magnetic structure should serve well for future theoretical and experimental studies into this and closely related compounds.Comment: 9 pages, 4 figure

AA-cation control of magnetoelectric quadrupole order in AA(TiO)Cu4_4(PO4_4)4_4 (AA = Ba, Sr, and Pb)

Ferroic magnetic quadrupole order exhibiting macroscopic magnetoelectric activity is discovered in the novel compound $A$(TiO)Cu$_4$(PO$_4$)$_4$ with $A$ = Pb, which is in contrast with antiferroic quadrupole order observed in the isostructural compounds with $A$ = Ba and Sr. Unlike the famous lone-pair stereochemical activity which often triggers ferroelectricity as in PbTiO$_3$, the Pb$^{2+}$ cation in Pb(TiO)Cu$_4$(PO$_4$)$_4$ is stereochemically inactive but dramatically alters specific magnetic interactions and consequently switches the quadrupole order from antiferroic to ferroic. Our first-principles calculations uncover a positive correlation between the degree of $A$-O bond covalency and a stability of the ferroic quadrupole order.Comment: 7 pages, 4 figure

Spinon localization in the heat transport of the spin-1/2 ladder compound (C5_5H12_{12}N)2_2CuBr4_4

We present experiments on the magnetic field-dependent thermal transport in the spin-1/2 ladder system (C$_5$H$_{12}$N)$_2$CuBr$_4$. The thermal conductivity $\kappa(B)$ is only weakly affected by the field-induced transitions between the gapless Luttinger-liquid state realized for $B_{c1}< B < B_{c2}$ and the gapped states, suggesting the absence of a direct contribution of the spin excitations to the heat transport. We observe, however, that the thermal conductivity is strongly suppressed by the magnetic field deeply within the Luttinger-liquid state. These surprising observations are discussed in terms of localization of spinons within finite ladder segments and spinon-phonon umklapp scattering of the predominantly phononic heat transport.Comment: 4 pages, 3 figure

Chromium at High Pressures: Weak Coupling and Strong Fluctuations in an Itinerant Antiferromagnet

The spin- and charge-density-wave order parameters of the itinerant antiferromagnet chromium are measured directly with non-resonant x-ray diffraction as the system is driven towards its quantum critical point with high pressure using a diamond anvil cell. The exponential decrease of the spin and charge diffraction intensities with pressure confirms the harmonic scaling of spin and charge, while the evolution of the incommensurate ordering vector provides important insight into the difference between pressure and chemical doping as means of driving quantum phase transitions. Measurement of the charge density wave over more than two orders of magnitude of diffraction intensity provides the clearest demonstration to date of a weakly-coupled, BCS-like ground state. Evidence for the coexistence of this weakly-coupled ground state with high-energy excitations and pseudogap formation above the ordering temperature in chromium, the charge-ordered perovskite manganites, and the blue bronzes, among other such systems, raises fundamental questions about the distinctions between weak and strong coupling.Comment: 11 pages, 9 figures (8 in color

The J_{eff}=1/2 insulator Sr3Ir2O7 studied by means of angle-resolved photoemission spectroscopy

The low-energy electronic structure of the J_{eff}=1/2 spin-orbit insulator Sr3Ir2O7 has been studied by means of angle-resolved photoemission spectroscopy. A comparison of the results for bilayer Sr3Ir2O7 with available literature data for the related single-layer compound Sr2IrO4 reveals qualitative similarities and similar J_{eff}=1/2 bandwidths for the two materials, but also pronounced differences in the distribution of the spectral weight. In particuar, photoemission from the J_{eff}=1/2 states appears to be suppressed. Yet, it is found that the Sr3Ir2O7 data are in overall better agreement with band-structure calculations than the data for Sr2IrO4.Comment: 5 pages, 3 figure

Magnetodielectric detection of magnetic quadrupole order in Ba(TiO)Cu4_4(PO4_4)4_4 with Cu4_4O12_{12} square cupolas

In vortex-like spin arrangements, multiple spins can combine into emergent multipole moments. Such multipole moments have broken space-inversion and time-reversal symmetries, and can therefore exhibit linear magnetoelectric (ME) activity. Three types of such multipole moments are known: toroidal, monopole, and quadrupole moments. So far, however, the ME-activity of these multipole moments has only been established experimentally for the toroidal moment. Here, we propose a magnetic square cupola cluster, in which four corner-sharing square-coordinated metal-ligand fragments form a noncoplanar buckled structure, as a promising structural unit that carries an ME-active multipole moment. We substantiate this idea by observing clear magnetodielectric signals associated with an antiferroic ME-active magnetic quadrupole order in the real material Ba(TiO)Cu$_4$(PO$_4$)$_4$. The present result serves as a useful guide for exploring and designing new ME-active materials based on vortex-like spin arrangements.Comment: 4 figure