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Understanding the microscopic origin of the superior electromechanical response in relaxor ferroelectrics requires knowledge not only of the atomic-scale formation of polar nanodomains (PNDs) but also the rules governing the arrangements and stimulated response of PNDs over longer distances. Using x-ray coherent nanodiffraction, we show the staggered self-assembly of PNDs into unidirectional mesostructures that we refer to as polar laminates in the relaxor ferroelectric 0.68PbMg1/3Nb2/3O3-0.32PbTiO3(PMN-0.32PT). We reveal the highly heterogeneous electric-field–driven responses of intra- and interlaminate PNDs and establish their correlation with the local strain and the nature of the PND walls. Our observations highlight the critical role of hierarchical lattice organizations on macroscopic material properties and provide guiding principles for the understanding and design of relaxors and a wide range of quantum and functional materials.more » « less
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We report the discovery of a novel form of Ruddlesden–Popper (RP) nickelate that stands as the first example of long-range, coherent polymorphism in this class of inorganic solids. Rather than the well-known, uniform stacking of perovskite blocks ubiquitously found in RP phases, this newly discovered polymorph of the bilayer RP phase La3Ni2O7 adopts a novel stacking sequence in which single-layer and trilayer blocks of NiO6 octahedra alternate in a “1313” sequence. Crystals of this new polymorph are described in space group Cmmm, although we note evidence for a competing Imam variant. Transport measurements at ambient pressure reveal metallic character with evidence of a charge density wave transition with an onset at T ≈ 134 K. The discovery of such polymorphism could reverberate to the expansive range of science and applications that rely on RP materials, particularly the recently reported signatures of superconductivity in bilayer La3Ni2O7 with Tc as high as 80 K above 14 GPa.more » « less
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Abstract The family of transition-metal dipnictides has been of theoretical and experimental interest because this family hosts topological states and extremely large magnetoresistance (MR). Recently, , a member of this family, has been predicted to support a topological crystalline insulating state. Here, by using high-resolution angle-resolved photoemission spectroscopy (ARPES), we reveal both closed and open pockets in the metallic Fermi surface (FS) and linearly dispersive bands on the ( ) surface, along with the presence of extreme MR observed from magneto-transport measurements. A comparison of the ARPES results with first-principles computations shows that the linearly dispersive bands on the measured surface of are trivial bulk bands. The absence of symmetry-protected surface state on the ( ) surface indicates its topologically dark nature. The presence of open FS features suggests that the open-orbit fermiology could contribute to the extremely large MR of .more » « less
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none (Ed.)The recent prediction that honeycomb lattices of Co2+ (3d7) ions could host dominant Kitaev interactions provides an exciting direction for exploration of new routes to stabilizing Kitaev’s quantum spin liquid in real materials. Na3Co2SbO6 has been singled out as a potential material candidate provided that spin and orbital moments couple into a Jeff = 1/2 ground state, and that the relative strength of trigonal crystal field and spin-orbit coupling acting on Co ions can be tailored. Using x-ray linear dichroism (XLD) and x-ray magnetic circular dichroism (XMCD) experiments, alongside configuration interaction calculations, we confirm the counterintuitive positive sign of the trigonal crystal field acting on Co2+ ions and test the validity of the Jeff = 1/2 description of the electronic ground state. The results lend experimental support to recent theoretical predictions that a compression (elongation) of CoO6 octahedra along (perpendicular to) the trigonal axis would drive this cobaltate toward the Kitaev limit, assuming the Jeff = 1/2 character of the electronic ground state is preserved.more » « less
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