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Abstract:

The local atomic and magnetic structures of the compounds AMnO₂ (A = Na, Cu), which realize a geometrically frustrated, spatially anisotropic triangular lattice of Mn spins, have been investigated by atomic and magnetic pair distribution function analysis of neutron total scattering data. Relief of frustration in CuMnO₂ is accompanied by a conventional cooperative symmetry-lowering lattice distortion driven by N'eel order. In NaMnO₂, however, the distortion has a short-range nature. A cooperative interaction between the locally broken symmetry and short-range magnetic correlations lifts the magnetic degeneracy on a nanometer length scale, enabling long-range magnetic order in the Na-derivative. The degree of frustration, mediated by residual disorder, contributes to the rather differing pathways to a single, stable magnetic ground state in these two related compounds. This study demonstrates how nanoscale structural distortions that cause local-scale perturbations can lift the ground state degeneracy and trigger macroscopic magnetic order.

Abstract:

The relevance of magnetic, structural, orbital, and charge degrees of freedom in the iron-based superconductors (FeSCs) and related materials occupies a central focus in condensed matter physics. While the majority of iron-based materials exhibit the same two-dimensional iron square lattice structural motif, a family of AFe₂X₃ (X = Se,S) compounds introduces a quasi-one-dimensional (1D) ladder motif, which resembles the two-legged spin ladder copper oxide materials. Furthermore, unlike most parent compounds of FeSCs, the members of this spin ladder family are insulators. Recently, a superconducting transition has been observed under pressure with T_c up to 24 K, similar to the pressure-induced superconductivity in the copper oxide ladder Sr_14−xCa_xCu₂₄O₄₁ material, stimulating much interest. Here, we review the magnetic, structural, and electronic properties in this family, particularly in the BaFe₂X₃ series tuned by pressure and by chemical substitution. The established pressure-temperature (P-T) and carrier concentration-temperature (x-T) phase diagrams in related materials provide useful information to extend the variety of high-temperature superconductors and compare with other FeSCs. We also review some essential information about analogous square lattice FeSCs.

Abstract:

We present a coordinated study of the paramagnetic-to-antiferromagnetic, rhombohedral-to-monoclinic, and metal-to-insulator transitions in thin-film specimens of the classic Mott insulator using low-energy muon spin relaxation, x-ray diffraction, and nanoscale-resolved near-field infrared spectroscopic techniques. The measurements provide a detailed characterization of the thermal evolution of the magnetic, structural, and electronic phase transitions occurring in a wide temperature range, including quantitative measurements of the high- and low-temperature phase fractions for each transition. The results reveal a stable coexistence of the high- and low-temperature phases over a broad temperature range throughout the transition. Careful comparison of temperature dependence of the different measurements, calibrated by the resistance of the sample, demonstrates that the electronic, magnetic, and structural degrees of freedom remain tightly coupled to each other during the transition process. We also find evidence for antiferromagnetic fluctuations in the vicinity of the phase transition, highlighting the important role of the magnetic degree of freedom in the metal-insulator transition.

Abstract: The majority of the iron-based superconductors (FeSCs) exhibit a two-dimensional square lattice structure. Recent reports of pressure-induced superconductivity in the spin-ladder system, BaFe₂X₃ (X=S, Se), introduce a quasi-one-dimensional prototype and an insulating parent compound to the FeSCs. Here we report x-ray, neutron diffraction, and muon spin relaxation experiments on BaFe₂Se₃ under hydrostatic pressure to investigate its magnetic and structural properties across the pressure-temperature phase diagram. A structural phase transition was found at a pressure of 3.7(3) GPa. Neutron diffraction measurements at 6.8(3) GPa and 120 K show that the block magnetism persists even at these high pressures. A steady increase and then fast drop of the magnetic transition temperature T_N and greatly reduced moment above the pressure P_s indicate potentially rich and competing phases close to the superconducting phase in this ladder system.

Abstract: Neutron and x-ray total scattering measurements have been performed on powder samples of the iron chalcogenide superconductor FeSe. Using pair distribution function analysis of the total scattering data to investigate short-range atomic correlations, we establish the existence of an instantaneous, local orthorhombic structural distortion attributable to nematic fluctuations that persists well into the high-temperature tetragonal phase, at least up to 300 K and likely to significantly higher temperatures. This short-range orthorhombic distortion is correlated over a length scale of about 1 nm at 300 K and grows to several nm as the temperature is lowered toward the long-range structural transition temperature. In the low-temperature nematic state, the local instantaneous structure exhibits an enhanced orthorhombic distortion relative to the average structure with a typical relaxation length of 3 nm. The quantitative characterization of these orthorhombic fluctuations sheds light on nematicity in this canonical iron-based superconductor.

Abstract:

We present a methodology based on ex situ (postgrowth) electrochemistry to control the oxygen concentration in thin films of the superconducting oxide La2CuO_4+y grown epitaxially on substrates of isostructural LaSrAlO₄. The superconducting transition temperature, which depends on the oxygen concentration, can be tuned by adjusting the pH level of the base solution used for the electrochemical reaction. As our main finding, we demonstrate that the dopant oxygens can either occupy the interstitial layer in an orientationally disordered state or organize into a crystalline phase via a mechanism in which dopant oxygens are inserted into the substrate, changing the lattice symmetry of both the substrate and the epitaxial film. We discuss this mechanism, and we describe the resulting methodology as a platform to be explored in thin films of other transition-metal oxides.