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Register a new userSolute effects on interfacial dislocation emission in nanomaterials: nucleation site competition and neutralization
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Interfacial nucleation is the dominant process of dislocation generation during the plastic deformation of nano-crystalline materials. Solute additions intended to stabilize nano-crystalline metals against grain growth, may segregate to the grain boundaries and triple junctions where they can affect the process of the dislocation emission. In this Letter we demonstrate that the effect of solute addition in a nano-crystalline material containing competing solute segregation sites and dislocation sources can be very complex due to different rates of segregation at different interfaces. Moreover, at large concentrations, when the solutes form clusters near the grain boundaries or triple junctions, the interfaces between these clusters and the matrix can introduce new dislocation emission sources, which can be activated under lower applied stress. Thus, the strength maximum can occur at a certain solute concentration: adding solutes beyond this optimal solute concentration can reduce the strength of the material.
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The origin of the $3 times 1$ reconstruction observed in epitaxial LaCoO$_{3}$ films on SrTiO$_3(001)$ is assessed by using first-principles calculations including a Coulomb repulsion term. We compile a phase diagram as a function of the oxygen pressure, which shows that ($3 times 1$)-ordered oxygen vacancies (LaCoO$_{2.67}$) are favored under commonly used growth conditions, while stoichiometric films emerge under oxygen-rich conditions. Growth of further reduced LaCoO$_{2.5}$ brownmillerite films is impeded by phase separation. We report two competing ground-state candidates for stoichiometric films: a semimetallic phase with $3 times 1$ low-spin/intermediate-spin/intermediate-spin magnetic order and a semiconducting phase with intermediate-spin magnetic order. This demonstrates that tensile strain induces ferromagnetism even in the absence of oxygen vacancies. Both phases exhibit an intriguing ($3 times 1$)-reconstructed octahedral rotation pattern and accordingly modulated La-La distances. In particular, charge and bond disproportionation and concomitant orbital order of the $t_{2g}$ hole emerge at the Co sites that are also observed for unstrained bulk LaCoO$_3$ in the intermediate-spin state and explain structural data obtained by x-ray diffraction at elevated temperature. Site disproportionation drives a metal-to-semiconductor transition that reconciles the intermediate-spin state with the experimentally observed low conductivity during spin-state crossover without Jahn-Teller distortions.
We report on detailed structural, electronic and magnetic studies of GdMn$_{1-x}$Cr$_x$O$_3$ for Cr doping levels 0 $le$ $x$ $le$ 1. In the solid solutions, the Jahn-Teller distortion associated with Mn$^{3+}$ ions gives rise to major changes in the ${bc}$-plane sub-lattice and also the effective orbital ordering in the ${ab}$-plane, which persist up to the compositions $x$ $sim$ 0.35. These distinct features in the lattice and orbital degrees of freedom are also correlated with $bc$-plane anisotropy of the local Gd environment. A gradual evolution of electronic states with doping is also clearly seen in O $K$-edge x-ray absorption spectra. Evidence of magnetization reversal in field-cooled-cooling mode for $x$ $ge$ 0.35 coinciding the Jahn-Teller crossover, suggests a close correlation between magnetic interaction and structural distortion. These observations indicate a strong entanglement between lattice, spin, electronic and orbital degrees of freedom. The nonmonotonic variation of remnant magnetization can be explained by doping induced modification of magnetic interactions. Density functional theory calculations are consistent with a layer-by-layer type doping with ferromagnetic (antiferomagnetic) coupling between Mn (Cr) ions for intermediate compound ($x$ = 0.5), which is distinct from that observed for the end members GMnO$_3$ and GdCrO$_3$.
This report classifies emission inhomogeneities that manifest in InGaN quantum well blue light-emitting diodes grown by plasma-assisted molecular beam epitaxy on free-standing GaN substrates. By a combination of spatially resolved electroluminescence and cathodoluminescence measurements, atomic force microscopy, scanning electron microscopy and hot wet KOH etching, the identified inhomogeneities are found to fall in four categories. Labeled here as type I through IV, they are distinguishable by their size, density, energy, intensity, radiative and electronic characteristics and chemical etch pits which correlates them with dislocations. Type I exhibits a blueshift of about 120 meV for the InGaN quantum well emission attributed to a perturbation of the active region, which is related to indium droplets that form on the surface in the metal-rich InGaN growth condition. Specifically, we attribute the blueshift to a decreased growth rate of and indium incorporation in the InGaN quantum wells underneath the droplet which is postulated to be the result of reduced incorporated N species due to increased N$_{2}$ formation. The location of droplets are correlated with mixed type dislocations for type I defects. Types II through IV are due to screw dislocations, edge dislocations, and dislocation bunching, respectively, and form dark spots due to leakage current and nonradiative recombination.
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