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Pennycook, Stephen J

Publications and source records attributed to Pennycook, Stephen J.

At least 19 records

A pathway for the growth of core-shell Pt-Pd nanoparticles

In this study, the aging of both Pt-Pd nanoparticles and core-shell Pt-Pd nanoparticles has been reported to result in alloying of Pt with Pd. In comparison to monometallic Pt catalysts, the growth of Pd-Pt bimetallics is slower; however, the mechanism of growth of particles and the mechanism by which Pd improves the hydrothermal durability of bimetallic Pd-Pt particles remains uncertain. In our work on hydrothermal aging of core-shell Pt-Pd nanoparticles, synthesized by solution methods, with varying Pd:Pt ratio of 1:4, 1:1, and 4:1, we compare the growth of core-shell Pt-Pd nanoparticles and find that particles grow by migrating and joining together. The unique feature of the observed growth is that Pd shells from both particles open up and join, allowing the cores to merge. At high temperatures, alloying occurs in good agreement with reports by other workers.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Observation of a periodic array of flux-closure quadrants in strained ferroelectric PbTiO 3 films

Nanoscale ferroelectrics are expected to exhibit various exotic domain configurations, such as the full flux-closure pattern that is well known in ferromagnetic materials. Here we observe not only the atomic morphology of the flux-closure quadrant but also a periodic array of flux closures in ferroelectric PbTiO 3 films, mediated by tensile strain on a GdScO 3 substrate. Using aberration-corrected scanning transmission electron microscopy, we directly visualize an alternating array of clockwise and counterclockwise flux closures, whose periodicity depends on the PbTiO 3 film thickness. In the vicinity of the core, the strain is sufficient to rupture the lattice, with strain gradients up to 10 9 per meter. We found engineering strain at the nanoscale may facilitate the development of nanoscale ferroelectric devices.

36 MATERIALS SCIENCE↗

Reversible electric-field control of magnetization at oxide interfaces

Electric field control of magnetism has remained a major challenge which would greatly impact data storage technology. Although progress in this direction has been recently achieved, reversible magnetization switching by an electric field requires the assistance of a bias magnetic field. In this work, we take advantage of the novel electronic phenomena emerging at interfaces between correlated oxides and demonstrate reversible, voltage-driven magnetization switching without magnetic field. Sandwiching a (non superconducting) cuprate between two manganese oxide layers, we find a novel form of magnetoelectric coupling arising from the orbital reconstruction at the interface between interfacial Mn spins and localized states in the CuO2 planes. This results in a ferromagnetic coupling between the manganite layers that can be controlled by a voltage. Consequently, the devices can be electrically toggled between two magnetization states (and corresponding spin-dependent resistance states in magnetic tunnel junctions) in the absence of a magnetic field.

Cuellar, F. A.↗

Oxygen-Vacancy-Induced Polar Behavior in (LaFeO 3 ) 2 /(SrFeO 3 ) Superlattices

Complex oxides displaying ferroelectric and/or multiferroic behavior are of high fundamental and applied interest. In this work, for the first time, we show that it is possible to achieve polar order in a superlattice made up of two nonpolar oxides by means of oxygen vacancy ordering. Using scanning transmission electron microscopy imaging, we show the polar displacement of magnetic Fe ions in a superlattice of (LaFeO 3 ) 2 /(SrFeO 3 ) grown on a SrTiO 3 substrate. Using density functional theory calculations, we systematically study the effect of epitaxial strain, octahedral rotations, and surface terminations in the superlattice and find them to have a negligible effect on the antipolar displacements of the Fe ions lying in between SrO and LaO layers of the superlattice (i.e., within La 0.5 Sr 0.5 FeO 3 unit cells). The introduction of oxygen vacancies, on the other hand, triggers a polar displacement of the Fe ions. We confirm this important result using electron energy loss spectroscopy, which shows partial oxygen vacancy ordering in the region where polar displacements are observed and an absence of vacancy ordering outside of that area.

36 MATERIALS SCIENCE↗

Simulation of Probe Position-Dependent Electron Energy-Loss Fine Structure

We present a theoretical framework for calculating probe-position-dependent electron energy-loss near-edge structure for the scanning transmission electron microscope by combining density functional theory with dynamical scattering theory. We show how simpler approaches to calculating near-edge structure fail to include the fundamental physics needed to understand the evolution of near-edge structure as a function of probe position and investigate the dependence of near-edge structure on probe size. It is within this framework that density functional theory should be presented, in order to ensure that variations of near-edge structure are truly due to local electronic structure and how much from the diffraction and focusing of the electron beam.

Oxley, M. P.↗

p-type doping of MoS{sub 2} thin films using Nb

We report on the first demonstration of p-type doping in large area few-layer films of (0001)-oriented chemical vapor deposited MoS{sub 2}. Niobium was found to act as an efficient acceptor up to relatively high density in MoS{sub 2} films. For a hole density of 3.1 × 10{sup 20} cm{sup −3}, Hall mobility of 8.5 cm{sup 2} V{sup −1} s{sup −1} was determined, which matches well with the theoretically expected values. X-ray diffraction scans and Raman characterization indicated that the film had good out-of-plane crystalline quality. Absorption measurements showed that the doped sample had similar characteristics to high-quality undoped samples, with a clear absorption edge at 1.8 eV. Scanning transmission electron microscope imaging showed ordered crystalline nature of the Nb-doped MoS{sub 2} layers stacked in the [0001] direction. This demonstration of substitutional p-doping in large area epitaxial MoS{sub 2} could help in realizing a wide variety of electrical and opto-electronic devices based on layered metal dichalcogenides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Band Gap Engineering and Layer-by-Layer Band Gap Mapping of Selenium-doped Molybdenum Disulfide

Ternary two-dimensional dichalcogenide alloys exhibit compositionally modulated electronic structure and hence, control of dopant concentration within each layer of these layered compounds provides a powerful way to modify their properties. The challenge then becomes quantifying and locating the dopant atoms within each layer in order to better understand and fine-tune the desired properties. Here we report the synthesis of selenium substitutionally doped molybdenum disulfide atomic layers, with a broad range of selenium concentrations, resulting in band gap modulations of over 0.2 eV. Atomic scale chemical analysis using Z-contrast imaging provides direct maps of the dopant atom distribution in individual MoS2 layers and hence a measure of the local band gaps. Furthermore, in a bilayer structure, the dopant distribution of each layer is imaged independently. We demonstrate that each layer in the bilayer contains similar doping levels, randomly distributed, providing new insights into the growth mechanism and alloying behavior in two-dimensional dichalcogenide atomic layers. The results show that growth of uniform, ternary, two-dimensional dichalcogenide alloy films with tunable electronic properties is feasible.

Gong, Yongji↗