Search for: All records

Despite the well-known tendency for many alloys to undergo ordering transformations, the microscopic mechanism of ordering and its dependence on alloy composition remains largely unknown. Using the example of Pt 85 Fe 15 and Pt 65 Fe 35 alloy nanoparticles (NPs), herein we demonstrate the composition-dependent ordering processes on the single-particle level, where the nanoscale size effect allows for close interplay between surface and bulk in controlling the phase evolution. Using in situ electron microscopy observations, we show that the ordering transformation in Pt 85 Fe 15 NPs during vacuum annealing occurs via the surface nucleation and growth of L1 2 -ordered Pt 3 Fe domains that propagate into the bulk, followed by the self-sacrifice transformation of the surface region of the L1 2 Pt 3 Fe into a Pt skin. By contrast, the ordering in Pt 65 Fe 35 NPs proceeds via an interface mechanism by which the rapid formation of an L1 0 PtFe skin occurs on the NPs and the transformation boundary moves inward along with outward Pt diffusion. Although both the “nucleation and growth” and the “interface” mechanisms result in a core–shell configuration with a thin Pt-rich skin, Pt 85 Fe 15 NPs have an L1 2 Pt 3 Fe core, whereas Pt 65 Fe 35 NPs are composed of an L1 0 PtFe core. Using atomistic modeling, we identify the composition-dependent vacancy-assisted counterdiffusion of Pt and Fe atoms between the surface and core regions in controlling the ordering transformation pathway. This vacancy-assisted diffusion is further demonstrated by oxygen annealing, for which the selective oxidation of Fe results in a large number of Fe vacancies and thereby greatly accelerates the transformation kinetics. 

Hydrogen-doped perovskites can be reconfigured by electrical pulses to take on all essential functions necessary for artificial intelligence hardware. 

Ternary III-nitride-based nanowires with highly efficient light-emitting properties are essential for a broad range of applications. By using the selective area molecular-beam epitaxy method, InGaN/AlGaN quantum disks (QDs) embedded in hexagonal GaN nanowires were successfully grown. With the help of atomic-scale-resolved transmission electron microscopy and atom probe tomography, atomic ordering and other related structural information, such as crystallography and local chemistry, have been unambiguously revealed to provide unique insights into the exceptionally strong photoluminescence enhancements. A boomerang-shaped InGaN/AlGaN QD was identified, and atomic-level 1 : 1 periodic chemical ordering within the boomerang shaped AlGaN layers along the c -direction was revealed, confirming the preferential site occupation of Al-atoms. This type of growth provides a strong suppression of the quantum-confined Stark effect and is thus likely a very strong contributor to the exceptional properties. This work therefore enables us to directly establish the key structural elements necessary to understand the exceptionally strong emission exhibited by these materials. Optimization of the configurations of QDs could be an alternative design tool for developing various advanced LED device applications with well-designed structure and desirable optical properties. 

Due to the increasing desire for nanoscale optoelectronic devices with green light emission capability and high efficiency, ternary III‐N‐based nanorods are extensively studied. Many efforts have been taken on the planar device configuration, which lead to unavoided defects and strains. With selective‐area molecular‐beam epitaxy, new “Russian Doll”‐type InGaN/AlGaN quantum wells (QWs) have been developed, which could largely alleviate this issue. This work combines multiple nanoscale characterization methods and k∙p theory calculations so that the crystalline structure, chemical compositions, strain effects, and light emission properties can be quantitatively correlated and understood. The 3D structure and atomic composition of these QWs are retrieved with transmission electron microscopy and atom probe tomography while their green light emission has been demonstrated with room‐temperature cathodoluminescence experiments. k∙p theory calculations, with the consideration of strain effects, are used to derive the light emission characteristics that are compared with the local measurements. Thus, the structural properties of the newly designed nanorods are quantitatively characterized and the relationship with their outstanding optical properties is described. This combined approach provides an innovative way for analyzing nano‐optical‐devices and new strategies for the structure design of light‐emitting diodes.