Selective Generation of V2 Silicon Vacancy Centers in 4H-Silicon Carbide.

The deterministic generation of individual color centers with defined orientations or types in solid-state systems is paramount for advancements in quantum technologies. Silicon vacancies in 4H-silicon carbide (4H-SiC) can be formed in V1 and V2 types. However, silicon vacancies are typically generated randomly between V1 and V2 types with similar probabilities. Here, we show that the preferred V2 centers can be selectively generated by focused ion beam (FIB) implantation on the m-plane in 4H-SiC. When implantation is on the m-plane (a-plane), the generation probability ratio between V1 and V2 centers increase exponentially (remains constant) with decreasing FIB fluences. With a fluence of 10 ions/spot, the probability to generate V2 centers is seven times higher than V1 centers. Our results represent a critical step toward the deterministic creation of specific defect types.

Anion-Regulated Selective Generation of Cobalt Sites in Carbon: Toward Superior Bifunctional Electrocatalysis.

The introduction of active transition metal sites (TMSs) in carbon enables the synthesis of noble-metal-free electrocatalysts for clean energy conversion applications; however, there are often multiple existing forms of TMSs, which are of different natures and catalytic models. Regulating the evolution of distinctive TMSs is highly desirable but remains challenging to date. Anions, as essential elements involved in the synthesis, have been totally neglected previously in the construction of TMSs. Herein, the effects of anions on the creation of different types of TMSs are investigated for the first time. It is found that the active cobalt-nitrogen sites tend to be selectively constructed on the surface of N-doped carbon by using chloride, while metallic cobalt nanoparticles encased in protective graphite layers are the dominant forms of cobalt species with nitrate ions. The obtained catalysts demonstrate cobalt-sites-dependent activity for oxygen reduction reaction and hydrogen evolution reaction in acidic media. The remarkably enhanced catalytic activities approaching that of benchmark Pt/C in an acidic medium have been obtained on the catalyst dominated with cobalt-nitrogen sites, confirmed by the advanced spectroscopic characterization. This finding demonstrates a general paradigm of anion-regulated evolution of distinctive TMSs, providing a new pathway for enhancing performances of various targeted reactions related with TMSs.