Continuous advancement in nonvolatile and morphotropic beyond-Moore electronic devices requires integration of ferroelectric and semiconductor materials. The emergence of hafnium oxide (HfO 2 )–based ferroelectrics that are compatible with atomic-layer deposition has opened interesting and promising avenues of research. However, the origins of ferroelectricity and pathways to controlling it in HfO 2 are still mysterious. We demonstrate that local helium (He) implantation can activate ferroelectricity in these materials. The possible competing mechanisms, including He ion–induced molar volume changes, vacancy redistribution, vacancy generation, and activation of vacancy mobility, are analyzed. These findings both reveal the origins of ferroelectricity in this system and open pathways for nanoengineered binary ferroelectrics.

Exsolution of excess transition metal cations from a non-stoichiometric perovskite oxide has sparked interest as a facile route for the formation of stable nanoparticles on the oxide surface. However, the atomic-scale mechanism of this nanoparticle formation remains largely unknown. The present in situ scanning transmission electron microscopy combined with density functional theory calculation revealed that the anti-phase boundaries (APBs) characterized by the a/2 < 011> type lattice displacement accommodate the excess B-site cation (Ni) through the edge-sharing of BO6 octahedra in a non-stoichiometric ABO3 perovskite oxide (La0.2Sr0.7Ni0.1Ti0.9O3-δ) and provide the fast diffusion pathways for nanoparticle formation by exsolution. Moreover, the APBs further promote the outward diffusion of the excess Ni toward the surface as the segregation energy of Ni is lower at the APB/surface intersection. The formation of nanoparticles occurs through the two-step crystallization mechanism, i.e., the nucleation of an amorphous phase followed by crystallization, and via reactive wetting on the oxide support, which facilitates the formation of a stable triple junction and coherent interface, leading to the distinct socketing of nanoparticles to the oxide support. The atomic-scale mechanism unveiled in this study can provide insights into the design of highly stable nanostructures.

The spontaneous formation of electronic orders is a crucial element for understanding complex quantum states and engineering heterostructures in 2D materials. A novel 19$\sqrt {19} $ ×19$\sqrt {19} $ charge order in few‐layer‐thick 1T‐TaTe2 transition metal dichalcogenide films grown by molecular beam epitaxy, which has not been realized, is report. The photoemission and scanning probe measurements demonstrate that monolayer 1T‐TaTe2 exhibits a variety of metastable charge density wave orders, including the 19$\sqrt {19} $ × 19$\sqrt {19} $ superstructure, which can be selectively stabilized by controlling the post‐growth annealing temperature. Moreover, it is found that only the 19$\sqrt {19} $ × 19$\sqrt {19} $ order persists in 1T‐TaTe2 films thicker than a monolayer, up to 8 layers. The findings identify the previously unrealized novel electronic order in a much‐studied transition metal dichalcogenide and provide a viable route to control it within the epitaxial growth process.

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