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The discovery of hydrogen‐induced electron localization and highly insulating states in d‐band electron correlated perovskites has opened a new paradigm for exploring novel electronic phases of condensed matters and applications in emerging field‐controlled electronic devices (e.g., Mottronics). Although a significant understanding of doping‐tuned transport properties of single crystalline correlated materials exists, it has remained unclear how doping‐controlled transport properties behave in the presence of planar defects. The discovery of an unexpected high‐concentration doping effect in defective regions is reported for correlated nickelates. It enables electronic conductance by tuning the Fermi‐level in Mott–Hubbard band and shaping the lower Hubbard band state into a partially filled configuration. Interface engineering and grain boundary designs are performed for H_xSmNiO₃/SrRuO₃heterostructures, and a Mottronic device is achieved. The interfacial aggregation of hydrogen is controlled and quantified to establish its correlation with the electrical transport properties. The chemical bonding between the incorporated hydrogen with defective SmNiO₃is further analyzed by the positron annihilation spectroscopy. The present work unveils new materials physics in correlated materials and suggests novel doping strategies for developing Mottronic and iontronic devices via hydrogen‐doping‐controlled orbital occupancy in perovskite heterostructures.

 

ABSTRACT In the search for chemically stable two-dimensional (2D) materials with high in-plane mobility, proper bandgap, and compatibility with vapor-based fabrication, van der Waals semiconductor SiP has become a potential candidate as a robust variation of black phosphorous. While bulk SiP crystals were synthesized in the 1970s, the vapor-based synthesis of SiP nanostructures or thin films is still absent. We here report the first chemical vapor growth of SiP nanostructures on SiO 2 /Si substrate. SiP islands with lateral size up to 20 μm and showing well-defined Raman signals were grown on SiO 2 /Si substrate or on SiP-containing concentric rings. The presence of SiP phase is confirmed by XRD. The formation of rings and islands is explained by a multiple coffee ring growth model where a dynamic fluctuation of droplet growth front induces the topography of concentric ring surfaces. This new growth method might shed light on the controlled growth of group IV-III high-mobility 2D semiconductors.