Electronic and plasmonic phenomena at nonstoichiometric grain boundaries in metallic SrNbO3

Abstract

Grain boundaries could exhibit exceptional electronic structure and exotic properties, which are determined by a local atomic configuration and stoichiometry that differs from the bulk. However, optical and plasmonic properties at the grain boundaries in metallic oxides have rarely been discussed before. Here, we show that non-stoichiometric grain boundaries in the newly discovered metallic SrNbO₃ photocatalyst show exotic electronic, optical and plasmonic phenomena in comparison to bulk. Aberration-corrected scanning transmission electron microscopy and first-principles calculations reveal that a Nb-rich grain boundary exhibits an increased carrier concentration with quasi-1D metallic conductivity, and newly induced electronic states contributing to the broad energy range of optical absorption. More importantly, dielectric function calculations reveal extended and enhanced plasmonic excitations compared with bulk SrNbO₃. Our results show that non-stoichiometric grain boundaries might be utilized to control the electronic and plasmonic properties in oxide photocatalysis.