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BaTiO3 is typically a strong n-type material with tuneable optoelectronicproperties via doping and controlling the synthesis conditions. It has a wideband gap that can only harness the ultraviolet region of the solar spectrum.Despite significant progress, achieving visible-light absorbing BTO withtuneable carrier concentration has been challenging, a crucial requirement formany applications. In this work, a p-type BTO with visible-light absorption isrealized via iridium doping. Detailed analysis using advanced spectroscopytools and computational electronic structure analysis is used to rationalizethe n- to p-type transition after Ir doping. Results offered mechanisticinsight into the interplay between the dopant site occupancy, the dopantposition within the band gap, and the defect chemistry affecting the carrierconcentration. A decrease in the Ti3+ donor levels concentration and themutually correlated oxygen vacancies upon Ir doping is attributed to the p-typebehavior. Due to the formation of Ir3+ or Ir4+ in-gap energy levels within theforbidden region, the optical transition can be elicited from or to such levelsresulting in visible-light absorption. This newly developed Ir-doped BTO can bea promising p-type perovskite-oxide with imminent applications in solar fuelgeneration, spintronics and optoelectronics.

Iridium-doping as a strategy to realize visible light absorption and p-type behavior in BaTiO3