Congratulations to Tyler Smart and Prof. Ping for their publication, in collaboration with Dr. Tuan Anh Pham and Dr. Tadashi Ogitsu of the Quantum Simulations Group at LLNL, just accepted by Physical Review Materials Rapid Communications! Link to the full article can be found here.
Small polarons (SPs) are known to exist in most important transition metal oxides (TMOs); however, the nature of small polaron formation remains enigmatic, and a fundamental understanding of how SPs impact the intrinsic electronic structure and optical properties of these materials is largely lacking. In this work, we employ first-principles calculations to investigate SP formation in Co3O4, a highly promising material for a wide range of emerging energy applications, and we resolve the conflicting findings that have been reported on the electronic structure of the system. We confirm that the intrinsic band gap of Co3O4 is 1.6 eV, and we show that the formation of hole small polarons significantly influences the optical absorption spectra, leading to a 0.8 eV transition that is often misinterpreted as the band edge that defines the fundamental gap. In addition, we discuss how uniaxial strain can be utilized to probe the Jahn-Teller distortion of SP states and in turn, effect their optical transitions. Beyond Co3O4, our study suggests a general roadmap for establishing a first-principles computational approach that can simultaneously achieve an accurate description of SP states, electronic band structure and optical transitions of polaronic magnetic oxides.