Accurate and efficient computation of the fundamental bandgap of the vacancy-ordered double perovskite Cs₂TiBr₆

Metal halide perovskites (MHPs) demonstrate an exceptional combination of properties. Rapid progress has extended their application beyond solar cells, light-emitting diodes, photodetectors, and lasers to include memristors, artificial synapse devices, and pressure induced emission. In particular, the vacancy-ordered double perovskite Cs₂TiBr₆ has been identified as a promising material. The effective characterization of MHPs requires accurate and efficient methods for the calculation of electronic structure. Koopmans compliant (KC) functionals are an accurate and computationally efficient alternative to many-body perturbation theory using the GW approximation but have yet only been validated on a small number of simple materials. In this work, KC functionals were applied to the more complex case of Cs₂TiBr₆ and gave a zero-temperature fundamental gap of 4.28 eV, in close agreement with the value of 4.44 eV obtained using the accurate, but more computationally expensive, evGW₀ approach. The temperature-dependent renormalization of the bandgap has also been investigated and found to be significant. Agreement with the experimental optical bandgaps of 1.76–2.0 eV would also require the inclusion of exciton binding energy.

Identifier
Source https://archive.materialscloud.org/record/2025.9
Metadata Access https://archive.materialscloud.org/xml?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:2528
Provenance
Creator Ingall, John; Linscott, Edward; Colonna, Nicola; Page, Alister; Keast, Vicki
Publisher Materials Cloud
Publication Year 2025
Rights info:eu-repo/semantics/openAccess; Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type Dataset
Discipline Materials Science and Engineering