2024/01/11 by Prakriti Kayastha, Kayastha, Prakriti, Giulia Longo +3
Engineering · Materials Science · #FOS: Physical sciences #Intermetallics and Advanced Alloy Properties #Materials Science (cond-mat.mtrl-sci) #Nuclear Materials and Properties #Thermal and Kinetic Analysis
paper · pdf · doi:10.48550/arxiv.2401.06092
openalex publication_date 2024/01/11 · openalex created_date 2024/01/13 · openalex updated_date 2026/08/01
The chalcogenide perovskite BaZrS3 has strong visible light absorption and high chemical stability, is nontoxic, and is made from earth-abundant elements. As such, it is a promising candidate material for application in optoelectronic technologies. However the synthesis of BaZrS3 thin-films for characterisation and device integration remains a challenge. Here we use density functional theory and lattice dynamics to calculate the vibrational properties of elemental, binary and ternary materials in the Ba-Zr-S system. This is used to build a thermodynamic model for the stability of BaZrS3, BaSx, and ZrSx in equilibrium with sulfur gas, across a range of temperatures and sulfur partial pressures. We highlight that reaction thermodynamics are highly sensitive to sulfur allotrope and the extent of allotrope mixing. We use our model to predict the synthesis conditions in which BaZrS3 and the intermediate binary compounds can form. At a moderate temperature of 500 °C we find that BaS3, associated with fast reaction kinetics, is stable at pressures above 3x105 Pa. We also find BaZrS3 is stable against decomposition into sulfur-rich binaries up to at least 1x107 Pa. Our work provides insights into the chemistry of this promising material and suggests the experimental conditions required for the successful synthesis of BaZrS3.