Strain tuned structural, mechanical, electronic, and optical properties of lead-free oxy-nitride SrTaO2N perovskite using first-principles study

Recent advancements in perovskite-based solar energy conversion technologies require materials having enhanced optoelectronic properties and stability. Harnessing density functional theory (DFT), we have investigated here a novel orthorhombic phase of a recently synthesized oxynitride perovskite, SrTaO2N, and its uniaxial strain-tunable electronic and optical properties. Phonon dispersion and formation energy calculations are utilized to determine lattice dynamic stability and exothermic formation feasibility of the structure, correspondingly. The predicted bandgap at the Heyd–Scuseria–Ernzerhof [generalized gradient approximation Perdew–Burke–Ernzerhof (GGA-PBE)] level is ∼2.125 eV (∼1.125 eV), which is highly receptive to uniaxial strains. The bandgap formed in between X and G points with high symmetry at the first Brillouin zone was further dissected using the atomic orbital projected density of states (PDOS). The PDOS showed that the N-pz orbital dominantly contributes to valence band maxima and the Ta-dz2 orbital to conduction band minima. Compressive uniaxial strain widens the bandgap by ∼1.21 times, while tensile uniaxial strain lowers the bandgap by ∼1.1 times from the intrinsic value, suggesting strain switchable bandgap nature in the material. An elastic constant matrix also evaluates the mechanical stability of strained structures, and we found that in the strained structures from −6% to +6%, SrTaO2N is mechanically stable and ductile. Optical absorption reveals an increased absorption coefficient in the visible spectrum. These strain-tuned optoelectronic properties through the DFT approach thus suggest an evident route to a wide range of optoelectronics applications of the SrTaO2N perovskite material.