Composition Dependent Strain Engineering of Lead-Free Halide Double Perovskite: Computational Insights

The critical photophysical properties of lead-free halide double perovskites (HDPs) must be substantially improved for various applications. In this regard, strain engineering is a powerful tool for enhancing optoelectronic performance with precise control. Here, we employ ab initio simulations to investigate the impact of mild compressive and tensile strains on the photophysics of Cs2AgB′X6 (B′ = Sb, Bi; X = Cl, Br) perovskites. Depending on the pnictogen and halide atoms, the band gap and band edge positions of HDPs can be tuned to a significant extent by controlling the applied external strain. Cs2AgSbBr6 has the most substantial strain response under structural perturbations. The subtle electronic interactions among the participating orbitals and the band dispersion at the edge states are enhanced under compressive strain, reducing the carrier effective masses. The exciton binding energies for these Br-based HDPs are in the range 59–78 meV and weaken in the compressed lattices, suggesting improved free carrier generation. Overall, the study emphasizes the potential of lattice strain engineering to boost the photophysical properties of HDPs that can ultimately improve their optoelectronic performance