Excitonic Properties and Optical Signatures in Quasi-1D Metal-Halide Perovskites with Tunable Octahedral Connectivity (2506.07762v1)

Abstract: Reducing the dimensionality of metal-halide perovskites enhances quantum and dielectric confinement, enabling tunable excitonic properties. In one dimension, the arrangement of metal-halide octahedra in chains with corner-, edge-, or face-sharing connectivity allows for additional structural flexibility. This not only expands material design possibilities but also reflects quasi-one-dimensional motifs that arise during perovskite formation but are poorly understood. Using first-principles many-body perturbation theory within the $GW$ and Bethe-Salpeter Equation framework, we provide a comprehensive picture of how one-dimensional confinement, octahedral connectivity and dielectric screening affect optical absorption and exciton photophysics in these materials. Our calculations reveal that increasing octahedral connectivity leads to increased exciton binding and complex, anisotropic optical signatures. However, in experimental compounds, pronounced dielectric screening effects can shift exciton binding energies by several hundred meV, altering these trends. These findings offer insights and design principles for excitonic properties, and aid the interpretation of optical experiments on one-dimensional perovskites.