Publication date: 21st July 2025
Excitons, neutral quasiparticles formed by electron-hole pairs, play a key role in the optoelectronic properties of semiconductors. Understanding their formation, transport, and dissociation is essential for interpreting experiments, predicting material behavior, and designing new materials for targeted applications. Low-dimensional halide perovskite semiconductors provide a versatile platform for studying excitons due to their structural tunability and facile fabrication. Quasi-two-dimensional (2D) halide perovskites, consisting of metal-halide octahedral layers separated by organic spacers, are particularly promising. Their unique structure, which disrupts octahedral connectivity in one direction, results in anisotropic charge-carrier masses and dielectric screening, promoting the formation of strongly bound excitons. First-principles calculations of excitonic properties in these materials have been limited by the large unit-cell sizes of most experimentally synthesized quasi-2D perovskites. However, recent advances in hardware and many-body perturbation theory methods, such as the GW and Bethe-Salpeter Equation approaches, now enable detailed insights into these systems. In this presentation, I will showcase how these methods allow for a microscopic understanding of the emergence of intra-, interlayer and charge-transfer excitons and their coupling to lattice degrees of freedom in low-dimensional halide perovskites. Our calculations provide predictive accuracy, explain experimental observations, and open pathways for tuning excitonic properties in these complex, heterogeneous materials.
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