Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.025
Publication date: 16th December 2024
There is recent evidence that, upon polaron formation, excitonic interactions in bulk lead halide perovskites experience different dielectric screening at short and long distances.[1,2] Above the polaron radius, static dielectric screening prevails. Under the polaron radius, dynamic screening prevails instead.
Here we investigate how such non-hydrogenic interactions affect the electronic structure of excitons, trions and biexcitons in confined halide perovskites: nanoplatelets and nanocrystals. To do so we develop a theoretical model which accounts for the main physical factors in these systems: (i) quantum confinement, through k·p theory, (ii) dielectric confinement, through image charge methods, (iii) electronic correlations, through a variational Quantum Monte Carlo method, and (iv) polaronic interactions, through Haken-like potentials.
We show that trions are formed by an exciton plus an excess carrier orbiting at longer distances, which reveals a significant ionic character of the bond. Biexcitons are formed by two excitons with strong intra-exciton interactions, and weaker inter-exciton ones. Polaronic interactions lead to large binding energies for excitons, trions and biexcitons. These are in good agreement with experimental measurements of nanoplatelets and Ruddlesden-Popper perovskites.[3-5] For nanocrystals, however, biexciton binding energies are systematically smaller than experimental values. This suggests excitons and biexcitons polarize the lattice differently.
We acknowledge support from Grant No. PID2021-128659NB-I00, funded by Ministerio de Ciencia e Innovación (MCIN/AEI/10.13039/501100011033 and ERDF A way of
making Europe)