Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.168
Publication date: 23rd September 2021
Cesium lead halide perovskite nanocrystals are a highly attractive class of materials for coherent light emission, with implications for lasing, light-emitting diodes, and quantum computing. Fine-tuning their properties for the above applications requires an exact understanding of their exciton fine structure, in particular, spacing and polarization of their triplet and singlet states. Experimental reports have been controversial, implicating that the Rashba effect may be inducing an inversion in the order of bright and dark states.
To aid in the resolution of this debate, we performed investigation of the fine structure of the triplet emission properties in these materials. Using the wave functions generated via DFT calculations including spin-orbit coupling for cubic, orthorhombic and tetragonal caesium lead halide perovskite nanocrystals of ~3 nm in diameter, we further augmented them with Coulomb coupling between the exciton configurations, to resolve the absorption and emission fine structure in a configuration interaction method.
We anticipate our work will aid in the resolution of the debated emission fine structure of CsPbBr3 nanocrystals and thereafter allow for the development of bright materials for optoelectronics.
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