Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.255
Publication date: 6th July 2018
Hot carriers refer to electrons (holes) that are formed from the thermalization of non-equilibrium photoexcited carrier populations following the absorption of above-bandgap photons. These hot carriers (HCs) later equilibrate within few picoseconds with the semiconductor lattice through carrier cooling processes such as carrier phonon scattering, Auger process, etc. The mechanisms and dynamics of HC cooling in semiconductors are of fundamental importance for enhancing device functionalities. Colloidal lead halide perovskite nanocrystals recently emerged as promising candidate materials for many optoelectronic applications. Building efficient and long-lasting devices from perovskite nanocrystals however remains a challenge. In this work, we study the size and temperature dependent cooling process of HC in CsPbBr3 nanocrystals using time-domain density functional theory. We provide detailed insights into the mechanism of cooling by analyzing the effect of the passivating ligands (alkyl ammonium) in this process. We demonstrate that the inorganic lattice plays a much larger role in mediating the thermalization to the band edge.
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