Carrier-Carrier vs Carrier-Phonon Interactions in Lead-halide Perovskite Materials: Role of Carrier Density, Nanoconfinement, and Surface Ligands
Artem Bakulin a
a Department of Chemistry and Centre for Plastic Electronics, Imperial College London, South Kensington Campus, London, United Kingdom
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting19 (NFM19)
#Exciup19. Excitonic up-downconversion
Berlin, Germany, 2019 November 3rd - 8th
Invited Speaker, Artem Bakulin, presentation 117
DOI: https://doi.org/10.29363/nanoge.nfm.2019.117
Publication date: 18th July 2019

The major efficiency limit in conventional solar cells is imposed by the rapid relaxation of above-bandgap “hot” carriers via electron-phonon coupling. To battle this limitation a number of non-trival photophysical phenonmena are investigated including singlet fission, carrier multiplication and hot carrier extraction. Lead-halide perovskites (LHPs) currently hold the efficiency record for solution-processable solar cells, and previous observations of slow hot-carrier cooling in these materials have piqued a deeper interest into their application in disruptive next-generation photovoltaics. However a coherent picture of carrier-carrier and carrier-phonon interactions in these systems is still under development.

Here we implement an ultrafast “pump-push-probe” technique to study the sub-ps cooling in LHP materials and use the observed cooling dynamics as probes for carrier-carrier and carrier-phonon interactions. We demonstrate that cooling in the all-inorganic CsPbBr3 is slower than its hybrid counterparts (e.g. FAPbBr3) in the high carrier density regime, owing to the relative abundance of optical phonon modes associated with the organic cation. The specific rates of cooling and their dependence on the hot and cold carrier densities are used to extract polaron sizes and coupling parameters for different perovskite materials. We scrutinise the thermal equilibration between cold and hot states in the single- and multiple-exciton-per-NC cases, and remark on the effect of surface ligands on the cooling dynamics.

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