Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.276
Publication date: 18th July 2023
Nanocrystals (NCs) have become a key component in lead halide perovskite-based devices due to their outstanding optoelectronic properties. While colloidal synthesis has reached an impressive level of maturity in less than a decade allowing for the fabrication of stable NCs with near unity quantum yield (QY), other fabrication approaches have emerged over the past few years. Among them, the synthesis within nanoporous matrices allows obtaining stable and ligand-free pNCs within thin films with optical quality perfectly suited for integration into devices. [1] Beyond the possibility of employing these films as active layers for solar cells with good efficiency [2] they represent an ideal test bench for exploring light matter interaction at the nanoscale in lead halide perovskites without ligand or solvent induced effects characteristic of colloidal NCs. [3]
In this work, we present a study on charge carrier recombination in FAPbBr3 NCs assemblies synthesized within metal-oxide porous matrices where interparticle distance is controlled via changes in the pore filling fraction. A broad photophysical characterization comprising time resolved absorption and emission spectroscopies as a function of temperature and fluence is employed to study the different recombination pathways of photogenerated carriers. We observe a transition from isolated emitters to interconnected NCs that preserve confinement effects while allowing for long range electronic transport. We show how interconnectivity determines charge carrier dynamics as it affects trap filling, radiative recombination and multiparticle interactions. These results are discussed in terms of recombination and diffusion models for both the isolated and interconnected case and study the transition between these scenarios. These findings provide an insight into the photophysical properties of an exciting nanostructured material in a configuration suited to be incorporated into a device.
Financial support of the Spanish Ministry of Science and Innovation under grants PID2020-116593RB-I00 and TED2021-129679B-C22, funded by MCIN/AEI/ 10.13039/501100011033 and by Unión Europea NextGenerationEU/PRTR, as well as of the Junta de Andalucía under grant P18-RT-2291 (FEDER/UE) is gratefully acknowledged. This research has also been supported by the Innovative Training Network Persephone ITN, which is funded from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 956270.
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