Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.336
Publication date: 18th December 2023
Self-assembled nanocrystals (NCs) into superlattices (SLs) are alternative materials to polycrystalline films and single crystals, which can behave very differently from their constituents, especially when they interact coherently with each other, leading to collective emission, as superfluorescence [1]. In this work we concentrate on the Superradiance (SR) emission observed in SLs formed by CsPbX3 NCs synthesized by hot injection with synthesized with oleic acid and oleylamine (OA/OAM) and didodecyldimethylammonium bromide (DDAB) ligands. These SLs were studied by Photoluminescence (PL), Time Resolved PL (TRPL) and Micro-PL/TRPL spectroscopy at low and high temperatures to extract information about the SR states and uncoupled domains of NCs. In the case of CsPbBr3 SLs formed by large sized NCs we have measured very narrow (1-5 meV) emission lines on the low energy side of their µ-PL spectra, which can be considered near homogeneous, and characterized by lifetimes as short as 160 ps. The enhancement factor estimated for these low energy narrow lines can reach values as high as 10, like the value estimated from the inverse ratio of their lifetimes over that in a film, which is associated to domains of nearly identical NCs formed by 1000 to 40000 NCs within the micrometric SLs [2]. Therefore, the nature of these emission lines is consistent with a SR exciton state whose origin is due to the coupling of optical dipoles in perovskite NCs; this origin is consistent with our estimate of the correlation length for these SL domains with correlated NCs. The coherence of the SR exciton state has been studied in the temperature region dominated by a radiative recombination dynamics (from 4 to 70-80 K). The importance of thermal decoherence for the SR state is observed above 25 K and due to its coupling with an effective phonon energy of around 8 meV. The emission of high energy states in the SL spectra are also characterized by short lifetimes, because of Förster transfer of energy (from small to large NCs of the distribution or from high to low emission energies). More recent work on perovskite SLs is being directed to a better control of the SL growth and evaluating the effect of a solid-state anion state procedure [3] on initially formed CsPbBr3 SL and the optical properties of the SLs, including the superriant state.
Financial support from the Spanish Ministry of Science (MICINN) through project no. PID2020- 120484RB-I00 is gratefully acknowledged.