Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.248
Publication date: 22nd December 2022
All-inorganic lead-halide perovskite (CsPbX3, X = Cl, Br, I) quantum dots (QDs) have emerged as a competitive platform for classical light emitting devices (in the weak light-matter interaction regime, e.g., LEDs and laser)[1], as well as for devices exploiting strong light-matter interaction and operated at room-temperature.[2] Many-body interactions and quantum correlations among photogenerated exciton complexes play an essential role, e.g., by determining the laser threshold, the overall brightness of LEDs, and the single-photon purity[3, 4] in quantum light sources. Here, by combining single-QD optical spectroscopy performed at cryogenic temperatures in combination with configuration interaction (CI) calculations, we address the trion and biexciton binding energies and unveil their peculiar size dependence. We find that trion binding energies increase from 7 meV to 17 meV for QD sizes decreasing from 30 nm to 9 nm, while the biexciton binding energies increase from 15 meV to 30 meV, respectively. CI calculations quantitatively corroborate the experimental results and suggest that the effective dielectric constant for biexcitons slightly deviates from the one of the single excitons, potentially as a result of coupling to the lattice in the multiexciton regime. Our findings provide a deep insight into the multiexciton properties in all-inorganic lead-halide perovskite QDs, essential for classical and quantum optoelectronic devices.
The authors acknowledge Dr. Frank Krumeich for having performed TEM characterization on the studied QDs. This project was funded by the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the grant agreement No 899141 (PoLLoC). J.E. acknowledges financial support from the Institute Universitaire de France. C.Z, M.I.B. and G.R. acknowledge funding from the Swiss National Science Foundation (Grant No. 200021_192308, "Q-Light - Engineered Quantum Light Sources with Nanocrystal Assemblies"). The project was also partially supported by the Air Force Office of Scientific Research and the Office of Naval Research under award number FA8655-21-1-7013 and by the Swiss National Science Foundation (Grant No. 188404, "Novel inorganic light emitters: synthesis, spectroscopy and applications").
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