DOI: https://doi.org/10.29363/nanoge.emlem.2022.034
Publication date: 15th July 2022
In the current context of rising popularity of perovskites as excellent materials for optoelectronics, inorganic lead halide perovskite (CsPbX3, X=Cl, Br, I) quantum dots constitute a promising platform for light emitting devices thanks to their emission spectra having extensive coverage of frequencies with narrow band as well as their photoluminescence (PL) quantum yield approaching 100% [1]. Understanding light-matter coupling and the various many-body effects is at the core of realizing the full potential of perovskite quantum dots as both classical and quantum light sources [2,3]. Many-body interaction is notably important not only for single-exciton PL [4] but also for the emission energies of trion and biexciton systems [5]. For this purpose, we utilize the Configuration Interaction (CI) approach to study the binding energies of these multiexcitonic complexes. Corroborating the experimental findings from single-dot spectroscopy, our calculations quantitatively reproduce the measured redshifts of the trion and biexciton relative to the single exciton emission from CsPbX3 quantum dots [6]. Additionally, the same theoretical method can also be employed to explain the sub-nanosecond exciton radiative lifetime in these fascinating materials [4].
[1] “Light Generation in Lead Halide Perovskite Nanocrystals: LEDs, Color Converters, Lasers, and Other Applications”, Yan, F. et al., Small 2019, https://onlinelibrary.wiley.com/doi/full/10.1002/smll.201902079
[2] “Coherent single-photon emission from colloidal lead halide perovskite quantum dots”, Utzat, H. et al., Science 2019, https://www.science.org/doi/10.1126/science.aau7392
[3] “The dark exciton ground state promotes photon-pair emission in individual perovskite nanocrystals”, Tamarat, P. et al., Nature Communications 2020, https://www.nature.com/articles/s41467-020-19740-7
[4] “Bright triplet excitons in caesium lead halide perovskites”, Becker, M. A. et al., Nature 2018, https://www.nature.com/articles/nature25147
[5] “Calculation of the biexciton shift in nanocrystals of inorganic perovskites”, Nguyen, T. P. T. et al., Phys. Rev. B 2020, https://journals.aps.org/prb/abstract/10.1103/PhysRevB.101.125424
[6] “Many-body Correlations and Bound Exciton Complexes in CsPbX3 (X=Br, Br/Cl) Quantum Dots”, Zhu, C. et al., in preparation
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).
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