Many-body Correlations and Exciton Complexes in CsPbBr3 Quantum Dots
Résumé
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.