Revealing and Manipulating Hidden Fine-Structure Coherence of Bright Excitons in CsPbI3 Perovskite Quantum Dots

Nano Lett. 2024 Oct 31. doi: 10.1021/acs.nanolett.4c04772. Online ahead of print.

Abstract

Observation and understanding of fine-structure splitting of bright excitons in lead halide perovskite quantum dots (QDs) are crucial to their emerging applications in quantum light sources and exciton coherence manipulation. Recent studies demonstrate that ensemble-level polarization-resolved transient absorption spectroscopy can reveal the quantum beats arising from the coherence between two fine-structure levels. Here we report the observation of an extra fine-structure quantum coherence hidden in previous studies by using cryo-magnetic quantum beat spectroscopy. In ∼6 nm CsPbI3 QDs, two splitting energies of 0.25 and 1.20 meV were observed at 1.7 K, which gradually increased to 0.74 and 1.55 meV, respectively, when a longitudinal magnetic field up to 7 T was applied. The field dependence allowed us to extract two distinct nominal Landé g-factors corresponding to QDs with different orientations with respect to the external field.

Keywords: cryo-magnetic spectroscopy; exciton coherence; exciton fine-structure splitting; perovskite quantum dots.