posted on 2023-11-21, 12:35authored byDallas
P. Strandell, Patanjali Kambhampati
Metal
halide perovskite nanocrystals are under intense investigation
for their outstanding optical and electronic properties. The presence
of higher fine structure states, let alone nonequilibrium processes
within the fine structure, and multiexcitonic fine structure remains
poorly understood due to a lack of experimental probes. Here, we use
time-resolved photoluminescence (t-PL) spectroscopy with an improvement
from 100 to 3 ps resolution which reveals previously unobserved spectral
dynamics from excitons to multiexcitons in 15 nm CsPbBr3 nanocrystals. The simple and immediate observation from temperature
dependence is a previously unobserved fine structure to the multiexcitons.
Further insight is gleaned from t-PL spectral bandwidth trajectories
at extrema in temperature and exciton density. The bandwidth trajectories
reveal the presence of a previously unobserved fine structure in excitons
as well as multiexcitons. The bandwidth trajectories reveal a complex
history, from multiexciton recombination to exciton thermalization
to Auger heating to lattice thermalization. Whereas the amplitude
of these spectral effects is large, ∼60 meV, modeling suggests
that the spectral effects are mostly phonon based illustrating the
importance of the lattice on light emission from metal halide perovskite
nanocrystals.