A systematic and comprehensive understanding of different
aspects
of the carrier dynamics of lead halide perovskite nanocrystals (LHP
NCs) is the key to improving the performance of this highly anticipated
material. Recent research suggests that the A-site cation of LHP materials
has a significant effect on their photophysical processes, but there
is still a lack of a systematic study on how the A-site cation affects
their biexciton dynamics. Herein, we fabricated CsPbBr3, MAPbBr3, and FAPbBr3 NCs with similar sizes
and morphologies and conducted femtosecond transient absorption (FTA)
experiments on them. By a global analysis, we found that all the FTA
spectra of CsPbBr3, MAPbBr3, and FAPbBr3 NCs include three decay-associated spectra (DAS) components
under high pump fluence, which, respectively, are attributed to hot
carrier cooling, biexciton Auger recombination (AR), and exciton recombination.
By analyzing the DAS component of biexciton of CsPbBr3,
MAPbBr3, and FAPbBr3 NCs, we extract their biexciton
AR lifetime and biexciton binding energy. It is found that the biexciton
AR lifetime of APbBr3 NCs becomes shorter as the A-site
cation changes from Cs+ to MA+ and to FA+ (∼77 ps for CsPbBr3, ∼56 ps for
MAPbBr3, and ∼42 ps for FAPbBr3), while
the biexciton binding energy of APbBr3 NCs becomes greater
as the A-site cation changes from Cs+ to MA+ and to FA+ (∼32 meV for CsPbBr3, ∼39
meV for MAPbBr3, and ∼45 meV for FAPbBr3). We also investigated how the A-site cation of APbBr3 NCs affects their hot carriers cooling time and found a consistent
result as the literature’s report (J. Am. Chem. Soc. 2019,
141, 3532–3540).