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Size-Dependent Biexciton Spectrum in CsPbBr3 Perovskite Nanocrystals
journal contribution
posted on 2019-10-11, 20:44 authored by Matthew
N. Ashner, Katherine E. Shulenberger, Franziska Krieg, Eric R. Powers, Maksym V. Kovalenko, Moungi G. Bawendi, William A. TisdaleWe
characterize exciton–exciton interactions in weakly confined
CsPbBr3 nanocrystals by combining fluence-dependent transient
absorption spectroscopy with a robust spectral deconvolution method.
This data-driven approach allows for the extraction of overlapping
transient absorption spectra of exciton and biexciton states while
making no assumptions about the spectral line shape. The ensemble
spectrum of the biexciton state is found to be broader and blue-shifted
from the spectrum of the exciton state, with both effects becoming
more prominent as nanocrystal size decreases. We conclude that exciton–exciton
interactions in CsPbBr3 are net repulsive at room temperature,
but red-shifted optical gain from the biexciton state is still possible
because the spectral broadening exceeds the blue-shifting. Finally,
we extract size-dependent biexciton lifetimes of 35–200 ps,
increasing with nanocrystal size. In contrast to the attractive exciton–exciton
interactions found in most conventional semiconductor nanocrystals,
repulsive exciton–exciton interactions may arise from polaron
formation in perovskites. These observations provide important insight
into lasing, high-flux emission, and multicarrier interactions in
this class of materials.