The fate of optical excitons in FAPbI3 nanocube superlattices
arxiv(2024)
摘要
Understanding the nature of the photoexcitation and ultrafast charge dynamics
pathways in organic halide perovskite superlattices is key for their potential
applications as tunable light emitters, photon harvesting materials and
light-amplification systems. In this work we apply two-dimensional coherent
electronic spectroscopy (2DES) to track in real time the formation of
near-infrared optical excitons and their ultrafast decay into bi-excitons in
CH(NH2)2PbI3 nanocube superlattices. On the picosecond timescale, the strong
coupling between localized charges and specific lattice distortions leads to
the progressive formation of long-lived localized trap states. The analysis of
the temperature dependence of the excitonic intrinsic linewidth, as extracted
by the anti-diagonal components of the 2D spectra, unveils a dramatic change of
the excitonic coherence time across the cubic to tetragonal structural
transition. Our results offer a new way to control and enhance the ultrafast
coherent dynamics of photocarrier generation in hybrid halide perovskite
synthetic solids.
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