Ultrafast Carrier Dynamics of Dual Emissions from the Orthorhombic Phase in Methylammonium Lead Iodide Perovskites Revealed by Two-Dimensional Coherent Spectroscopy

The fundamental understanding of photoexcitation landscape and dynamics in hybrid organic-inorganic perovskites is essential for improving their performance in solar cells and other applications. The dual emission features from the orthorhombic phase in perovskites have been the focus of numerous recent studies, and yet their underlying molecular origin remains elusive. We use optical two-dimensional coherent spectroscopy to study the carrier dynamics and coupling of the dual emissions in a methylammonium lead iodide film at 115 K. The two-dimensional spectra reveal an ultrafast redistribution of the photoexcited carriers into the two emission resonances within 250 fs. The high-energy resonance is a short-lived transient state, and the low-energy emission state interacts with coherent phonons. The observed carrier dynamics provide important experimental evidence that can be compared with potential theoretical models and contribute to the understanding of the dual emissions as well as the overall energy level structure in hybrid organic-inorganic perovskites.