Exciton-Exciton and Exciton-Lattice Interactions in 2D and 0D Perovskites
William Tisdale a
a Massachusetts Institute of Technology (MIT), Massachusetts Avenue, 77, Cambridge, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting19 (NFM19)
#PERInt19. Interplay of composition, structure and electronic properties in halide-perovskites
Berlin, Germany, 2019 November 3rd - 8th
Organizer: Pablo P. Boix
Oral, William Tisdale, presentation 090
DOI: https://doi.org/10.29363/nanoge.nfm.2019.090
Publication date: 18th July 2019

When fabricated in a nanostructured form – either as layered 2D quantum wells or colloidal nanocrystals – hybrid perovskite nanomaterials exhibit a combination of interesting properties revealing both quantum mechanical and classical composite effects. In this talk, I will discuss the thermal, vibrational, and excitonic properties of hybrid perovskite nanomaterials as a function of composition, structure, and temperature. In particular, I will discuss ultrafast spectroscopic studies of exciton-lattice interactions in 2D Ruddlesden-Popper perovskites and the unique behavior of biexcitons in colloidal CsPbBr3 nanocrystals. Using a combination of excited state resonant impulsive stimulated Raman scattering (RISRS), low-frequency Raman scattering, density functional theory (DFT), and temperature-dependent photoluminescence, we investigate the effect of organic cation size on exciton-phonon coupling in a series of 2D lead iodide perovskites. We find that inorganic cage motion dominates excited state dynamics in this family, with minimal contribution from the organic cations. In CsPbBr3 nanocrystals, we analyze fluence-dependent transient absorption data to extract the overlapping spectra of exciton and biexciton states while making no assumptions about their spectral lineshapes. From the size-dependence of these spectra, we make conclusions about the nature of exciton-exciton interactions in these colloidal systems and how they differ from conventional II-VI quantum dots.

This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under award no. DE-SC0019345.

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