Exciton and Charge Carrier Nonlinear Dynamics in Hybrid Organic-Inorganic Metal Halides
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Rojas Gatjens, Jorge Esteban
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Abstract
Hybrid-organic inorganic metal-halide semiconductors pose an interesting photophysical scenario. Due to the ionic and dynamic nature of the structure, their excited-state properties are highly correlated with the structure's vibrations, distortions, and solvation dynamics. This thesis studies the interactions between excited states (nonlinear dynamics), their manifestation in physical observables, and their relation to the material's structure and fabrication. We explore the exciton and charge carrier nonlinear dynamics, via incoherent and coherent spectroscopy, in hybrid organic-inorganic mixed-halide lead perovskites, Ruddlesden-Popper metal halides, and perovskite nanocrystals. The many-body interactions manifest in incoherent spectroscopy as nonlinearities in the photoluminescence and/or photocurrent and, in two-dimensional coherent spectroscopy lineshapes, in the spectral linewidth, phase, and many-particle state feature (e.g. biexcitons, trions). For bulk hybrid organic-inorganic mixed-halide lead perovskites, we resolve incoherent nonlinear dynamics with sub-picosecond resolution in the photoluminescence and photocurrent. We were able to characterize the competition between defect-assisted recombination, Auger recombination, and amplified spontaneous emission. For the Ruddlesden-Popper metal halide perovskites and perovskite nanocrystals, we used two-dimensional coherent spectroscopy to explore ultrafast exciton scattering events and exciton-carrier coupling dictating the exciton-quantum dynamics. The work of this thesis sheds light on the many-body interactions in hybrid-organic inorganic metal-halide semiconductors and provides the tools to transition from the description to the control of nonlinear dynamics.
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2024-04-27
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Dissertation