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Ultra–Broadband Two–Dimensional Electronic Spectroscopy and Pump–Probe Microscopy of Molecular Systems

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Ultrafast spectroscopy offers an unprecedented view on the dynamic nature of chemical reactions. From charge transfer in semiconductors to folding and isomerization of proteins, these all important processes can now be monitored and in some instances even controlled on real, physical timescales. One of the biggest challenges of ultrafast science is the incredible energetic complexity of most systems. It is not uncommon to encounter macromolecules or materials with absorption spectra spanning significant portions of the visible spectrum. Monitoring a multitude of electronic and vibrational transitions, all dynamically interacting with each other on femtosecond timescales poses a truly daunting experimental task. The first part of this thesis deals with the development of a novel Two–Dimensional Electronic Spectroscopy (2DES) and its associated, advanced detection methodologies. Owing to its ultra–broadband implementation, this technique enables us to monitor femtosecond chemical dynamics that span the energetic landscape of the entire visible spectrum. In order to demonstrate the utility of our method, we apply it to two laser dye molecules, IR–144 and Cresyl Violet. Variation of photophysical properties on a microscopic scale in either man–made or naturally occurring systems can have profound implications on how we understand their macroscopic properties. Recently, inorganic hybrid perovskites have been tapped as the next generation solar energy harvesting materials. Their remarkable properties include low exciton binding energy, low exciton recombination rates and long carrier diffusionlengths. Nevertheless, considerable variability in device properties made with nearly identical preparation methods has puzzled the community. In the second part of this thesis we use non–linear pump probe microscopy to study the heterogeneous nature of femtosecond carrier dynamics in thin film perovskites. We show that the local morphology of the perovskite thin films has a profound influence on the underlying photophysics, opening new avenues for further optimization of device performance.

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  • 04/18/2018
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