<p> The interaction of light with semiconductors provides essential insight into their electronic and photonic properties. Excitons, excited electron-hole pairs, determine the optical response of nanomaterials and act as nanoscale energy carriers, making excitonic materials excellent candidates for optoelectronic, photovoltaic, and quantum devices. Unique phenomena can be brought about by using excitonic materials as building blocks in designing new systems and taking advantage of excitons’ dimensionality. For example, growing quantum dots into highly ordered arrays enhances exciton transport due to the strong dipolar coupling between excitons. Alternatively, forming vertical heterostructures between monolayer transition metal dichalcogenides introduces moiré superlattices, which localize the excitons introducing nonlinear interactions that be exploited for quantum information processing. Understanding these complex excitonic systems requires experimental tools capable of high spatial and temporal resolutions.</p>
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<p>This thesis aims to contribute to understanding the complex excitons and charges formed at nanoscale interfaces with ultrafast techniques. In the discussed work, we take advantage of the 100s of fs time resolution and 10s of nm spatial precision to visualize exciton migration and dynamics associated with complex excitonic systems. First, we introduce the optical techniques needed to help us understand the fundamental photophysics of the studied systems (Chapter 2). Next, we provide an example of how we can use these methods to understand exciton coherence in perovskite quantum dot solids exhibiting superradiance (Chapter 3) and enhanced exciton transport (Chapter 4) due to low disorder and strong dipolar coupling. We also characterize and explore the behavior of highly excited excitons, Rydberg states, in transition metal dichalcogenides (Chapter 5). Then, we examine the properties of heterostructures formed between two monolayers of transition metal dichalcogenides exhibiting moiré superlattices and investigate the nonlinear exciton-exciton interactions modulated by the moiré potentials (Chapter 6). We also explore charge carrier behavior at interfaces of two different excitonic materials in molybdenum disulfide-single-wall carbon nanotube heterojunctions containing one- and two-dimensional excitons (Chapter 7). Finally, we visualize and quantify charge carrier migration across an alloyed cadmium sulfide and cadmium selenide lateral heterojunction (Chapter 8). We hope to give the reader a better understanding of these complex systems and open up new possibilities for their efficient use through the results presented in this thesis. </p>
| Identifer | oai:union.ndltd.org:purdue.edu/oai:figshare.com:article/21685055 |
| Date | 09 December 2022 |
| Creators | Daria D Blach (14212742) |
| Source Sets | Purdue University |
| Detected Language | English |
| Type | Text, Thesis |
| Rights | CC BY 4.0 |
| Relation | https://figshare.com/articles/thesis/Ultrafast_Imaging_of_Energy_and_Charge_Transfer_at_Nanoscale_Interfaces/21685055 |
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