Dissertation
Theoretical considerations and computational strategies for molecular electronic device design
Doctor of Philosophy (Ph.D.), Drexel University
Sep 2019
DOI:
https://doi.org/10.17918/00000217
Abstract
The key feature of electronic devices is the interface through which electrons or holes flow. The behavior of such a device is therefore dependent upon how energetically favorable this charge injection process is. The energetics of the system can be computed using quantum chemical methods and the charge injection barrier can be inferred from these results. The efficiency of one type of electronic device, the dye-sensitized solar cell (DSSC), is strongly influenced by dye molecule orientation and interactions with the substrate. Understanding the factors controlling the surface orientation of sensitizing organic molecules and being able to study them using electronic structure calculations will aid in the improvement of both traditional DSSCs and other devices that integrate molecular linkers at interfaces. Chapter 3 first presents a general approach to understand relative dye-substrate orientation and analytical expressions predicting orientation are provided. The effects of substrate, solvent, and protonation state on dye molecule orientation are considered. A two-part analytical model is developed that predicts the binding energy of a molecule and quantifies the dye solvation energy for two solvents. This affords the rapid prediction of dye molecule and MOF linker binding preference on the basis of the size of the adsorbing molecule, identity of the surface, and the solvent environment. Once binding orientation is predicted, the charge injection barrier between the materials that constitute the interface can be computed. This computation and its challenges are discussed in Chapter 4. Finally, with the rapid advancement of the field of interface materials, it is surprising that materials science topics are currently underrepresented in the chemistry curriculum. Chapter 5 describes student activities that were developed in order to introduce concepts surrounding the electronic structure of materials to upper-level-undergraduate and introductory-graduate-level chemistry students.
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Details
- Title
- Theoretical considerations and computational strategies for molecular electronic device design
- Creators
- Janna Domenico
- Contributors
- Karl Sohlberg (Advisor)
- Awarding Institution
- Drexel University
- Degree Awarded
- Doctor of Philosophy (Ph.D.)
- Publisher
- Drexel University; Philadelphia, Pennsylvania
- Number of pages
- xvii, 180 pages
- Resource Type
- Dissertation
- Language
- English
- Academic Unit
- College of Arts and Sciences; Chemistry; Drexel University
- Other Identifier
- 991014695544804721