Pandey, Richa2013-08-292013-08-292012-07https://hdl.handle.net/11299/156012University of Minnesota Ph.D. dissertation. July 2012. Major: Chemical Engineering. Advisor: Russell J. Holmes. 1 computer file (PDF); ix, 177 pages, appendices A-E.Organic photovoltaic cells (OPVs) have received significant industrial and academic interest in the last decade as a promising source of inexpensive renewable energy. However, further improvements in device performance and improved lifetimes are required for the commercialization of OPVs. This work is primarily focused on developing a novel device architecture to improve device performance and characterizing structure-property-performance relationships for OPVs. The excitonic nature of organic semiconductors necessitates the use of an electron donor-acceptor (D-A) heterojunction for efficient exciton dissociation and the generation of photocurrent. In many organic semiconductors, the optical absorption length is much larger than the exciton diffusion length. This trade-off between absorption and exciton diffusion is often overcome by increasing the area of the dissociating D-A interface using engineered film morphologies. This thesis presents an approach to maximize cell efficiency using a continuously graded D-A heterojunction. The graded heterojunction allows for an increase in the D-A interface area for an enhanced exciton diffusion efficiency, while also preserving the charge collection efficiency, leading to a significant improvement in device performance relative to that of optimized planar and uniformly mixed OPVs. In addition, this work correlates the optimized D-A composition gradient to the underlying film morphology and charge transport properties of uniform D-A mixtures. Subsequently, a new characterization technique to calculate the charge collection efficiency of OPVs is discussed. This technique is used to demonstrate the enhanced charge collection efficiency in graded heterojunctions relative to uniformly mixed heterojunctions. Afterwards, the properties of a new material and its potential as an electron donor material in OPVs are examined. Finally, an overview of the results and the ideas for future work are presented.en-USGraded heterojunctionOrganic semiconductorsPhotovoltaic cellsThesis or Dissertation