Trimetallic nitride endohedral C80 fullerenes and their application in organic photovoltaic devices
Ross, Russel Brett.
Thesis (Ph.D.)--Georgetown University, 2009.; Includes bibliographical references.; Text (Electronic thesis) in PDF format. Trimetallic nitride endohedral C80 fullerenes (TNEF) materials offer a reduced lowest unoccupied molecular orbital energy (LUMO) offset when compared with many of the polymer donor systems currently being employed in Organic Photovoltaic (OPV) research. This lower LUMO offset allows for higher open circuit voltages, and therefore, higher efficiencies in OPV devices. Presented here is a comprehensive study of the room temperature absorption and emission of a series of trimetallic nitride endohedral metallofullerenes, M3N@C80, (M= Er, Gd, Ho, Lu, Sc, Y), as well the investigation and demonstration of TNEFs use as an acceptor material in OPV devices. Morphology and electrode contacts are shown to have large influence on TNEF-based OPV performance, in poly(3-hexyl)thiophene (P3HT) and 1-(3-hexoxycarbonyl)propyl-1-phenyl-[6,6]-Lu3N@C81 (Lu3N@C80-PCBH) based OPV devices. Decreasing the LUMO offset between P3HT and the acceptor material, reduced energy losses in the charge transfer process, which yield an increased open circuit voltage to 280mV above reference devices made with P3HT & [6,6]-phenyl-C61-butyric methyl ester (C60-PCBM). OPV energy conversion efficiencies of > 4% are observed with P3HT/Lu3N@C80-PCBH active layer with a predicted upper limit on power conversion efficiency of > 6% for this donor/acceptor system. The data displayed within this work constitutes proof of concept that the varying reduction potential (160 -290 meV vs. C60-PCBM) of the TNEF acceptor molecules provides a pathway to enhancing OPV device performance by closing down the molecular orbital offset of the donor/acceptor heterojunction. TNEF acceptor materials in single bulk heterojunction devices offer a viable path to 11% conversion efficiency with already-reported-on low-band-gap donors.
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