Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 136, Issue 7, Pages 2876-2884Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja411859m
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Funding
- ANSER Center, an Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001059]
- Northwestern Materials Science and Engineering Center (NSF) [DMR-1121262]
- Corpus Christi College, Cambridge
- VENI grant from The Netherlands Organization for Scientific Research (NWO)
- EPSRC
- U.S.-Israel Binational Science Foundation [2011509]
- Engineering and Physical Sciences Research Council [EP/G060738/1] Funding Source: researchfish
- EPSRC [EP/G060738/1] Funding Source: UKRI
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Natural photosynthetic complexes accomplish the rapid conversion of photoexcitations into spatially separated electrons and holes through precise hierarchical ordering of chromophores and redox centers. In contrast, organic photovoltaic (OPV) cells are poorly ordered, utilize only two different chemical potentials, and the same materials that absorb light must also transport charge; yet, some OPV blends achieve near-perfect quantum efficiency. Here we perform electronic structure calculations on large clusters of functionalized fullerenes of different size and ordering, predicting several features of the charge generation process, outside the framework of conventional theories but clearly observed in ultrafast electro-optical experiments described herein. We show that it is the resonant coupling of photogenerated singlet excitons to a high-energy manifold of fullerene electronic states that enables efficient charge generation, bypassing localized charge-transfer states. In contrast to conventional views, our findings suggest that fullerene cluster size, concentration, and dimensionality control charge generation efficiency, independent of exciton delocalization.
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