Journal
SCIENCE ADVANCES
Volume 2, Issue 4, Pages -Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.1501491
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Funding
- King Abdullah University of Science and Technology [URF/1/2268-01-01]
- ONR Global [N62909-15-1-2003]
- National Natural Science Foundation of China [91433115]
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We report the crystal structure and hole-transport mechanism in spiro-OMeTAD [2,2',7,7'-tetrakis(N,N-di-p-methoxyphenyl-amine) 9,9'-spirobifluorene], the dominant hole-transporting material in perovskite and solid-state dye-sensitized solar cells. Despite spiro-OMeTAD's paramount role in such devices, its crystal structure was unknown because of highly disordered solution-processed films; the hole-transport pathways remained ill-defined and the charge carrier mobilities were low, posing a major bottleneck for advancing cell efficiencies. We devised an antisolvent crystallization strategy to grow single crystals of spiro-OMeTAD, which allowed us to experimentally elucidate its molecular packing and transport properties. Electronic structure calculations enabled us to map spiro-OMeTAD's intermolecular charge-hopping pathways. Promisingly, single-crystal mobilities were found to exceed their thin-film counterparts by three orders of magnitude. Our findings underscore mesoscale ordering as a key strategy to achieving breakthroughs in hole-transport material engineering of solar cells.
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