Spiro-OMeTAD single crystals: Remarkably enhanced charge-carrier transport via mesoscale ordering
Type
ArticleAuthors
Shi, Dong
Qin, X.
Li, Yuan
He, Yao
Zhong, Cheng
Pan, Jun
Dong, H.
Xu, Wei
Li, T.
Hu, W.
Bredas, Jean-Luc

Bakr, Osman

KAUST Department
Functional Nanomaterials Lab (FuNL)Imaging and Characterization Core Lab
KAUST Catalysis Center (KCC)
KAUST Solar Center (KSC)
Laboratory for Computational and Theoretical Chemistry of Advanced Materials
Material Science and Engineering Program
Physical Science and Engineering (PSE) Division
Date
2016-04-15Online Publication Date
2016-04-15Print Publication Date
2016-04-15Permanent link to this record
http://hdl.handle.net/10754/619758
Metadata
Show full item recordAbstract
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.Citation
Spiro-OMeTAD single crystals: Remarkably enhanced charge-carrier transport via mesoscale ordering 2016, 2 (4):e1501491 Science AdvancesSponsors
O.M.B. and J.-L.B acknowledges the financial support of King Abdullah University of Science and Technology Grant URF/1/2268-01-01. J.-L.B. also acknowledges support from ONR Global through Grant N62909-15-1-2003. H.D. thanks the National Natural Science Foundation of China (91433115). Author contributions: D.S. conceived the idea. O.M.B. crafted the overall experimental plan and directed the research. D.S. optimized the crystallization. D.S. and W.X. performed the confocal optical microscope imaging. D.S. and Y.H. performed single-crystal XRD and data analysis. D.S., X.Q., H.D., T.L., and W.H. planned and performed the mobility measurements and analyzed the data. Y.L., C.Z., and J.-L.B. planned and performed the theoretical calculations. Y.L., C.Z., and J.-L.B. analyzed the data of the theoretical part. J.P. assisted D.S. in the experiments. D.S., Y.L., J.-L.B., and O.M.B. wrote the manuscript. All authors discussed and commented on the manuscript. Competing interests: The authors declare that they have no competing interests. Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials. Additional data related to this paper may be requested from the authors.Journal
Science AdvancesPubMed ID
27152342Additional Links
http://advances.sciencemag.org/cgi/doi/10.1126/sciadv.1501491Relations
Is Supplemented By:- [Dataset]
Shi, D., Qin, X., Li, Y., He, Y., Zhong, C., Pan, J., … Bakr, O. M. (2016). CCDC 1475944: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1ljv32. DOI: 10.5517/ccdc.csd.cc1ljv32 HANDLE: 10754/624579
ae974a485f413a2113503eed53cd6c53
10.1126/sciadv.1501491
Scopus Count
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