TY - JOUR
T1 - Spiro-OMeTAD single crystals: Remarkably enhanced charge-carrier transport via mesoscale ordering
AU - Shi, Dong
AU - Qin, X.
AU - Li, Yuan
AU - He, Yao
AU - Zhong, Cheng
AU - Pan, Jun
AU - Dong, H.
AU - Xu, Wei
AU - Li, T.
AU - Hu, W.
AU - Bredas, Jean-Luc
AU - Bakr, Osman
N1 - KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: 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.
PY - 2016/4/15
Y1 - 2016/4/15
N2 - 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.
AB - 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.
UR - http://hdl.handle.net/10754/619758
UR - http://advances.sciencemag.org/cgi/doi/10.1126/sciadv.1501491
UR - http://www.scopus.com/inward/record.url?scp=84983484047&partnerID=8YFLogxK
U2 - 10.1126/sciadv.1501491
DO - 10.1126/sciadv.1501491
M3 - Article
C2 - 27152342
VL - 2
SP - e1501491
JO - Science Advances
JF - Science Advances
SN - 2375-2548
IS - 4
ER -