Show simple item record

dc.contributor.authorShi, Dong
dc.contributor.authorQin, X.
dc.contributor.authorLi, Yuan
dc.contributor.authorHe, Yao
dc.contributor.authorZhong, Cheng
dc.contributor.authorPan, Jun
dc.contributor.authorDong, H.
dc.contributor.authorXu, Wei
dc.contributor.authorLi, T.
dc.contributor.authorHu, W.
dc.contributor.authorBredas, Jean-Luc
dc.contributor.authorBakr, Osman
dc.date.accessioned2016-09-04T07:24:49Z
dc.date.available2016-09-04T07:24:49Z
dc.date.issued2016-04-15
dc.identifier.citationSpiro-OMeTAD single crystals: Remarkably enhanced charge-carrier transport via mesoscale ordering 2016, 2 (4):e1501491 Science Advances
dc.identifier.issn2375-2548
dc.identifier.pmid27152342
dc.identifier.doi10.1126/sciadv.1501491
dc.identifier.urihttp://hdl.handle.net/10754/619758
dc.description.abstractWe 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.
dc.description.sponsorshipO.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.
dc.language.isoen
dc.publisherAmerican Association for the Advancement of Science (AAAS)
dc.relation.urlhttp://advances.sciencemag.org/cgi/doi/10.1126/sciadv.1501491
dc.rightsThis is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited. http://creativecommons.org/licenses/by-nc/4.0/
dc.subjectMaterials science
dc.subjectcrystal structure
dc.subjectperovskite
dc.subjectsolar cells
dc.subjecthole-transport material
dc.subjectspiro-OMeTAD
dc.subjectphotovoltaics
dc.subjectsolid-state dye-sensitized solar cell
dc.titleSpiro-OMeTAD single crystals: Remarkably enhanced charge-carrier transport via mesoscale ordering
dc.typeArticle
dc.contributor.departmentFunctional Nanomaterials Lab (FuNL)
dc.contributor.departmentImaging and Characterization Core Lab
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentKAUST Solar Center (KSC)
dc.contributor.departmentLaboratory for Computational and Theoretical Chemistry of Advanced Materials
dc.contributor.departmentMaterial Science and Engineering Program
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalScience Advances
dc.eprint.versionPublisher's Version/PDF
dc.contributor.institutionKey Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Zhongguancun North First Street No. 2, Beijing 100190, P. R. China.
dc.contributor.institutionSchool of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China.
dc.contributor.institutionDepartment of Chemistry, National University of Singapore, 3 Science Drive, Singapore 117543, Singapore.
dc.contributor.affiliationKing Abdullah University of Science and Technology (KAUST)
kaust.personShi, Dong
kaust.personLi, Yuan
kaust.personHe, Y.
kaust.personZhong, Cheng
kaust.personPan, J.
kaust.personXu, W.
kaust.personBredas, Jean-Luc
kaust.personBakr, Osman M.
dc.relation.issupplementedbyDOI:10.5517/ccdc.csd.cc1ljv32
refterms.dateFOA2018-06-14T02:24:45Z
display.relations<b> Is Supplemented By:</b> <br/> <ul><li><i>[Dataset]</i> <br/> 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: <a href="https://doi.org/10.5517/ccdc.csd.cc1ljv32">10.5517/ccdc.csd.cc1ljv32</a> HANDLE: <a href="http://hdl.handle.net/10754/624579">10754/624579</a></li></ul>
dc.date.published-online2016-04-15
dc.date.published-print2016-04-15


Files in this item

Thumbnail
Name:
e1501491.full.pdf
Size:
1.593Mb
Format:
PDF
Description:
Main article

This item appears in the following Collection(s)

Show simple item record