Spiro-OMeTAD single crystals: Remarkably enhanced charge-carrier transport via mesoscale ordering

Handle URI:
http://hdl.handle.net/10754/619758
Title:
Spiro-OMeTAD single crystals: Remarkably enhanced charge-carrier transport via mesoscale ordering
Authors:
Shi, Dong ( 0000-0003-4009-2686 ) ; Qin, X.; Li, Yuan ( 0000-0002-4958-6132 ) ; He, Yao; Zhong, Cheng; Pan, Jun; Dong, H.; Xu, Wei; Li, T.; Hu, W.; Bredas, Jean-Luc ( 0000-0001-7278-4471 ) ; Bakr, Osman M. ( 0000-0002-3428-1002 )
Abstract:
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.
KAUST Department:
Solar and Photovoltaic Engineering Research Center (SPERC); Physical Sciences and Engineering (PSE) Division; Imaging and Characterization Core Lab
Citation:
Spiro-OMeTAD single crystals: Remarkably enhanced charge-carrier transport via mesoscale ordering 2016, 2 (4):e1501491 Science Advances
Publisher:
American Association for the Advancement of Science (AAAS)
Journal:
Science Advances
Issue Date:
15-Apr-2016
DOI:
10.1126/sciadv.1501491
Type:
Article
ISSN:
2375-2548
Sponsors:
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.
Is Supplemented By:
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:http://hdl.handle.net/10754/624579
Additional Links:
http://advances.sciencemag.org/cgi/doi/10.1126/sciadv.1501491
Appears in Collections:
Articles

Full metadata record

DC FieldValue Language
dc.contributor.authorShi, Dongen
dc.contributor.authorQin, X.en
dc.contributor.authorLi, Yuanen
dc.contributor.authorHe, Yaoen
dc.contributor.authorZhong, Chengen
dc.contributor.authorPan, Junen
dc.contributor.authorDong, H.en
dc.contributor.authorXu, Weien
dc.contributor.authorLi, T.en
dc.contributor.authorHu, W.en
dc.contributor.authorBredas, Jean-Lucen
dc.contributor.authorBakr, Osman M.en
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 Advancesen
dc.identifier.issn2375-2548-
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.en
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.en
dc.language.isoenen
dc.publisherAmerican Association for the Advancement of Science (AAAS)en
dc.relation.urlhttp://advances.sciencemag.org/cgi/doi/10.1126/sciadv.1501491en
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/en
dc.subjectMaterials scienceen
dc.subjectcrystal structureen
dc.subjectperovskiteen
dc.subjectsolar cellsen
dc.subjecthole-transport materialen
dc.subjectspiro-OMeTADen
dc.subjectphotovoltaicsen
dc.subjectsolid-state dye-sensitized solar cellen
dc.titleSpiro-OMeTAD single crystals: Remarkably enhanced charge-carrier transport via mesoscale orderingen
dc.typeArticleen
dc.contributor.departmentSolar and Photovoltaic Engineering Research Center (SPERC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentImaging and Characterization Core Laben
dc.identifier.journalScience Advancesen
dc.eprint.versionPublisher's Version/PDFen
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.en
dc.contributor.institutionSchool of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China.en
dc.contributor.institutionDepartment of Chemistry, National University of Singapore, 3 Science Drive, Singapore 117543, Singapore.en
dc.contributor.affiliationKing Abdullah University of Science and Technology (KAUST)en
kaust.authorShi, Dongen
kaust.authorLi, Yuanen
kaust.authorHe, Y.en
kaust.authorZhong, C.en
kaust.authorPan, J.en
kaust.authorXu, W.en
kaust.authorBredas, J.-L.en
kaust.authorBakr, Osman M.en
dc.relation.isSupplementedByShi, 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.cc1ljv32en
dc.relation.isSupplementedByDOI:10.5517/ccdc.csd.cc1ljv32en
dc.relation.isSupplementedByHANDLE:http://hdl.handle.net/10754/624579en
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