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dc.contributor.authorLiu, Qi
dc.contributor.authorYin, Jun
dc.contributor.authorZhang, Bin-Bin
dc.contributor.authorChen, Jia-Kai
dc.contributor.authorZhou, Yang
dc.contributor.authorZhang, Lu-Min
dc.contributor.authorWang, Lu-Ming
dc.contributor.authorZhao, Qing
dc.contributor.authorHou, Jingshan
dc.contributor.authorShu, Jie
dc.contributor.authorSong, Bo
dc.contributor.authorShirahata, Naoto
dc.contributor.authorBakr, Osman
dc.contributor.authorMohammed, Omar F.
dc.contributor.authorSun, Hong-Tao
dc.date.accessioned2021-04-04T08:16:23Z
dc.date.available2021-04-04T08:16:23Z
dc.date.issued2021-04-01
dc.date.submitted2021-01-27
dc.identifier.citationLiu, Q., Yin, J., Zhang, B.-B., Chen, J.-K., Zhou, Y., Zhang, L.-M., … Sun, H.-T. (2021). Theory-Guided Synthesis of Highly Luminescent Colloidal Cesium Tin Halide Perovskite Nanocrystals. Journal of the American Chemical Society. doi:10.1021/jacs.1c01049
dc.identifier.issn0002-7863
dc.identifier.issn1520-5126
dc.identifier.pmid33794093
dc.identifier.doi10.1021/jacs.1c01049
dc.identifier.urihttp://hdl.handle.net/10754/668499
dc.description.abstractThe synthesis of highly luminescent colloidal CsSnX<sub>3</sub> (X = halogen) perovskite nanocrystals (NCs) remains a long-standing challenge due to the lack of a fundamental understanding of how to rationally suppress the formation of structural defects that significantly influence the radiative carrier recombination processes. Here, we develop a theory-guided, general synthetic concept for highly luminescent CsSnX<sub>3</sub> NCs. Guided by density functional theory calculations and molecular dynamics simulations, we predict that, although there is an opposing trend in the chemical potential-dependent formation energies of various defects, highly luminescent CsSnI<sub>3</sub> NCs with narrow emission could be obtained through decreasing the density of tin vacancies. We then develop a colloidal synthesis strategy that allows for rational fine-tuning of the reactant ratio in a wide range but still leads to the formation of CsSnI<sub>3</sub> NCs. By judiciously adopting a tin-rich reaction condition, we obtain narrow-band-emissive CsSnI<sub>3</sub> NCs with a record emission quantum yield of 18.4%, which is over 50 times larger than those previously reported. Systematic surface-state characterizations reveal that these NCs possess a Cs/I-lean surface and are capped with a low density of organic ligands, making them an excellent candidate for optoelectronic devices without any postsynthesis ligand management. We showcase the generalizability of our concept by further demonstrating the synthesis of highly luminescent CsSnI<sub>2.5</sub>Br<sub>0.5</sub> and CsSnI<sub>2.25</sub>Br<sub>0.75</sub> NCs. Our findings not only highlight the value of computation in guiding the synthesis of high-quality colloidal perovskite NCs but also could stimulate intense efforts on tin-based perovskite NCs and accelerate their potential applications in a range of high-performance optoelectronic devices.
dc.description.sponsorshipThis work was partly supported by a curiosity-driven research project in NIMS, three projects from JST (JST A-step, JPMJTS1619), JSPS (19K22176), and the National Natural Science Foundation of China (11874275). Computational work was supported by the Supercomputing Laboratory at King Abdullah University of Science and Technology (KAUST).
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttps://pubs.acs.org/doi/10.1021/jacs.1c01049
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.1c01049.
dc.titleTheory-Guided Synthesis of Highly Luminescent Colloidal Cesium Tin Halide Perovskite Nanocrystals
dc.typeArticle
dc.contributor.departmentChemical Science Program
dc.contributor.departmentFunctional Nanomaterials Lab (FuNL)
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentKAUST Solar Center (KSC)
dc.contributor.departmentMaterial Science and Engineering Program
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.contributor.departmentUltrafast Laser Spectroscopy and Four-dimensional Electron Imaging Research Group
dc.identifier.journalJournal of the American Chemical Society
dc.rights.embargodate2022-04-01
dc.eprint.versionPost-print
dc.contributor.institutionCollege of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China
dc.contributor.institutionInternational Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), 1-2-1 Sengen, Tsukuba 305-0047, Japan
dc.contributor.institutionGraduate School of Chemical Sciences and Engineering, Hokkaido University, Sapporo 060-0814, Japan
dc.contributor.institutionSchool of Materials Science and Engineering, Shanghai Institute of Technology, Shanghai 201418, China
dc.contributor.institutionAnalysis and Testing Center, Soochow University, Jiangsu 215123, China
dc.contributor.institutionDepartment of Physics, Chuo University, Tokyo 112-8551, Japan
kaust.personYin, Jun
kaust.personZhou, Yang
kaust.personBakr, Osman M.
kaust.personMohammed, Omar F.
kaust.acknowledged.supportUnitSupercomputing Laboratory


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