Theory-Guided Synthesis of Highly Luminescent Colloidal Cesium Tin Halide Perovskite Nanocrystals
Mohammed, Omar F.
KAUST DepartmentChemical Science Program
Functional Nanomaterials Lab (FuNL)
KAUST Catalysis Center (KCC)
KAUST Solar Center (KSC)
Material Science and Engineering Program
Physical Science and Engineering (PSE) Division
Ultrafast Laser Spectroscopy and Four-dimensional Electron Imaging Research Group
Embargo End Date2022-04-01
Permanent link to this recordhttp://hdl.handle.net/10754/668499
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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.
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
SponsorsThis 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).
PublisherAmerican Chemical Society (ACS)
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