Colloidal Synthesis and Optical Properties of Perovskite-Inspired Cesium Zirconium Halide Nanocrystals
MacManus-Driscoll, Judith L
ACS Materials Letters
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Abfalterer, A., Shamsi, J., Kubicki, D., Savory, C. N., Xiao, J., Divitini, G., Li, W., et al. (2020). Colloidal Synthesis and Optical Properties of Perovskite-Inspired Cesium Zirconium Halide Nanocrystals. ACS Materials Letters, 1644-1652. https://doi.org/10.1021/acsmaterialslett.0c00393
Optoelectronic devices based on lead halide perovskites are processed in facile ways yet are remarkably efficient. There are extensive research efforts investigating lead-free perovskite and perovskite-related compounds, yet there are challenges to synthesize these materials in forms that can be directly integrated into thin film devices rather than as bulk powders. Here, we report on the colloidal synthesis and characterization of lead-free, antifluorite Cs2ZrX6 (X = Cl, Br) nanocrystals that are readily processed into thin films. We use transmission electron microscopy and powder X-ray diffraction measurements to determine their size and structural properties, and solid-state nuclear magnetic resonance measurements reveal the presence of oleate ligand together with a disordered distribution of Cs surface sites. Density functional theory calculations reveal the band structure and fundamental band gaps of 5.06 eV and 3.91 eV for Cs2ZrCl6 and Cs2ZrBr6, respectively, consistent with experimental values. Finally, we demonstrate that the Cs2ZrCl6 and Cs2ZrBr6 nanocrystal thin films exhibit tunable, broad white photoluminescence with quantum yields of 45% for the latter, with respective peaks in the blue and green spectral regions and mixed systems exhibiting properties in between. Our work represents a critical step towards application of lead-free Cs2ZrX6 nanocrystal thin films into next-generation light emitting applications.
S.D.S. acknowledges the Royal Society and Tata Group (UF150033). A.A. acknowledges the Royal Society for funding. We are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/P020194/1) and to UCL for the provision of the Legion (Legion@UCL), Myriad (Myriad@UCL) and Grace (Grace@UCL) computing clusters. Computational work was also performed on the ARCHER UK National Supercomputing Service, via our membership of the UK’s HEC Materials Chemistry Consortium, funded by EPSRC (EP/L000202 and EP/R029431). J.X. thanks the EPSRC Cambridge NanoDTC, EP/L015978/1. W.-W.L. and J.L.M.-D. acknowledge support from EPSRC Grant EP/L011700/1, EP/N004272/1, and the Isaac Newton Trust (Minute 13.38(k)). J.L.M.-D. acknowledges support from the Royal Academy of Engineering, Grant CiET1819_24. This work was supported through the Cambridge Royce facilities grant EP/P024947/1 and Sir Henry Royce Institute - recurrent grant EP/R00661X/1. S.M. acknowledges an EPSRC studentship. K.G. appreciates support from the Polish Ministry of Science and Higher Education within the Mobilnosc Plus program (Grant no. 1603/MOB/V/2017/0). The DNP MAS NMR experiments were performed at the Nottingham DNP MAS NMR Facility which is funded by the University of Nottingham and EPSRC (EP/L022524/1) and EP/R042853/1. We thank Adam Brown for support with XPS measurements. J.S. and S.D.S. acknowledge the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (HYPERION, Grant Agreement Number 756962). This work has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement No. 841136.
Royal Society (UF150033)
European Commission Horizon 2020 (H2020) ERC (756962)
European Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (841136)
European Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (841386)
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External DOI: https://doi.org/10.1021/acsmaterialslett.0c00393
This record's URL: https://www.repository.cam.ac.uk/handle/1810/312191
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