Proceedings of nanoGe Spring Meeting 2022 (NSM22)
DOI: https://doi.org/10.29363/nanoge.nsm.2022.168
Publication date: 7th February 2022
The unique properties of lead halide perovskite nanocrystals (NCs) have drawn major attention of researchers over the last decade. However, the high toxicity of the lead in the composition and the relatively low phase stability are delaying their commercialization, therefore, diminishing their advantages [1]. These challenges are one of the major focuses of the community leading to the ongoing search for new stable lead-free compositions. However, up to date, there are only a few promising candidates to surpass the characteristics of lead halide perovskite NCs [2].
So far, no attention to cesium manganese chloride (CsMnCl3) NCs was given likely due to the absence of promising properties [3]. We are the first ones to synthesize and characterize emissive colloidal CsMnCl3 NCs through the conventional hot-injection route. The optical, structural, and morphological properties of CsMnCl3 NCs were studied by the means of steady-state-, time-resolved, and low-temperature spectroscopy, transmission electron microscopy (TEM), inductively coupled plasma mass spectrometry (ICP-MS), and X-ray diffractometry (XRD) respectively. The synthesized CsMnCl3 NCs display photoluminescence at 670 nm, large Stokes shift (250 nm), broad emission (FWHM = 97 nm), lifetime decay in the millisecond range, and fairly high quantum yield of 25%.
Moreover, Rietveld structural refinement was carried out to confirm the adopted structure of the NCs and investigate the relationship between synthesis conditions, crystal structure, and photoluminescence. It was found that when the synthesis temperature was tuned, the CsMnCl3 adopt different crystal structures (i.e. cubic and rhombohedral). By optimizing the temperature and the precursors' ratio, a pure rhombohedral structure is formed. It is worth nothing, that up to date, there is no work showing the luminescent rhombohedral CsMnCl3 as well as the dependence between the synthesis conditions, structure, and optical properties.
In addition, the synthesized NCs show moderate phase and optical stability (more than 2 weeks) under the ambient conditions (dark, RH 40-60%, RT). Together with its unique optical properties, CsMnCl3 is a promising candidate to substitute lead-halide perovskite NCs. The results of our work provide important insights into the photochemistry of manganese-based materials.
Dr. Mari Honkanen and Tampere Microscopy Center are gratefully acknowledged for the TEM images. This work is part of the Academy of Finland Flagship Programme, Photonics Research and Innovation (PREIN), Decision No 320165. A.M. and P.V. thank the financial support of Tampere University, Faculty of Engineering and Natural Sciences. M.L. thanks Finnish Cultural Foundation (00210670) for funding. J-H.S. thanks Academy of Finland (project 308307). P.V. and J-H.S. also acknowledge the support of Jane & Aatos Erkko foundation (project ‘ASPIRE’).
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