Lapointe Victoria, Green Philippe B, Chen Alexander N, Buonsanti Raffaella, Majewski Marek B
Department of Chemistry and Biochemistry, Centre for NanoScience Research, Concordia University 7141 Sherbrooke Street West Montreal Quebec H4B 1R6 Canada
Laboratory of Nanochemistry for Energy, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne Sion CH-1950 Switzerland.
Chem Sci. 2024 Feb 19;15(12):4510-4518. doi: 10.1039/d3sc06662b. eCollection 2024 Mar 20.
Superlattice formation afforded by metal halide perovskite nanocrystals has been a phenomenon of interest due to the high structural order induced in these self-assemblies, an order that is influenced by the surface chemistry and particle morphology of the starting building block material. In this work, we report on the formation of superlattices from aluminum oxide shelled CsPbBr perovskite nanocrystals where the oxide shell is grown by colloidal atomic layer deposition. We demonstrate that the structural stability of these superlattices is preserved over 25 days in an inert atmosphere and that colloidal atomic layer deposition on colloidal perovskite nanocrystals yields structural protection and an enhancement in photoluminescence quantum yields and radiative lifetimes as opposed to gas phase atomic layer deposition on pre-assembled superlattices or excess capping group addition. Structural analyses found that shelling resulted in smaller nanocrystals that form uniform supercrystals. These effects are in addition to the increasingly static capping group chemistry initiated where oleic acid is installed as a capping ligand directly on aluminum oxide. Together, these factors lead to fundamental observations that may influence future superlattice assembly design.
金属卤化物钙钛矿纳米晶体形成的超晶格一直是一个备受关注的现象,这是因为这些自组装结构中诱导出了高度的结构有序性,这种有序性受到起始构建块材料的表面化学和颗粒形态的影响。在这项工作中,我们报道了由氧化铝包覆的CsPbBr钙钛矿纳米晶体形成超晶格的情况,其中氧化物壳层是通过胶体原子层沉积生长的。我们证明,这些超晶格在惰性气氛中25天内保持结构稳定性,并且与在预组装超晶格上进行气相原子层沉积或添加过量封端基团相反,在胶体钙钛矿纳米晶体上进行胶体原子层沉积可产生结构保护,并提高光致发光量子产率和辐射寿命。结构分析发现,包覆导致形成均匀超晶体的纳米晶体尺寸变小。这些效应还包括直接在氧化铝上安装油酸作为封端配体引发的越来越静态的封端基团化学。这些因素共同导致了一些基本观察结果,可能会影响未来超晶格组装设计。