Publication date: 8th June 2021
Cesium lead halide (CsPbX3) perovskite semiconductor nanocrystals (NCs) increasingly mesmerize researchers because they exhibit outstanding optoelectronic properties. One of the remaining hurdles is atomistic structure determination due to their soft structure and their small size.[1] We address this challenge by using solution NMR spectroscopy. This easy-to-use technique can not only give insights into the elemental composition, but also into structural properties. Thanks to the incoherent tumbling of the NCs in in their colloidal state, the spectra of the crystalline cores resemble traditional solution NMR spectra. The identification of surface and core sites could be done by probing different size selected NCs. For mixed halide CsPb(Br/Cl)3 NCs an anion segregation within the cores was observed, favoring the bigger bromide to be located on the more disordered and enlarged surface sites. The influence of the various available capping ligands on the structure in the NCs was studied, revealing an increased amount of disorder for zwitterionic, covalent-bonded ligands compared to their ionic-bonded counterparts which could be correlated with their optical properties. To corroborate our experimental data, we performed ab inito molecular dynamics simulations, which point to the role of the surface in causing the strain distribution and disorder within numerous sizes of NCs. These findings showcase the great potential of solution NMR in shedding light on the inorganic structure of colloidal NCs.
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