Publication date: 15th May 2025
Atomic engineering of colloidal semiconductor nanomaterials requires the development of a synthetic reaction with well-defined precursors, pathways, and products. However, achieving atomic-level control remains challenging due to the complexity in the synthesis and structures of nanomaterials. Here, we will discuss the cation exchange induced transformation to synthesize II-VI and IV-VI semiconductor nanoclusters with atomic precision. We first demonstrated the reaction of a Cu26Se13(PEt2Ph)14 template cluster with a CdI2(PPr3)2 complex, producing a Cd26Se17I18(PPr3)10 cluster with an enlarged anion framework (Se13 ® Se17) and exchanged surface ligands (PEt2Ph ® I– + PPr3). The prototype reaction was then generalized to precisely program the synthesis of homolog M14Se13 (M = Zn, Cd, Hg) clusters protected by chelating diamine ligands, enabling a precise understanding of their geometric and electronic structures. In all exchange with IIB cations, the icosahedral Se13 anion framework is preserved, which can be attributed to the compatibility between tetrahedral bonding and icosahedral packing. In contrast, when exchanged with Pb2+, a single-sized PbSe cluster with a sharp absorption peak at 546 nm was obtained, but the anion lattice is rearranged to cubic-close packing to accommodate the octahedral coordination of Pb2+ cations. This precise and programmable synthesis via cation exchange is expected to enrich the library of atomically precise semiconductor nanostructures and elucidate their precise structure-property relationships.
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