low-Dimensional Organic Lead Halides with Organic-Inorganic Collaborative Luminescence Regulated by Anion in Dimension

摘要

Low-dimensional (LD) organic-metal halides (OMHs) have been extensively investigated because of their excellent optical properties. However, the rational synthetic control (dimension regulation) of LD-OMHs has not yet been established well. The effect of organic cations on the luminescence also remains unexplored. Here, we designed a double-chain ammonium salt 1 with two amine functional groups. Using hydrogen bonding between -N-H3 protons and halogen ions synthesized zero-dimensional (0D) OMH C_(12)H_(30)N4Pb2Br_g (2). Furthermore, through introducing other ionic interactions to regulate the dimension of OMHs, we obtained one-dimensional (1D) OMH C_(12)H_(30)N4Pb2Cl_(7.5)Br_(0.5) (3) by anion exchange of 2. Through the in-depth analysis of their crystal structure, it is understood that the design of organic cations and the exchange of anions can regulate the dimension of OMHs through the change of hydrogen bonds in the structure. This sets a foundation for the formation of a synthesis mechanism for LD-OMHs and effective regulation of OMHs dimension. Through crystal structure analysis, experiments, and theoretical calculations, this work proves that the emission of 2 is not dominated by a single factor of organic cations or metal halogen octahedrons but by the interaction of organic cations and metal octahedrons. Moreover, the 1D-OMH 3 shows tunable emissions from blue to white light under varying excitation wavelengths, which provides a foundation for expanding the application of OMHs.