The aggregation process plays a significant role in regulating the aggregate structures from molecules toward macroscopic photophysical properties.Pyrene(Py),as the simplest dimer candidate,serves as a suitable model ...The aggregation process plays a significant role in regulating the aggregate structures from molecules toward macroscopic photophysical properties.Pyrene(Py),as the simplest dimer candidate,serves as a suitable model for studying the aggregation.Herein,a series of Py-based aggregation-induced emission(AIE)materials have been investigated by clarifying the comprehensive roles of oxygen,substituents,molecular motion,and packing during aggregation,initially realizing the aim of controlling aggregate structures.With a largely planar and conjugated conformation,Py shows anomalous AIE characteristics due to the oxygen quenching at the molecular level but turn-on fluorescence in the aggregate state because of the oxygen isolation.Although introducing substituents induces molecular motion and similarly weakened luminescence in the molecular state,the impact of substituents on the aggregate-state photophysical properties enormously differs,exhibiting from weak blue,strong cyan,and strong green to weak yellow emissions,due to variable aggregate structures.Interestingly,the natural alicycle-substituted Py-dehydroabietylamine(Py-DAA)exhibits both mechanochromism and acidichromism,which can be synergistically applied in dynamic encryption-decryption.This work not only elucidates the unique AIE property of Py for the first time but also clarifies the bridging role of aggregation between single-molecular and aggregate states,achieving preliminary control over the aggregate structures.展开更多
基金supported by the National Natural Science Foundation of China(21601087)the Natural Science Foundation of Jiangsu Province(BK20231296)+3 种基金the Open Fund of Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates,Guangzhou 510640,China(South China University of Technology[2023B1212060003])the Shenzhen Key Laboratory of Functional Aggregate Materials(ZDSYS20211021111400001)the Science Technology Innovation Commission of Shenzhen Municipality(KQTD20210811090142053)the Key Research and Development Project of Yunnan Province(202303AC100010).
文摘The aggregation process plays a significant role in regulating the aggregate structures from molecules toward macroscopic photophysical properties.Pyrene(Py),as the simplest dimer candidate,serves as a suitable model for studying the aggregation.Herein,a series of Py-based aggregation-induced emission(AIE)materials have been investigated by clarifying the comprehensive roles of oxygen,substituents,molecular motion,and packing during aggregation,initially realizing the aim of controlling aggregate structures.With a largely planar and conjugated conformation,Py shows anomalous AIE characteristics due to the oxygen quenching at the molecular level but turn-on fluorescence in the aggregate state because of the oxygen isolation.Although introducing substituents induces molecular motion and similarly weakened luminescence in the molecular state,the impact of substituents on the aggregate-state photophysical properties enormously differs,exhibiting from weak blue,strong cyan,and strong green to weak yellow emissions,due to variable aggregate structures.Interestingly,the natural alicycle-substituted Py-dehydroabietylamine(Py-DAA)exhibits both mechanochromism and acidichromism,which can be synergistically applied in dynamic encryption-decryption.This work not only elucidates the unique AIE property of Py for the first time but also clarifies the bridging role of aggregation between single-molecular and aggregate states,achieving preliminary control over the aggregate structures.