Synthesis and characterization of multi-stimuli-responsive luminescent two-coordinate copper(I) complexes featuring 1,3-imidazolium-derived mesoionic carbenes
摘要
Stimulus-responsive luminescent materials have attracted considerable attention because of their potential applications in information decryption and anti-counterfeiting. Carbene-metal-amide (CMA) complexes are promising for the development of stimulus-responsive luminescent materials due to their easily tunable excited states and flexible structures. In this study, we designed and synthesized a series of luminescent CMA complexes (1–8) containing 1,3-imidazolium-derived mesoionic carbenes (iMICs) with tunable π-accepting properties. Interestingly, complexes 1–6 emitted solution-phase phosphorescence when their concentration was increased or the excitation wavelength was decreased, whereas complexes 7 and 8 did not emit phosphorescence under similar conditions. Furthermore, complexes 1–4 displayed aggregation-induced phosphorescence in solution and room-temperature phosphorescence in the solid state. These observed changes in the optical properties correlated with the gradual increase in the energy gap between the lowest singlet and triplet excited states determined by theoretical calculations. Moreover, we demonstrated the high-level information encryption and anti-counterfeiting via on-demand multicolor displays. These findings demonstrate that 1,3-imidazolium-derived iMICs, which are readily amenable to structural modification, can substantially influence the molecular configuration and excited-state dynamics of CMA complexes, thus offering a viable strategy for precise modulation of their photophysical properties.