Abstract
Ionic aggregates are among the most common forms of matter, yet the investigation of their molecular motion is often constrained by the instability of isolated anions and cations, as well as the lack of real-time monitoring techniques. This study presents a zwitterionic strategy that integrates both cations and anions into one fluorescent organic framework, forming a zwitterionic molecule. The zwitterionic strategy simplifies the intricate cation-anion systems that are typically found in conventional inorganic salts and imparts them with fluorescent properties, facilitating real-time tracking of ionic-interaction-induced molecular motion within ionic aggregates. Specifically, a blue shift in the fluorescence wavelength signified changes in aggregate states due to intermolecular motion, whereas a decrease in intensity was linked to intramolecular-motion-caused conformational changes. This spontaneous molecular motion enabled dynamic switching of the excited state energy-decay pathway, leading to switchable color-light responses. Overall, the zwitterionic strategy offers a novel framework for exploring the properties and behaviors of molecules in ionic aggregates.