Host‐Guest Systems Enable Efficient Organic Afterglow via a Facile Spraying Method

Abstract Unlocking the afterglow properties of the fluorescence molecules at room temperature is an urgent challenge. Herein, inks prepared with dimethyl terephthalate (DTT) and carbazole (Cz) analogs with heteroatom (C, S, and O) substituents on the N as host and guest molecules can be directly sprayed onto different substrates to unlock the excitation‐wavelength dependent (Ex‐De) afterglow characteristics of the guest compound. Additionally, with the increase in the number of lone pair electrons, spin‐orbit coupling (SOC) increases, resulting in a longer afterglow duration lasting up to 4.5 s with Φ_p>27%. Theory calculations and experiments indicate that the afterglow originated from the interactions between the host and guest molecules restricting the non‐radiative transition of the triplet excitons. Different Ex (with watershed at 310 nm) lead to the variation in the conformation of the S₀^DTT and S₁^DTT, which in turn affects the strength of host‐guest interactions and contributes to the Ex‐De characteristics. Benefiting from facile preparation, substrate‐independent applicability, and Ex‐De characteristics, the afterglow samples are demonstrated for applications in multilevel information security fields. This work proposes a general strategy for unlocking the afterglow emission of traditional molecules, which is valuable for the discovery of high‐performance afterglow materials in the future.