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Organic ultra‐long room‐temperature phosphorescence (RTP) materials in the amorphous state have attracted widespread attention due to their simple preparation and flexibility to adopt various forms in sensors, bioimaging, and encryption applications. However, the amorphous molecular host for the host–guest RTP systems is highly demanded but limited. Here, a universal molecular host (DPOBP−Br) has been designed by integration of an amorphous moiety of diphenylphosphine oxide (DPO) and an intersystem crossing (ISC) group of 4‐bromo‐benzophenone (BP−Br). Various commercial fluorescence dyes were doped into the tight and transparent DPOBP−Br film, respectively, resulting in amorphous host–guest systems with ultra‐long RTP colors from green to red. It was found that DPOBP−Br acted as a universal "triplet exciton pump" for promoting the generation of triplet excitons in the guest, through energy transfer processes and external heavy‐atom effect based on DPOBP−Br. Interestingly, dynamic RTP was achieved by controlling residual oxygen concentration in the amorphous matrix by UV irradiation. Therefore, multi‐dimensional anti‐counterfeiting coatings were realized even on curved surfaces, simultaneously exhibiting spatial and 2D‐time dependence. This work provides a strategy to design new amorphous molecular hosts for RTP systems and demonstrates the advanced information encryption with tempo‐spatial resolution based on the dynamic ultra‐long RTP of an amorphous system. [ABSTRACT FROM AUTHOR]

Organic ultra‐long room‐temperature phosphorescence (RTP) materials in the amorphous state have attracted widespread attention due to their simple preparation and flexibility to adopt various forms in sensors, bioimaging, and encryption applications. However, the amorphous molecular host for the host–guest RTP systems is highly demanded but limited. Here, a universal molecular host (DPOBP−Br) has been designed by integration of an amorphous moiety of diphenylphosphine oxide (DPO) and an intersystem crossing (ISC) group of 4‐bromo‐benzophenone (BP−Br). Various commercial fluorescence dyes were doped into the tight and transparent DPOBP−Br film, respectively, resulting in amorphous host–guest systems with ultra‐long RTP colors from green to red. It was found that DPOBP−Br acted as a universal "triplet exciton pump" for promoting the generation of triplet excitons in the guest, through energy transfer processes and external heavy‐atom effect based on DPOBP−Br. Interestingly, dynamic RTP was achieved by controlling residual oxygen concentration in the amorphous matrix by UV irradiation. Therefore, multi‐dimensional anti‐counterfeiting coatings were realized even on curved surfaces, simultaneously exhibiting spatial and 2D‐time dependence. This work provides a strategy to design new amorphous molecular hosts for RTP systems and demonstrates the advanced information encryption with tempo‐spatial resolution based on the dynamic ultra‐long RTP of an amorphous system. [ABSTRACT FROM AUTHOR]