Manipulation of time-dependent multicolour evolution of X-ray excited afterglow in lanthanide-doped fluoride nanoparticles

External manipulation of emission colour is of significance for scientific research and applications, however, the general stimulus-responsive colour modulation method requires both stringent control of microstructures and continously adjustment of particular stimuli conditions. Here, we introduce pathways to manipulate the kinetics of time evolution of both intensity and spectral characteristics of X-ray excited afterglow (XEA) by regioselective doping of lanthanide activators in core-shell nanostructures. Our work reported here reveals the following phenomena: 1. The XEA intensities of multiple lanthanide activators are significantly enhanced via incorporating interstitial Na⁺ ions inside the nanocrystal structure. 2. The XEA intensities of activators exhibit diverse decay rates in the core and the shell and can largely be tuned separately, which enables us to realize a series of core@shell NPs featuring distinct time-dependent afterglow colour evolution. 3. A core/multi-shell NP structure can be designed to simultaneously generate afterglow, upconversion and downshifting to realize multimode time-dependent multicolour evolutions. These findings can promote the development of superior XEA and plentiful spectral manipulation, opening up a broad range of applications ranging from multiplexed biosensing, to high-capacity information encryption, to multidimensional displays and to multifunctional optoelectronic devices.