ABSTRACT Lanthanide(III) coordination scintillators feature efficient triplet harvesting and narrow‐band emission, making them promising for X‐ray imaging applications. However, their rigid coordination environments hinder melt‐processing into large‐area, transparent glassy scintillator screens. Herein, a “rigid‐node flexible‐linker” molecular design strategy that facilitates chain‐mobility‐enabled glass‐forming in lanthanide coordination scintillators by constructing one‐dimensional (1D) coordination chains is proposed. By integrating dibenzoylmethane antenna with flexible dual‐phosphine‐oxide linkers (OP‐Cn, n = 2, 4, 6, 8), a series of 1D Eu‐OP‐Cn coordination polymers is constructed, enabling the simultaneous realization of efficient ligand‐sensitized radioluminescence and the chain‐mobility required for vitrification, thereby allowing transformation from crystalline powders into glassy states. Benefiting from rigid local coordination environments that suppress nonradiative decay, crystalline Eu‐OP‐C2 exhibits a near‐unity photoluminescence quantum yield (97.5%) and an ultrahigh relative light yield of 70379 photons MeV −1 . Besides, elongating the alkyl‐chain length increases segmental flexibility, allowing Eu‐OP‐C6/C8 to form water‐stable, transparent glassy scintillators via melt‐quenching method. Notably, Eu‐OP‐C8 glass delivers radioluminescence intensity 12.1 times higher than Bi 4 Ge 3 O 12 , enabling high‐resolution X‐ray imaging (> 30 lp mm −1 ) and real‐time underwater X‐ray videography (2K, 60 fps). Moreover, this strategy is readily extendable to Tb 3+ , Sm 3+ and Dy 3+ , establishing a general molecular‐design paradigm for melt‐processable lanthanide coordination glassy scintillators.
Wei et al. (Fri,) studied this question.