Deprotonation-mediated vitrification of organic-inorganic hybrid perovskites

Glasses made from organic-inorganic hybrid perovskites are emerging non-crystalline semiconducting materials whose versatile composition and exceptional processability allow for manifold applications. The current melt-quenching approaches are compatible to only few perovskite crystals, as most undergo irreversible decomposition prior to melting. Herein, we report a general flux-mediated approach to produce a library of high-quality perovskite glasses with different organic molecules, metal centers, and framework dimensionality. We show that the partial deprotonation of organic moiety by alkali metal hydroxide flux modulates the intermolecular interactions in perovskites, and activates the flow unit, which depresses the fusion temperature ranging 21–77 °C with flux ratio <1.1 wt%. More critically, the utilization of hydroxide flux creates a large melt window, and enables the thermal vitrification of many inherently non-meltable systems, such as (BA)₂PbI₄ (BA = butylamine) and (DGA)PbI₄ (DGA = 1,1-dimethylbiguanide). Using these semiconductive glasses, we realize high-performance X-ray detection devices showing a sensitivity of 35674.1 μC Gy_air⁻¹ cm⁻² under 500 V mm⁻¹ electric field, and a high-resolution X-ray imaging system via its seamless integration on commercial thin-film transistor backplanes.