The CuI-derived inorganic−organic hybrid compounds are considered as promising phosphors for the lighting industry. Herein, exploiting N-monoalkylated hexaminium salts, [R-HMTA]X (R = Me, Et, Pr, and propargyl; X = Cl and I), as multibridging ligands, we have designed and synthesized a unique class of one-dimensional and two-dimensional hybrid CuImaterials. The reactions of these salts with CuI give rise to Allin-One (AIO) type compounds combining ionic and dative bonds between inorganic and organic components. The latter is formed by structurally unique inorganic [Cu x I y ] (y−x)− clusters, chains, or sheets interconnected through [R-HMTA] + cations via multiple Cu−N bonds. The so-designed compounds at ambient temperature exhibit tunable luminescence spanning from deep blue to red color (λ em = 430−625 nm) with microsecond lifetimes and the quantum efficiency of up to 78%. Remarkably, the AIO materials feature nontrivial excitation-(ED) and temperature-dependent (TD) luminescence, allowing their emission color to be finely adjusted from deep blue to red through changing the excitation wavelength and/or temperature. Based on the TD emission spectroscopy and theoretical calculations, a possible mechanism of the luminescence has been proposed. The very interesting luminescence characteristics coupled with good thermal and photostability render these AIO hybrid materials possible candidates for applications in energy-efficient lighting devices.

First examples of zwitterionic CuI-based complexes showing red photoluminescence are reported.

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