CPL-active hybrid copper(I) halides enabled by cation inclusion with chiral crown-ether

Chiral hybrid metal halides with high photoluminescence quantum yield (PLQY) and superior dissymmetry factor (g_lum) are promising candidates for circularly polarized luminescence (CPL) emitting sources. However, it is a great challenge to achieve both high g_lum and large PLQY. Here, we report a new supramolecular strategy to fabricate chiral hybrid Cu(I)-halides with near-unity quantum yields and intense CPL emissions. The dissymmetry factor can be dramatically modulated by tuning the host-guest complexations. Attributing to the chirality and variable conformations of the host-guest complexes, a series of chiral [G@L^R/S]₂Cu₄I₆ have been prepared. The incorporation of different cations within the chiral L^R/S hosts leads to variations of packing modes along the c-axis and different extent of distortions in the [Cu₄I₆]²⁻polyhedra. Among them, [H₃O@L^R/S]⁺ cations are stacked based on Van der Waals interactions and hierarchically self-assemble into a right/left-handed helix in [H₃O@L^R/S]₂Cu₄I₆, which results in a high g_lum of −7×10⁻³ and a large PLQY of 96.92%. Notably, [G@L^R/S]₂Cu₄I₆ shows promising applications in single-component white light emitting diodes (WLEDs), exhibiting a maximum dissymmetry factor of −1.2×10⁻³. The effective host-guest complexation and oriented hierarchical self-assembly provide an effective strategy for the development of high-performance CPL materials.