Amplified and Inverted Circularly Polarized Luminescence with Color Evolution from Multiple-Constituent Coassemblies Directed by Diverse Noncovalent Forces

Rationally utilizing diverse noncovalent interactions to direct multicomponent chiral coassemblies is crucial for constructing circularly polarized luminescence (CPL) materials with high dissymmetry factor (<i>g</i>_lum) and precisely controlled emission colors and handedness, which are essential for advanced optical devices and display technologies. Herein, we show the programmable coassembly of fluorenylmethyloxycarbonyl (Fmoc)-conjugated phenylalanine (<b>Phe</b>) and pyrene derivatives (<b>Py1</b> and <b>Py2</b>) with different alkyl spacer lengths, which shall form ternary coassemblies with metal ions, octafluoronaphthalene (<b>OFN</b>), or 1,2,4,5-tetracyanobenzene (<b>TCNB</b>) through coordination, arene-perfluoroarene, or charge transfer forces, to enhance and flexibly control the chiroptical properties. The binary assemblies of <b>Phe/Py1</b> and <b>Phe/Py2</b> display opposite CPL with <i>g</i>_lum values around 10^-2. Strikingly, incorporating metal ions into the binary coassembly systems inverts the handedness of CPL and significantly amplifies the |<i>g</i>_lum| values (reaching up to 0.15). CPL properties of <b>Phe/Py1-2</b> can be further controlled by coassembling with <b>OFN</b> and <b>TCNB</b>, achieving inverted handedness, tunable emission bands, and dissymmetry factors. This work provides insight into how diverse noncovalent forces drive multiple-constituent chiral coassembly through different pathways, which would be helpful for the development of highly efficient and significantly tuned CPL materials.