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 (glum) 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 (Phe) and pyrene derivatives (Py1 and Py2) with different alkyl spacer lengths, which shall form ternary coassemblies with metal ions, octafluoronaphthalene (OFN), or 1,2,4,5-tetracyanobenzene (TCNB) through coordination, arene-perfluoroarene, or charge transfer forces, to enhance and flexibly control the chiroptical properties. The binary assemblies of Phe/Py1 and Phe/Py2 display opposite CPL with glum values around 10–2. Strikingly, incorporating metal ions into the binary coassembly systems inverts the handedness of CPL and significantly amplifies the |glum| values (reaching up to 0.15). CPL properties of Phe/Py1–2 can be further controlled by coassembling with OFN and TCNB, 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.