Amplified and Inverted Circularly Polarized Luminescence with Color Evolution from Multiple-Constituent Coassemblies...

Rationally utilizing diverse noncovalent interactions to direct multicomponent chiral coassemblies is crucial for constructing circularly polarized luminescence (CPL) materials with high dissymmetry factor (g_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 (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 g_lum values around 10^-2. Strikingly, incorporating metal ions into the binary coassembly systems inverts the handedness of CPL and significantly amplifies the |g_lum| 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.