Chiral Fullerene Enables Strong, Sign-Tunable, and Full-Spectrum Circularly Polarized Luminescence with a Third-Order Nonlinear Optical Response in Liquid Crystal Matrices

Herein, we employ a chiral fulleropyrrolidine dopant to afford effective chirality amplification within liquid crystal matrices. Chiral fullerenes, when doped into nematic host 5CB at very low concentrations, effectively induce a transition to a cholesteric phase. Intriguingly, the concentration of chiral fullerene dictates the helical sense of the resulting cholesteric phase, leading to handedness inversion. As a result, subsequent incorporation with fluorescent dyes leads to multicolor circularly polarized luminescence (CPL). The luminescence dissymmetry factors can all reach values above 0.1. Moreover, the handedness of the CPL can be precisely controlled by modulating the fullerene doping concentration. Remarkably, this ternary CLC system simultaneously performs an efficient nonlinear optical response with a nonlinear absorption coefficient reaching 1.5 × 10⁵ cm GW^-1. The diverse modular design of chiral fullerene-based derivatives, combined with their chemical additivity, will open a new avenue for engineering chiroptical materials and advanced photonic devices.