Self-Assembly of Cholesteryl Carbon Dots with Circularly Polarized Luminescence in Solution and Solvent-Free Phases

: Incorporating carbon dots (CDs) into chiral self-assemblies will endow the system with intriguing optoelectronic, catalytic, and chiroptical activities. Utilization of chiral substituents to rationally manipulate chiral self-assembly of the CDs, however, remains a major challenge. In this work, cholesteryl monoprotected ethylene diamine was used as a precursor to synthesize CDs with a cholesteryl periphery. The rigid, apolar, and chiral cholesteryl facilitates the polarity-sensitive self-assembly of CDs in organic solvents, showing circularly polarized luminescence (CPL) with dissymmetry g-factor at 10-3 grade. Temperature-variable characterizations suggested the formation of thermotropic liquid crystals within a wide temperature range driven by the interdigitation of cholesteryl segments, which further anchor the graphitic CD cores into tetragonal and cubic arrays. Self-assembly in a solvent-free state arouses sufficient chirality transfer and boosted the g-factors to 10-2 order of magnitude. This work unveils multiple and chiral self-assembly of CDs controlled by the cholesteryl substituents, exhibiting variable architectures and tunable CPL.