Double helical π-aggregate nanoarchitectonics for amplified circularly polarized luminescence

The canonical double helical pi-stacked array of base pairs within DNA interior has inspired the interest in supramolecular double helical architectures with advanced electronic, magnetic and optical functions. Here, we report a selective-recognized and chirality-matched co-assembly strategy for the fabrication of fluorescent pi-amino acids into double helical pi-aggregates, which show exceptional strong circularly polarized luminescence (CPL). The single crystal structure of the optimal combination of co-assemblies shows that the double-stranded helical organization of these pi-amino acids is cooperatively assisted by both CH-pi and hydrogen-bond arrays with chirality match. The well-defined spatial arrangement of the pi-chromophores could effectively suppress the non-radiative decay pathways and facilitate chiral exciton couplings, leading to superior CPL with a strong figure of merit (g(lum) = 0.14 and QY = 0.76). Our findings might open a new door for developing DNA-inspired chiroptical materials with prominent properties by enantioselective co-assembly initiated double helical pi-aggregation. Synthesized or self-assembled helical architectures advance the development of chiral functional materials. Here the authors report a selective-recognized and chirality-matched co-assembly strategy for the fabrication of fluorescent pi-amino acids into double helical pi-aggregates with exceptional strong circularly polarized luminescence