Chiral Memory‐Driven Helical Supramolecular Photodetector for Deciphering Circularly Polarized Light

ABSTRACT Chiral π‐conjugated organic small molecules, due to their intrinsic chirality, well‐defined molecular structures and ease of modification, are promising for circularly polarized light (CPL) detection. However, their practical application is hindered by low absorption dissymmetry factor ( g abs ), arising from imbalanced electric and magnetic transition dipole moments ( µ and m ). Here, a template‐free method using chiral memory effect was reported to fabricate helical supramolecules with high g abs . Two chiral dinaphthocoronene tetraimides enantiomer pairs were synthesized: ( R )‐PDI‐( R )‐NI‐Ph/( S )‐PDI‐( S )‐NI‐Ph and ( S )‐PDI‐( R )‐NI‐Ph/( R )‐PDI‐( S )‐NI‐Ph. After annealing films at 350°C to remove chiral pendants, ( R )‐PDI‐( R )‐NI/( S )‐PDI‐( S )‐NI films showed much higher | g abs | (0.08) than the other set (0.01), with helical assemblies formed via chiral memory effect. Notably, large‐area arrays of ( R )‐PDI‐( R )‐NI films enabled CPL imaging, and a bionic artificial visual system was constructed with this film as “retina” and an artificial neural network as “neural center” for reliable CPL discrimination, offering a scalable strategy for high‐performance chiral optoelectronics.