New synthesis of multi-layer 3D chiral molecules has been developed under novel conditions to give better outcomes.The aggregation-induced emission (ALE),UV irradiation/excitation,charge transfer (CT) and local excited (LE) ππ* transitions have been investigated on a representative individual enantiomer of pseudo C2 asymmetry which was made possibly by differentiating moieties on phosphorous on N-phosphonyl ring of chiral sandwich framework.Meanwhile,a new tandem C-N/C-C coupling reaction was unexpectedly rendered providing a novel access to special benzo[a]carbazoles.