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New synthesis of multi-layer 3D chiral molecules has been developed under novel conditions to give better outcomes. The aggregation-induced emission (AIE), UV irradiation/excitation, charge transfer (CT) and local excited (LE) ππ* transitions have been investigated on a representative individual enantiomer of pseudo C2asymmetry 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.