Just Accepted Articles have been posted online after technical editing and typesetting for immediate view. The final edited version with page numbers will appear in the Current Issue soon.
Precisely detecting the chirality at the binding sites determined by the topological structure of G-quadruplex (G4) DNA is of paramount importance for uncovering the ligand-triggered conformational selection mechanisms and elucidating the structure-property relationship of G4 DNA. However, due to the dynamics structural nature of G4 DNA itself, real-time sensing the chirality at the binding sites in G4 DNA is challenge. Herein, we present a pioneering approach to conduct in-depth investigations on the chirality at the binding sites of G4 DNAs with parallel, hybrid, and antiparallel topological configurations by using femtosecond time-resolved circularly polarized luminescence (fs-TRCPL) spectroscopy combined with femtosecond transient absorption (fs-TA) spectroscopy. We unveiled that all three types of G4 DNAs possess two chiral active binding cites, resulting in the generation of characteristic circularly polarized luminescence (CPL) signals and time-dependent emission dissymmetry factors (glum(t)).