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To study the binding mechanism of 4',6-diamidino-2-phenylindole (DAPI) and polyphosphate (Poly-P) and find fluorescent dyes which can dye Poly-P better, the interaction model of DAPI and Poly-P was calculated by the self-consistent-charge, density functional tight-binding (SCC-DFTB-D) method, and the binding sites of DAPI and Poly-P were analyzed. Further, Cy3, Rhodamine 6G and Fluorescein, which are structurally similar to DAPI, were selected to analyze their interactions with Poly-P. The binding energies and frontier orbital properti