Induction of a Four‐Way Junction Structure in the DNA Palindromic Hexanucleotide 5′‐d(CGTACG)‐3′ by a Mononuclear Platinum Complex

Abstract

are supramolecular DNAa ssemblies comprising four interacting DNAs trands that in biology are involved in DNA-damage repair.I nt his study,anew mononuclear platinum(II) complex 1 was prepared that is capable of driving the crystallization of the DNAoligomer 5'-d(CGTACG)-3' specifically into a4WJ-like motif.I nt he crystal structure of the 1-CGTACGa dduct, the distorted-square-planar platinum complex binds to the core of the 4WJ-like motif through p-p stacking and hydrogen bonding,without forming any platinum-nitrogen coordination bonds.O ur observations suggest that the specific molecular properties of the metal complex are crucially responsible for triggering the selective assembly of this peculiar DNAs uperstructure.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.org/10.

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“…133 In 2019, Van Rixel et al used the QM/MM technique to describe aromatic Pt-compound intercalation-binding mode to a noncanonical site created by two DNA tetrads, as well as the drug-induced deformation. 134 The studies on Au(I)-compounds binding to telomeric DNA G-quadruplex were experimentally confirmed using ESI-MS and X-ray diffraction, while QM/MM simulations confirmed its binding mode within a G-quadruplex. 135 Apart from biomolecule interactions, QM/MM was also successfully used to investigate the emission spectrum of platinum(II) bipyridine complex, which was due to the excited state of metal–metal to ligand charge transfer triplet ( 3 MMLCT).…”

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“…This deprotonation is interpreted as a consequence of the high electrophilicity of the Au(III) center, which draws the electron density of the conjugated ligand, thereby making the NH bridges very acidic. 54 The Au-N bond lengths of all complexes were similar, within the range of 1.977-2.044 Å (Supporting Information Table S4). However, [2] + and [3] + showed much more distorted coordination spheres than [1] 2+ , with a higher tetrahedral distortion index τ = 0.179 and 0.167, respectively, compared with τ = 0.109 for [1] 2+ .…”

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“…139 Regarding 4WJs, the first metal complex (square planar Pt 2+ chelated by a tetradentate polypyridyl ligand) that acts as an effective template for the assembly of a 4WJ-like DNA superstructure has been described. 140 Metal complexes, due to their own high tolerance for structural and electronic modification, can clearly exploit various DNA binding sites with great success. 80,94,134,141 Moreover, metal complexes may interact with a diverse range of molecular targets, not limited to DNA, which might allow the development of metallodrugs with multi-faceted cellular targets.…”