Abstract
In this work we present the results of a molecular simulation study of the interaction between a tetracationic his iron(II) supramolecular cylinder, [Fe2(C25H20N4)3] 4+, and DNA. This supramolecular cylinder has been shown to bind in the major groove of DNA and to induce dramatic coiling of the DNA. The simulations have been designed to elucidate the interactions that lead the cylinder to target the major groove and that drive the subsequent DNA conformational changes. Three sets of multi-nanosecond simulations have been performed: one of the uncomplexed d(CCCCCTTTTTCC)· d(GGAAAAAGGGGG) dodecamer; one of this DNA complexed with the cylinder molecule; and one of this DNA complexed with a neutralised version of the cylinder. Coiling of the DNA was observed in the DNA - cylinder simulations, giving insight into the molecular level nature of the supramo lecular coiling observed experimentally. The cylinder charge was found not to be essential for the DNA coiling, which implies that the DNA response is moderated by the short range interactions that define the molecular shape. Cylinder charge did, however, affect the integrity of the DNA duplex, to the extent that, under some circumstances, the tetracationic cylinder induced defects in the DNA base pairing at locations adjacent to the cylinder binding site.
Original language | English |
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Pages (from-to) | 3493-3506 |
Number of pages | 14 |
Journal | Chemistry - A European Journal |
Volume | 12 |
Issue number | 13 |
DOIs | |
Publication status | Published - 24 Apr 2006 |
Externally published | Yes |
Keywords
- Bio-supramolecular chemistry
- DNA recognition
- Helical structures
- Molecular dynamics
- Noncovalent interactions