TY - DATA T1 - Molecular Restructuring of Water and Lipids upon the Interaction of DNA with Lipid Monolayers PY - 2010/06/16 AU - R. Kramer Campen AU - Thuy T. M. Ngo AU - Maria Sovago AU - Jean-Marie Ruysschaert AU - Mischa Bonn UR - https://acs.figshare.com/articles/journal_contribution/Molecular_Restructuring_of_Water_and_Lipids_upon_the_Interaction_of_DNA_with_Lipid_Monolayers/2760079 DO - 10.1021/ja100838q.s001 L4 - https://ndownloader.figshare.com/files/4453339 KW - CH stretch modes KW - OD stretch KW - water structure KW - gene therapy KW - Molecular Restructuring KW - cationic system KW - D 2O KW - zwitterionic lipid monolayers KW - lipid tails KW - lipid interface KW - DNA KW - DPPC KW - DPTAP KW - lipid cofactors KW - lipid monolayers KW - Lipid MonolayersUnderstanding KW - VSF N2 - Understanding the molecular mechanism of DNA/lipid interaction is critical in optimizing the use of lipid cofactors in gene therapy. Here, we address this question by employing label-free vibrational sum frequency (VSF) spectroscopy to study the interaction of DNA with lipid monolayers of the cationic lipids DPTAP(1,2-dipalmitoyl-3-trimethylammonium-propane) and diC14-amidine as well as the zwitterionic lipid DPPC (1,2-dipalmitoyl-sn-glycero-3-phosphocholine) in the presence and absence of calcium. Our approach has the advantage both of allowing us to explicitly probe intermolecular interactions and of providing insight into the structure of water and lipids around DNA at the lipid interface. We find, by examination of the OD stretch of interfacial D2O, that water structure differs markedly between systems containing DNA adsorbed to cationic and those that contain DNA adsorbed to zwitterionic lipid monolayers (in the presence or absence of Ca2+). The spectral response of interfacial water in the cationic system is consistent with a highly structured, undercoordinated, structural ‘type’ of water. Further, by investigation of CH stretch modes of the diC14-amidine lipid tails, we demonstrate that the adsorption of DNA to this lipid leads to increased ordering of lipid tails. ER -