Molecular restructuring of water and lipids upon the interaction of DNA with lipid monolayers

R. Kramer Campen, Thuy Ngo, Maria Sovago, Jean Marie Ruysschaert, Mischa Bonn

Research output: Contribution to journalArticle

33 Citations (Scopus)

Abstract

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 D 2O, 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.

Original languageEnglish (US)
Pages (from-to)8037-8047
Number of pages11
JournalJournal of the American Chemical Society
Volume132
Issue number23
DOIs
StatePublished - Jun 16 2010
Externally publishedYes

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Lipids
Monolayers
DNA
Water
Gene therapy
Vibrational spectra
Propane
Genetic Therapy
Adsorption
Labels
Calcium
Spectrum Analysis
Spectroscopy

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Molecular restructuring of water and lipids upon the interaction of DNA with lipid monolayers. / Campen, R. Kramer; Ngo, Thuy; Sovago, Maria; Ruysschaert, Jean Marie; Bonn, Mischa.

In: Journal of the American Chemical Society, Vol. 132, No. 23, 16.06.2010, p. 8037-8047.

Research output: Contribution to journalArticle

Campen, R. Kramer ; Ngo, Thuy ; Sovago, Maria ; Ruysschaert, Jean Marie ; Bonn, Mischa. / Molecular restructuring of water and lipids upon the interaction of DNA with lipid monolayers. In: Journal of the American Chemical Society. 2010 ; Vol. 132, No. 23. pp. 8037-8047.
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