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Summary

A DNA fluorescent probe shows high affinity for the dodecane/water interface and negatively charged lipid interfaces. Its adsorption behavior is influenced by lipid charge and molecular orientation at the interface.

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Area of Science:

  • Interfacial science
  • Molecular dynamics simulations
  • Fluorescent probe chemistry

Background:

  • Understanding molecular interactions at interfaces is crucial for various applications.
  • DNA fluorescent probes are valuable tools for studying biological systems.
  • Lipid interfaces play key roles in biological membranes and drug delivery systems.

Purpose of the Study:

  • To investigate the adsorption of a thiazole orange DNA fluorescent probe at oil-water and lipid-water interfaces.
  • To determine the influence of lipid charge on probe adsorption.
  • To elucidate the molecular mechanisms governing probe-interface interactions.

Main Methods:

  • Surface Second Harmonic Generation (SSHG) spectroscopy to probe interfacial molecular orientation and concentration.
  • All-atomistic Molecular Dynamics (MD) simulations to model interfacial behavior at the atomic level.
  • Calculation of Gibbs free energy of adsorption to quantify binding affinity.

Main Results:

  • The DNA probe exhibits high affinity for the dodecane/water interface (Gibbs free energy ~ -45 kJ/mol).
  • Similar high affinity was observed at dodecane/phospholipid/water interfaces with negatively charged DPPG lipids.
  • No significant adsorption occurred at interfaces with zwitterionic DPPC lipids, attributed to unfavorable Coulombic interactions.
  • Probe orientation differs between bare and DPPG-coated interfaces, with intercalation into DPPG monolayers.

Conclusions:

  • The cationic DNA probe strongly adsorbs at hydrophobic-hydrophilic interfaces, with affinity modulated by lipid charge.
  • Coulombic interactions are critical in determining probe adsorption at lipid interfaces.
  • The probe's interfacial orientation is adaptable, allowing it to intercalate into charged lipid monolayers for enhanced stabilization.