Abstract
Time-resolved second harmonic generation (SHG) spectroscopy is used to investigate acetaminophen (APAP)-induced changes in the adsorption and transport properties of malachite green isothiocyanate (MGITC) dye to the surface of unilamellar 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC) liposomes in an aqueous colloidal suspension. The adsorption of MGITC to DOPC liposome nanoparticles in water is driven by electrostatic and dipole-dipole interactions between the positively charged MGITC molecules and the zwitterionic phospholipid membranes. The SHG intensity increases as the added MGITC dye concentration is increased, reaching a maximum as the MGITC adsorbate at the DOPC bilayer interface approaches a saturation value. The experimental adsorption isotherms are fit using the modified Langmuir model to obtain the adsorption free energies, adsorption equilibrium constants, and the adsorbate site densities to the DOPC liposomes both with and without APAP. The addition of APAP is shown to increase MGITC adsorption to the liposome interface, resulting in a larger adsorption equilibrium constant and a higher adsorption site density. The MGITC transport times are also measured, showing that APAP decreases the transport rate across the DOPC liposome bilayer, especially at higher MGITC concentrations. Studying molecular interactions at the colloidal liposome interface using SHG spectroscopy provides a detailed foundation for developing potential liposome-based drug-delivery systems.