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Christine A Gobrogge1, Robert A Walker1,2

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This study quantifies how coumarin dyes partition into lipid vesicles using time-resolved fluorescence. Coumarin 152 shows a significantly higher affinity for lipid bilayers compared to coumarin 461, with partitioning thermodynamics varying with temperature.

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Area of Science:

  • Biophysics
  • Physical Chemistry
  • Materials Science

Background:

  • Lipid bilayers are crucial in biological systems, influencing drug delivery and membrane protein function.
  • Understanding solute partitioning into lipid bilayers is key to designing effective drug delivery systems.
  • 7-aminocoumarin dyes offer unique fluorescence properties for probing microenvironments.

Purpose of the Study:

  • To characterize and quantify the partitioning of coumarin 152 (C152) and coumarin 461 (C461) into 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) lipid vesicles.
  • To investigate the influence of solute concentration and temperature on solute-lipid interactions.
  • To determine the thermodynamic parameters governing solute partitioning.

Main Methods:

  • Time-resolved fluorescence spectroscopy was employed to monitor coumarin dye behavior.
  • Multiexponential fluorescence decay analysis was used to differentiate solute populations.
  • Partition coefficients and thermodynamic quantities (enthalpy, entropy) were calculated from fluorescence data.

Main Results:

  • C152 exhibited approximately 10-fold greater affinity for DPPC lipid bilayers than C461.
  • Solute partitioning was observed in the aqueous buffer, vesicle headgroup region, and bilayer interior.
  • Partitioning was exothermic with negative entropy changes below and above the lipid phase transition temperature.
  • Near the transition temperature, partitioning became endothermic and entropically favored.

Conclusions:

  • The chemical structure, specifically the 4-position substituent, significantly impacts coumarin dye affinity for lipid bilayers.
  • Temperature-dependent thermodynamics reveal distinct partitioning behaviors across the lipid gel-liquid crystalline phase transition.
  • These findings provide insights into solute-membrane interactions relevant for drug delivery and biophysical studies.