In Situ Heterodyne-Detected Second-Harmonic Generation Study of the Influence of Cholesterol on Dye Molecule Adsorption on Lipid Membrane.

J Phys Chem B

Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

Published: February 2024


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Article Abstract

Cholesterol plays an essential role in regulating the functionality of biomembranes. This study employed in situ second-harmonic generation (SHG) to investigate the adsorption behavior of the dye molecule 4-(4-(diethylamino)styryl)--methyl-pyridinium iodide (D289) on a biomimic membrane composed of 1,2-dipalmitoyl--glycero-3-phospho-(1'-rac-glycerol) (sodium salt) (DPPG) and cholesterol. The time-dependent polarization SHG intensity exhibited an initial rapid increase, followed by a subsequent decline. The initial increased SHG intensity is responsible for the electrostatic interaction-driven adsorption of D289 onto the membrane, while the decrease in the SHG signal results from the broadening of the orientation distribution within the membrane. Heterodyne-detected SHG (HD-SHG) measurements demonstrated that the adsorption of dye molecules influenced the phase of the induced electric field. The interfacial potential Φ(0) as a function of time was measured, and we found that even after reaching a stable Stern layer state, the diffusion layer continued to exhibit a dynamic change. This study offers a comprehensive understanding of the influence of cholesterol on adsorption, reorientation dynamics, and dynamic changes in the reorientation of water in the diffusion layer.

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http://dx.doi.org/10.1021/acs.jpcb.3c07130DOI Listing

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