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Gramicidin Lateral Distribution in Phospholipid Membranes: Fluorescence Phasor Plots and Statistical Mechanical Model
摘要： When using small mole fraction increments to study gramicidins in phospholipid membranes, we found that the phasor dots of intrinsic ?uorescence of gramicidin D and gramicidin A in dimyristoyl-sn-glycero-3-phosphocholine (DMPC) unilamellar and multilamellar vesicles exhibit a biphasic change with peptide content at 0.143 gramicidin mole fraction. To understand this phenomenon, we developed a statistical mechanical model of gramicidin/DMPC mixtures. Our model assumes a sludge-like mixture of ?uid phase and aggregates of rigid clusters. In the ?uid phase, gramicidin monomers are randomly distributed. A rigid cluster is formed by a gramicidin dimer and DMPC molecules that are condensed to the dimer, following particular stoichiometries (critical gramicidin mole fractions, Xcr including 0.143). Rigid clusters form aggregates in which gramicidin dimers are regularly distributed, in some cases, even to superlattices. At Xcr, the size of cluster aggregates and regular distributions reach a local maximum. Before a similar model was developed for cholesterol/DMPC mixtures (Sugar and Chong (2012) J. Am. Chem. Soc. 134, 1164–1171) and here the similarities and differences are discussed between these two models.
关键词： lipid bilayers,membrane organization,gramicidins,statistical mechanics,?uorescence spectroscopy,peptide-lipid interactions
更新于2025-09-23 15:21:21
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Out-of-Plane Nanoscale Reorganization of Lipid Molecules and Nanoparticles Revealed by Plasmonic Spectroscopy
摘要： Lipid bilayers assembled on solid substrates have been extensively studied with single-molecule resolution as the molecules diffuse in 2D, however the out-of-plane motion is typically ignored. Here we present sub-nanometer out-of-plane diffusion of nanoparticles attached to hybrid lipid bilayers (HBLs) assembled on metal surfaces. The nanoscale cavity formed between Au nanoparticle and Au film provides strongly-enhanced optical fields capable of locally probing HBLs assembled in the gaps. This allows us to spectroscopically resolve the nanoparticles assembled on bilayers, near edges, and in membrane defects, showing the strong influence of charged lipid rafts. Nanoparticles sitting on the edges of the HBL are observed to flip onto and off the bilayer, with flip energies of 10 meV showing how thermal energies dynamically modify lipid arrangements around a nanoparticle. We further resolve the movement of individual lipid molecules by doping the HBL with low concentrations of Texas-red (TxR) dye-labeled lipids.
关键词： Purcell factor,Plasmonics,Single-molecule,Nano-assembly,Nanocavities,Lipid bilayers
更新于2025-09-23 15:19:57
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Formation of lipid bilayers on the pore walls of macroporous silicon
摘要： Electron paramagnetic resonance (EPR) spectroscopy was used to study the pore filling of macroporous silicon with lipid vesicles (liposomes), added with a spin label. Different EPR spectra were obtained with the magnetic field parallel and perpendicular to the macroporous silicon sample surface. These spectra could be well simulated with an admixture of the isotropic spectrum of liposomes, plus a simulated spectrum corresponding to a cylindrical distribution of lipid bilayers. This means that a portion of the liposomes were disrupted, and supported lipid bilayers were formed covering the inner surface of the pores. Diverse protocols can be explored in order to optimize the lipid covering of the pore walls, and to achieve an adequate lipid hydration. This system can be used as a platform to study lipid phase transitions in a confined environment, and to characterize membrane proteins.
关键词： Liposomes,Electron paramagnetic resonance/electron spin resonance,Supported lipid bilayers,Porous silicon,Spin labels
更新于2025-09-19 17:15:36
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Nanoparticles at Biomimetic Interfaces: A Combined Experimental and Simulation Study on Charged Gold Nanoparticles/Lipid Bilayers Interfaces
摘要： The poor understanding of the interaction of nanomaterials with biologically relevant interfaces is recognized as one of the major issues currently limiting the development of nanomedicine. The central purpose of this study is to compare experimental (Confocal Microscopy, Fluorescence Correlation Spectroscopy, X-ray Reflectivity) and computational (Molecular Dynamics simulations) results to thoroughly describe the interaction of cationic gold nanoparticles (AuNP) with mixed zwitterionic/anionic lipid membranes. The adhesion of AuNPs to the lipid membrane is investigated on different length scales from a structural and dynamical point of view; with this approach, a series of complex phenomena, spanning from lipid extraction, localized membrane disruption, lateral phase separation and slaved diffusion, are characterized and interpreted from a molecular level to macroscopic observations.
关键词： Nanoparticles,Gold Nanoparticles,Molecular Dynamics,X-ray Reflectivity,Fluorescence Correlation Spectroscopy,Lipid Bilayers,Biomimetic Interfaces,Confocal Microscopy
更新于2025-09-04 15:30:14
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Charge and Coordination Directed Liposome Fusion onto SiO2 and TiO2 Nanoparticles
摘要： TiO2 and SiO2 are very useful materials for building biointerfaces. A particular interesting aspect is their interactions with lipid bilayers. Many past research efforts focused on phosphocholine (PC) lipids, which form supported lipid bilayers (SLB) on SiO2 at physiological conditions but are adsorbed as intact liposomes on TiO2. Low pH was required to form PC SLBs on TiO2. This work intends to understand the surface forces and chemistry responsible for such differences. Two charge neutral lipids: 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC) and 2-((2,3-bis(oleoyloxy)propyl)dimethylammonio)ethyl ethyl phosphate (DOCPe); and two negatively charged lipids: 1,2-dioleoyl-sn-glycero-3-phospho-L-serine (DOPS) and 2-((2,3-bis(oleoyloxy)propyl)dimethylammonio)ethyl hydrogen phosphate (DOCP) were used. Using calcein leakage assays, adsorption measurement, cryo-TEM, and washing, we concluded that charge is the dominating factor on SiO2. The two neutral lipids form SLB on SiO2 at pH 3 and 7, but the two negatively charged ones cannot form. On TiO2, both charge and coordination chemistry are important. The two anionic lipids formed SLB from pH 3 to 10. DOCP had stronger affinity than DOPS likely due to the tighter terminal phosphate binding of the former. The two neutral liposomes formed SLB only at pH 3, where phosphate interaction and van der Waals force are deemed important. The pH 3 prepared TiO2 DOPC SLBs are destabilized at neutral pH, indicating reversible nature of the interaction. This work has provided new insights into two important materials interacting with common liposomes, which are important for reproducible biosensing, device fabrication, and drug delivery applications.
关键词： coordination chemistry,liposome fusion,SiO2,TiO2,charge,supported lipid bilayers
更新于2025-09-04 15:30:14