Shedding light on membrane-templated clustering of gold nanoparticles

Montis, Costanza; Caselli, Lucrezia; Valle, Francesco; Zendrini, Andrea; Carlà, Francesco; Schweins, Ralf; Maccarini, Marco; Bergese, Paolo; Berti, Debora

doi:10.1016/j.jcis.2020.03.123

Cited by 40 publications

(44 citation statements)

References 54 publications

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“…This result further extends the characterisation of NPs–lipid interaction and corroborates our vision of rafts’ boundaries as regions of increased permeability (Kuzmin et al ., 2005; Rawicz et al ., 2008; Sheikh & Jarvis, 2011), where the membrane can easily wrap around the adsorbed NPs. Recent findings (Montis et al ., 2020) confirm these results, suggesting that free‐standing lipid bilayers can bend around the AuNPs surface, guided by citrate‐lipid ligand exchange at the interface. All the above hypotheses are confirmed by the evaluation of the AuNPs contact angle with respect to the SLB.…”

Section: Resultssupporting

confidence: 57%

Gold nanoparticles interacting with synthetic lipid rafts: an AFM investigation

Ridolfi

Caselli

Montis

et al. 2020

Journal of Microscopy

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Inorganic nanoparticles (NPs) represent promising examples of engineered nanomaterials, providing interesting biomedical solutions in several fields, like therapeutics and diagnostics. Despite the extensive number of investigations motivated by their remarkable potential for nanomedicinal applications, the interactions of NPs with biological interfaces are still poorly understood. The effect of NPs on living organisms is mediated by biological barriers, such as the cell plasma membrane, whose lateral heterogeneity is thought to play a prominent role in NPs adsorption and uptake pathways. In particular, biological membranes feature the presence of rafts, that is segregated lipid micro and/or nanodomains in the so-called liquid ordered phase (L o), immiscible with the surrounding liquid disordered phase (L d). Rafts are involved in various biological functions and act as sites for the selective adsorption of materials on the membrane. Indeed, the thickness mismatch present along their boundaries generates energetically favourable conditions for the adsorption of NPs. Despite its clear implications in NPs internalisation processes and cytotoxicity, a direct proof of the selective adsorption of NPs along the rafts' boundaries is still missing to date. Here we use multicomponent supported lipid bilayers (SLBs) as reliable synthetic models, reproducing the nanometric lateral heterogeneity of cell membranes. After being characterised by atomic force microscopy (AFM) and neutron reflectivity (NR), multidomain SLBs are challenged by prototypical inorganic nanoparticles, that is citrated gold nanoparticles (AuNPs), under simplified and highly controlled conditions. By exploiting AFM, we demonstrate that AuNPs preferentially target lipid phase

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Section: Resultssupporting

confidence: 57%

Gold nanoparticles interacting with synthetic lipid rafts: an AFM investigation

Ridolfi

Caselli

Montis

et al. 2020

Journal of Microscopy

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“…This finding is fully in line with a recent report 44 , where AuNPs wrapping, modulated by the membrane bending modulus, is recognized as the main driver for the membrane-templated aggregation of AuNPs, through the mechanism sketched in Figure 3c We chose EVs to further validate the method and to provide evidence of its applicability on membranous nanoparticles which are more challenging both in terms of compositional and structural complexity, as well as in analyte availability. Specifically, we assayed a sample EVs from the murine cell line TRAMP-C2, with size and z-potential similar to the PC synthetic liposomes (see Supporting Information for details).…”

Section: Si)supporting

confidence: 86%

A Plasmon-Based Nanoruler to Probe the Mechanical Properties of Synthetic and Biogenic Nanosized Lipid Vesicles

Caselli

Ridolfi²,

Cardellini³

et al. 2020

Preprint

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<p><b>Membrane-delimited compartments, as lipid vesicles, are ubiquitous in natural and synthetic systems. The mechanical properties of such vesicles are crucial for several physical, chemical, and biological processes. However, their accurate determination is still challenging and requires sophisticated instruments and data analysis. Here we report the first evidence that the surface plasmon resonance (SPR) of citrated gold nanoparticles (AuNPs) adsorbed on synthetic vesicles is finely sensitive to the vesicles’ mechanical properties. We leverage this finding to demonstrate that the spectrophotometric tracking of the SPR provides quantitative access to the stiffness of vesicles of synthetic and natural origin, such as extracellular vesicles (EVs). This plasmon-based “stiffness nanoruler” paves the way for developing a facile, cost-effective, and high-throughput method to assay the mechanical properties of vesicles of nanometric size and unknown composition.</b></p>

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“…The preferential interaction of individual NPs with lipid phase boundaries further suggests that bilayer‐mediated interactions could drive the assembly of NPs that induce local changes to bilayer curvature upon adsorption, potentially leading to attractive interactions that overcome the electrostatic repulsion between charged NPs. Supporting this hypothesis, some experiments have demonstrated that small, charged NPs assemble on the surface of vesicles 31,43‐45 . Continuum modeling and mesoscopic particle‐based simulations have similarly shown that bilayer‐mediated interactions can drive NP assembly 46‐48 .…”

Section: Introductionmentioning

confidence: 93%

“…that small, charged NPs assemble on the surface of vesicles. 31,[43][44][45] Continuum modeling and mesoscopic particle-based simulations have similarly shown that bilayer-mediated interactions can drive NP assembly. [46][47][48] However, these methods often predict substantially larger membrane deformations than observed in CG or atomistic MD simulations, and the methods neglect intermolecular interactions between NPs (such as electrostatic interactions) that could compete against bilayer-mediated attraction.…”

Section: Supporting This Hypothesis Some Experiments Have Demonstratedmentioning

confidence: 99%

Bilayer‐mediated assembly of cationic nanoparticles adsorbed to lipid bilayers: Insights from molecular simulations

Sheavly

Lehn

2020

AIChE Journal

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Understanding interactions between functionalized gold nanoparticles (NPs) and lipid bilayers is essential for biomedical applications. Experiments have shown that NPs that are stable in solution can assemble into clusters when adsorbed to a lipid bilayer, suggesting that bilayer-mediated interactions facilitate assembly. In this work, we use coarse-grained molecular dynamics simulations to study bilayer-mediated interactions between NPs adsorbed to single-and multicomponent lipid bilayers. We perform unbiased simulations and umbrella sampling calculations using an implicit solvent force field to determine the thermodynamic contributions to assembly. We show that bilayer-mediated interactions drive the assembly of NPs into linear aggregates on liquid-disordered bilayers, which we attribute to a reduction in bilayer curvature. Similar bilayer-mediated interactions induce the alignment of NP clusters with phase boundaries in phase-separated bilayers. Together, these simulation results provide new physical insight into the balance of forces that dictate the assembly of charged NPs at multicomponent lipid bilayer interfaces.

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Shedding light on membrane-templated clustering of gold nanoparticles

Cited by 40 publications

References 54 publications

Gold nanoparticles interacting with synthetic lipid rafts: an AFM investigation

Gold nanoparticles interacting with synthetic lipid rafts: an AFM investigation

A Plasmon-Based Nanoruler to Probe the Mechanical Properties of Synthetic and Biogenic Nanosized Lipid Vesicles

Bilayer‐mediated assembly of cationic nanoparticles adsorbed to lipid bilayers: Insights from molecular simulations

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