Lipid Hydroperoxidation Effect on the Dynamical Evolution of the Conductance Process in Bilayer Lipid Membranes: A Condition Toward Criticality

Corvalán, Natalia Andrea; Caviglia, Agustin F.; Felsztyna, Iván; Itri, Rosângela; Lascano, Ramiro

doi:10.1021/acs.langmuir.0c01243

Cited by 10 publications

(8 citation statements)

References 69 publications

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“…Here, the snorkelling POPC-OOH chains lead to POPC depletion at the water/lipid interface and, simultaneously, to a higher density of the lipid tails from the non-oxidized POPC lipid molecules and the bilayer’s core. We also observed an increase in water penetration with increasing amounts of POPC-OOH, in agreement with previous reports 36 , 37 , 75 . With regard to the location of BC10, peak density was within the highest density region of the membrane and in a similar location to our previous studies 55 , 76 , 77 , regardless of the bilayer’s composition (Fig.…”

Section: Resultssupporting

confidence: 93%

“…Our data suggests, for the first time, that lipid peroxides can cluster together creating regions of higher order, even in the absence of canonical L o domain-forming lipids. Prior electrical current recordings of POPC-OOH containing membranes by Corvalán et al 36 also indirectly suggested that lipid peroxides could cluster together, leading to the formation of ion lipid conductive pores. Altogether, these findings indicate that the presence of lipid peroxidation products can promote the appearance of lipid clusters of higher local order, which can play a crucial role in signal transduction and mechanical behavior of the cell’s membrane.…”

Section: Resultsmentioning

confidence: 96%

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Directly imaging emergence of phase separation in peroxidized lipid membranes

et al. 2023

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Lipid peroxidation is a process which is key in cell signaling and disease, it is exploited in cancer therapy in the form of photodynamic therapy. The appearance of hydrophilic moieties within the bilayer’s hydrocarbon core will dramatically alter the structure and mechanical behavior of membranes. Here, we combine viscosity sensitive fluorophores, advanced microscopy, and X-ray diffraction and molecular simulations to directly and quantitatively measure the bilayer’s structural and viscoelastic properties, and correlate these with atomistic molecular modelling. Our results indicate an increase in microviscosity and a decrease in the bending rigidity upon peroxidation of the membranes, contrary to the trend observed with non-oxidized lipids. Fluorescence lifetime imaging microscopy and MD simulations give evidence for the presence of membrane regions of different local order in the oxidized membranes. We hypothesize that oxidation promotes stronger lipid-lipid interactions, which lead to an increase in the lateral heterogeneity within the bilayer and the creation of lipid clusters of higher order.

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Section: Resultssupporting

confidence: 93%

Section: Resultsmentioning

confidence: 96%

Directly imaging emergence of phase separation in peroxidized lipid membranes

et al. 2023

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“…To reiterate, we think that the different magnitude (∼1000-fold) between the optical g -factors and the photochemical responses in our experiments may be the result of photochemical amplification through the steady-state generation of ROS, leading to the enrichment of an intrinsically small stereochemical bias (in this case, the relatively small chiroptical activities of our photocatalysts). In parallel to this, enantioselective amplification and autocatalytic effects are well documented in the literature, being particularly relevant in biological homochirality. − Therefore, the role played by the autocatalytic generation of ROS as one more factor behind the photochemical bias cannot be discarded under the experimental conditions presented herein and should be investigated further. − Importantly, the polarization-dependent photochemical output is observed consistently by us in a complete set of experiments, for the L-SiO 2 @Au@TiO 2 and R-SiO 2 @Au@TiO 2 nanoribbons and the experiment with alternating polarizers (Figure e).…”

Section: Resultsmentioning

confidence: 52%

Chiral Generation of Hot Carriers for Polarization-Sensitive Plasmonic Photocatalysis

et al. 2022

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Mastering the manipulation of chirality at the nanoscale has long been a priority for chemists, physicists, and materials scientists, given its importance in the biochemical processes of the natural world and in the development of novel technologies. In this vein, the formation of novel metamaterials and sensing platforms resulting from the synergic combination of chirality and plasmonics has opened new avenues in nano-optics. Recently, the implementation of chiral plasmonic nanostructures in photocatalysis has been proposed theoretically as a means to drive polarization-dependent photochemistry. In the present work, we demonstrate that the use of inorganic nanometric chiral templates for the controlled assembly of Au and TiO 2 nanoparticles leads to the formation of plasmon-based photocatalysts with polarization-dependent reactivity. The formation of plasmonic assemblies with chiroptical activities induces the asymmetric formation of hot electrons and holes generated via electromagnetic excitation, opening the door to novel photocatalytic and optoelectronic features. More precisely, we demonstrate that the reaction yield can be improved when the helicity of the circularly polarized light used to activate the plasmonic component matches the handedness of the chiral substrate. Our approach may enable new applications in the fields of chirality and photocatalysis, particularly toward plasmon-induced chiral photochemistry.

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“…In particular, previous micropipette experiments on POPC-OOH giant unilamellar vesicles (GUVs) determined an increase of 15% in the area excess in respect to non-oxidized 1-palmitoyl-2-oleoyl- sn -glycero-3-phosphocholine (POPC) membranes . This effect was later confirmed by small-angle X-ray scattering (SAXS) data analysis and found to be accompanied by membrane thickness reduction. , Interestingly, accumulation of POPC-OOH in the membrane does not change its permeability, although the hydroperoxidized lipid bilayer becomes more susceptible to electroporation. − Further, liquid disordered (Ld)/liquid ordered (Lo) phase separation has also been observed in a 1,2-dipalmitoyl- sn -glycero-3-phosphocholine (DPPC)/POPC-OOH/cholesterol system, showing that POPC-OOH can modulate lipid domains …”

Section: Introductionmentioning

confidence: 89%

Lipid Hydroperoxide Compromises the Membrane Structure Organization and Softens Bending Rigidity

et al. 2021

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Lipid hydroperoxides are key mediators of diseases and cell death. In this work, the structural and dynamic perturbations induced by the hydroperoxidized POPC lipid (POPC-OOH) in fluid POPC membranes, at both 23 and 37 °C, were addressed using advanced small-angle X-ray scattering (SAXS) and fluorescence methodologies. Notably, SAXS reveals that the hydroperoxide group decreases the lipid bilayer bending rigidity. This alteration disfavors the bilayer stacking and increases the swelling in-between stacked bilayers. We further investigated the changes in the apolar/polar interface of hydroperoxide-containing membranes through time-resolved fluorescence/anisotropy experiments of the probe TMA-DPH and time-dependent fluorescence shifts of Laurdan. A shorter mean fluorescence lifetime for TMA-DPH was obtained in enriched POPC-OOH membranes, revealing a higher degree of hydration near the membrane interface. Moreover, a higher microviscosity near TMA-DPH and lower order are predicted for these oxidized membranes, at variance with the usual trend of variation of these two parameters. Finally, the complex relaxation process of Laurdan in pure POPC-OOH membranes also indicates a higher membrane hydration and viscosity in the close vicinity of the −OOH moiety. Altogether, our combined approach reveals that the hydroperoxide group promotes alterations in the membrane structure organization, namely, at the level of membrane order, viscosity, and bending rigidity.

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Lipid Hydroperoxidation Effect on the Dynamical Evolution of the Conductance Process in Bilayer Lipid Membranes: A Condition Toward Criticality

Cited by 10 publications

References 69 publications

Directly imaging emergence of phase separation in peroxidized lipid membranes

Directly imaging emergence of phase separation in peroxidized lipid membranes

Chiral Generation of Hot Carriers for Polarization-Sensitive Plasmonic Photocatalysis

Lipid Hydroperoxide Compromises the Membrane Structure Organization and Softens Bending Rigidity

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