Vibrational studies of saccharide-induced lipid film reorganization at aqueous/air interfaces

Link, Katie A.; Hsieh, Chia‐Yun; Tuladhar, Aashish; Chase, Zizwe A.; Wang, Zheming; Wang, Hongfei; Walker, Robert A.

doi:10.1016/j.chemphys.2018.02.011

Cited by 18 publications

(34 citation statements)

References 46 publications

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“…8,9 It is thought that soluble saccharides co-adsorb to insoluble organic films at the SSML and transfer into SSA via bubble bursting at the ocean surface. [10][11][12][13][14] Chemical composition is a significant driver of SSA particle radiative properties, so climate models require predictive representations of marine aerosol composition to accurately model climate processes in the marine boundary layer. 10,[15][16][17][18] SSA containing polysaccharides, especially polysaccharides within marine microgels, comprise a significant fraction of cloud condensation nuclei (CCN) [19][20][21][22] and ice nucleating particles (INPs), [23][24][25][26][27][28][29][30] thereby affecting cloud formation and albedo.…”

Section: Introductionmentioning

confidence: 99%

“…[59][60][61][62] Cooperative adsorption (coadsorption) to insoluble lipid monolayers has been indirectly observed for other saccharides and polysaccharides as well. 10,11,13,63 Electrostatic interactions between charged saccharides and either charged or zwitterionic lipid headgroups have been the predominant mechanism of co-adsorption proposed. For example, the cationic polysaccharide chitosan primarily interacts with negatively charged and zwitterionic phospholipids through electrostatic interactions between the chitosan ammonium and phospholipid phosphate moieties.…”

Section: Introductionmentioning

confidence: 99%

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Calcium bridging drives polysaccharide co-adsorption to a proxy sea surface microlayer

Carter-Fenk

Dommer²,

Fiamingo

et al. 2021

Phys. Chem. Chem. Phys.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Calcium bridging drives polysaccharide co-adsorption to a proxy sea surface microlayer

Carter-Fenk

Dommer²,

Fiamingo

et al. 2021

Phys. Chem. Chem. Phys.

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“…The high sensitivity of the 100-kHz VSFG spectroscopy makes the study of molecular structural changes in, e.g. , proteoglycans accessible upon their interaction with other molecules or saccharides with lipids [ 47 ].…”

Section: Emerging Bioanalytical Tools For the Characterization Of Gag-lipid Interactionsmentioning

confidence: 99%

Analytical challenges of glycosaminoglycans at biological interfaces

2021

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The analysis of glycosaminoglycans (GAGs) is a challenging task due to their high structural heterogeneity, which results in diverse GAG chains with similar chemical properties. Simultaneously, it is of high importance to understand their role and behavior in biological systems. It has been known for decades now that GAGs can interact with lipid molecules and thus contribute to the onset of atherosclerosis, but their interactions at and with biological interfaces, such as the cell membrane, are yet to be revealed. Here, analytical approaches that could yield important knowledge on the GAG-cell membrane interactions as well as the synthetic and analytical advances that make their study possible are discussed. Due to recent developments in laser technology, we particularly focus on nonlinear spectroscopic methods, especially vibrational sum-frequency generation spectroscopy, which has the potential to unravel the structural complexity of heterogeneous biological interfaces in contact with GAGs, in situ and in real time. Graphical abstract

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Section: Introductionmentioning

confidence: 99%

Calcium Bridging Drives Polysaccharide Co-Adsorption to a Proxy Sea Surface Microlayer

Carter-Fenk¹,

Dommer²,

Fiamingo³

et al. 2021

Preprint

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Saccharides comprise a significant mass fraction of organic carbon in sea spray aerosol (SSA), but the mechanisms through which saccharides are transferred from seawater to the ocean surface and eventually into SSA are unclear. It is hypothesized that saccharides cooperatively adsorb to other insoluble organic matter at the air/sea interface, known as the sea surface microlayer (SSML). Using a combination of surface-sensitive infrared reflection-absorption spectroscopy and all-atom molecular dynamics simulations, we demonstrate that the marine-relevant, anionic polysaccharide alginate co-adsorbs to an insoluble palmitic acid monolayer via divalent cationic bridging interactions. Ca2+ induces the greatest extent of alginate co-adsorption to the monolayer, evidenced by the ~30% increase in surface coverage, whereas Mg2+ only facilitates one-third the extent of co-adsorption at seawater-relevant cation concentrations due to its strong hydration propensity. Na+ cations alone do not facilitate alginate co-adsorption, and palmitic acid protonation hinders the formation of divalent cationic bridges between the palmitate and alginate carboxylate moieties. Alginate co-adsorption is largely confined to the interfacial region beneath the monolayer headgroups, so surface pressure, and thus monolayer surface coverage, only changes the amount of alginate co-adsorption by less than 5%. Our results provide physical and molecular characterization of a potentially significant polysaccharide enrichment mechanism within the SSML.

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Vibrational studies of saccharide-induced lipid film reorganization at aqueous/air interfaces

Cited by 18 publications

References 46 publications

Calcium bridging drives polysaccharide co-adsorption to a proxy sea surface microlayer

Calcium bridging drives polysaccharide co-adsorption to a proxy sea surface microlayer

Analytical challenges of glycosaminoglycans at biological interfaces

Calcium Bridging Drives Polysaccharide Co-Adsorption to a Proxy Sea Surface Microlayer

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