Ion Depletion in the Interfacial Microenvironment from Cell–Surface Interactions

Jarisz, Tasha A.; Hennecker, Christopher; Hore, Dennis K.

doi:10.1021/jacs.2c05340

Cited by 3 publications

(3 citation statements)

References 54 publications

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“…Sum frequency generation (SFG) spectroscopy is now an indispensable tool for probing soft interfaces such as gas/liquid, liquid/liquid, and solid/liquid interfaces. The water surface (i.e., water/vapor interface) is still one of the most important interfaces in the realm of SFG spectroscopy, because it has been benchmarking the experimental and theoretical SFG techniques since their infancy as well as because SFG studies of aqueous interfaces still actively provide intriguing novel topics. − One remaining question about SFG spectroscopy of water is that the H/D isotopic dilution dependence of the complex χ (2) (second-order nonlinear optical susceptibility) spectrum of the water surface in the OH-stretch region is not well reproduced by theoretical calculations. Here, the isotopic dilution means the reduction of H 2 O concentration by adding D 2 O.…”

mentioning

confidence: 99%

Experimental and Theoretical Heterodyne-Detected Sum Frequency Generation Spectroscopy of Isotopically Pure and Diluted Water Surfaces

Yamaguchi

Takayama

Otosu

et al. 2022

J. Phys. Chem. Lett.

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The χ (2) (second-order nonlinear optical susceptibility) spectrum of the water surface has been a matter of debate for a few decades. Here, we report that we experimentally measured the isotopic dilution dependence of the χ (2) spectrum and theoretically reproduced it by employing the quantum/classical mixed approach with a new idea to subtract an artifact. The present theoretical framework allows for clarifying the effects of the intramolecular, intermolecular, and Fermi resonance couplings on the OH-stretch vibrational spectra of water at the surface as well as in the bulk.

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confidence: 99%

Experimental and Theoretical Heterodyne-Detected Sum Frequency Generation Spectroscopy of Isotopically Pure and Diluted Water Surfaces

Yamaguchi

Takayama

Otosu

et al. 2022

J. Phys. Chem. Lett.

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“…The increase in entropy between two NPs when they are close together compared to when they are independent is proportional to ln(V − 2V d + V 0 ) − ln(V − 2V d ), which leads to attractive interactions between NPs and is known as the depletion effect. 30 This is a pure entropy-driven effect; under this effect, NPs tend to aggregate. 31,32 NPs within the ordered structure formed by BCPs also experience attractive interactions induced by the block chains.…”

Section: ■ Introductionmentioning

confidence: 99%

“…If the volume of overlap is V 0 , then the volume inaccessible to polymer chains in the entire system decreases by V 0 , and then the increase in the translational entropy of the polymer is proportional to ln( V – 2 V d + V 0 ). The increase in entropy between two NPs when they are close together compared to when they are independent is proportional to ln( V – 2 V d + V 0 ) – ln( V – 2 V d ), which leads to attractive interactions between NPs and is known as the depletion effect . This is a pure entropy-driven effect; under this effect, NPs tend to aggregate. , …”

Section: Introductionmentioning

confidence: 99%

Nonadditive Effective Interactions and Entropy-Driven Non-Close-Packed Self-Assembly Cluster of Nanoparticle in Ordered Block Copolymer Structure

Liu,

Zhang,

Zhao

et al. 2024

Macromolecules

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In general, nanoparticles with additive interactions tend to aggregate into a close-packed cluster, which minimizes surface area. Within the ordered structures formed by block copolymers, the effective interactions between nanoparticles exhibit nonadditive characteristics induced by the depletion effect with the block chains as depletant. Especially when the size of the nanoparticles is comparable to that of the polymer, the structure of the cluster formed by nanoparticles significantly influences the conformation of block chains in the phase domain, and the changes of chain conformation affect the mutual interactions between nanoparticles as well. Driven by these nonadditive attractive interactions, novel self-assembly behaviors of nanoparticles will be observed, which differ from those of nanoparticles with additive interactions. This review employs selfconsistent field theory to quantitatively investigate the additivity of the effective two-body interactions between spherical nanoparticles in lamellar structures formed by block copolymers. The self-assembly behaviors of nanoparticles with these nonadditive attractive interactions are well addressed. It has been observed that the three-dimensional (3D) or two-dimensional (2D) close-packed structure with minimal surface area is stable only when the nanoparticles are relatively small compared to the block chain length. For large-sized nanoparticles, a non-close-packed structure, ring-like cluster, is formed. By comparing the conformational characteristics of polymers in the system with different aggregation structures of nanoparticles, this article reveals the entropy-driven mechanism that the relative sizes of polymers and nanoparticles can be used to tune the competition between the depletion effect and polymer conformational entropy and then regulate the directed self-assembly of nanoparticles (NPs) in block copolymer (BCP) behaviors. When nanoparticles are relatively small, the aggregates have a negligible impact on the polymer conformations. At this stage, the depletion effect dominates the self-assembly of the nanoparticles, and close-packed structures can be obtained. When the size of nanoparticles is comparable to that of the block chains, the competition between the attractive interactions induced by the depletion effect and the conformational entropy loss caused by exclusion due to cluster results in the formation of non-close-packed ring-like clusters. However, when nanoparticles are slightly larger than the block chains, they cause deformation of the interface of the phase domain, and at this point, interfacial tension-induced interactions begin to dominate the assembly of nanoparticles. This novel mechanism can be applied to the directed assembly of nanoparticles in various periodic structures formed by block copolymers and can also be used in the design of novel self-assembly structures for isotropic nanoparticles.

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Algae–water–silica interactions in low and high ionic strength environments

Azam,

Lu,

Rathore

et al. 2023

Journal of Applied Physics

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The interaction between algae and solid surfaces is of direct interest for the optimization of biofuel production technologies. Silica is particularly relevant due the use of solgel matrices for enhanced growth and ease of processing, where ionic strength variation is an important consideration. Here, an inverted fluorescence experiment is used to perform measurements of the distance between a silica surface and algae in solution. At low ionic strength, the average algae–silica distance is approximately 90 nm but increases to roughly 130 nm at 1 M NaCl, contradicting the prediction based on simple electrical double layer interaction models. These findings illustrate the role of biochemical and electrostatic interactions at charged aqueous interfaces of relevance to biofuel production.

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Ion Depletion in the Interfacial Microenvironment from Cell–Surface Interactions

Cited by 3 publications

References 54 publications

Experimental and Theoretical Heterodyne-Detected Sum Frequency Generation Spectroscopy of Isotopically Pure and Diluted Water Surfaces

Experimental and Theoretical Heterodyne-Detected Sum Frequency Generation Spectroscopy of Isotopically Pure and Diluted Water Surfaces

Nonadditive Effective Interactions and Entropy-Driven Non-Close-Packed Self-Assembly Cluster of Nanoparticle in Ordered Block Copolymer Structure

Algae–water–silica interactions in low and high ionic strength environments

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