Dataset Information

Direct visualization of cooperative adsorption of a string-like molecule onto a solid.

ABSTRACT: Natural systems, composite materials, and thin-film devices adsorb macromolecules in different phases onto their surfaces. In general, polymer chains form interfacial layers where their aggregation states and thermal molecular motions differ from the bulk. Here, we visualize well-defined double-stranded DNAs (dsDNAs) using atomic force microscopy and molecular dynamics simulations to clarify the adsorption mechanism of polymer chains onto solid surfaces. Initially, short and long dsDNAs are individually and cooperatively adsorbed, respectively. Cooperative adsorption involves intertwining of multiple chains. The dependence of adsorption on the chain affects the formation of the interfacial layer, realizing different mechanical properties of DNA/filler bulk composites. These findings will contribute to the development of light and durable polymer composites and films for various industrial, biomedical, and environmental applications.

SUBMITTER: Morimitsu Y

PROVIDER: S-EPMC9555780 | biostudies-literature | 2022 Oct

REPOSITORIES: biostudies-literature

ACCESS DATA

Publications

Direct visualization of cooperative adsorption of a string-like molecule onto a solid.

Morimitsu Yuma Y Matsuno Hisao H Oda Yukari Y Yamamoto Satoru S Tanaka Keiji K

Science advances 20221012 41

Natural systems, composite materials, and thin-film devices adsorb macromolecules in different phases onto their surfaces. In general, polymer chains form interfacial layers where their aggregation states and thermal molecular motions differ from the bulk. Here, we visualize well-defined double-stranded DNAs (dsDNAs) using atomic force microscopy and molecular dynamics simulations to clarify the adsorption mechanism of polymer chains onto solid surfaces. Initially, short and long dsDNAs are indi ...[more]

PMID: 36223469

Similar Datasets

Project description:Despite the fundamental nature and practical importance of melting, there is still no generally accepted theory of this ubiquitous phenomenon. Even the earliest simulations of melting of hard discs by Alder and Wainwright indicated the active role of collective atomic motion in melting and here we utilize molecular dynamics simulation to determine whether these correlated motions are similar to those found in recent studies of glass-forming (GF) liquids and other condensed, strongly interacting, particle systems. We indeed find string-like collective atomic motion in our simulations of "superheated" Ni crystals, but other observations indicate significant differences from GF liquids. For example, we observe neither stretched exponential structural relaxation, nor any decoupling phenomenon, while we do find a boson peak, findings that have strong implications for understanding the physical origin of these universal properties of GF liquids. Our simulations also provide a novel view of "homogeneous" melting in which a small concentration of interstitial defects exerts a powerful effect on the crystal stability through their initiation and propagation of collective atomic motion. These relatively rare point defects are found to propagate down the strings like solitons, driving the collective motion. Crystal integrity remains preserved when the permutational atomic motions take the form of ring-like atomic exchanges, but a topological transition occurs at higher temperatures where the rings open to form linear chains similar in geometrical form and length distribution to the strings of GF liquids. The local symmetry breaking effect of the open strings apparently destabilizes the local lattice structure and precipitates crystal melting. The crystal defects are thus not static entities under dynamic conditions, such as elevated temperatures or material loading, but rather are active agents exhibiting a rich nonlinear dynamics that is not addressed in conventional "static" defect melting models.

Project description:The adsorption of thallium (Tl) onto phyllosilicate minerals plays a critical role in the retention of Tl in soils and sediments and the potential transfer of Tl into plants and groundwater. Especially micaceous minerals are thought to strongly bind monovalent Tl(I), in analogy to their strong binding of Cs. To advance the understanding of Tl(I) adsorption onto phyllosilicate minerals, we studied the adsorption of Tl(I) onto Na- and K-saturated illite and Na-saturated smectite, two muscovites, two vermiculites and a naturally Tl-enriched soil clay mineral fraction. Macroscopic adsorption isotherms were combined with the characterization of the adsorbed Tl by X-ray absorption spectroscopy (XAS). In combination, the results suggest that the adsorption of Tl(I) onto phyllosilicate minerals can be interpreted in terms of three major uptake paths: (i) highest-affinity inner-sphere adsorption of dehydrated Tl+ on a very low number of adsorption sites at the wedge of frayed particle edges of illite and around collapsed zones in vermiculite interlayers through complexation between two siloxane cavities, (ii) intermediate-affinity inner-sphere adsorption of partially dehydrated Tl+ on the planar surfaces of illite and muscovite through complexation onto siloxane cavities, (iii) low-affinity adsorption of hydrated Tl+, especially in the hydrated interlayers of smectite and expanded vermiculite. At the frayed edges of illite particles and in the vermiculite interlayer, Tl uptake can lead to the formation of new wedge sites that enable further adsorption of dehydrated Tl+. On the soil clay fraction, a shift in Tl(I) uptake from frayed edge sites (on illite) to planar sites (on illite and muscovite) was observed with increasing Tl(I) loading. The results from this study show that the adsorption of Tl(I) onto phyllosilicate minerals follows the same trends as reported for Cs and Rb and thus suggests that concepts to describe the retention of (radio)cesium by different types of phyllosilicate minerals in soils, sediments and rocks are also applicable to Tl(I).

Dataset Information

Direct visualization of cooperative adsorption of a string-like molecule onto a solid.

Publications

Direct visualization of cooperative adsorption of a string-like molecule onto a solid.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets