Browse
Submit Data
Databases
API
Help

Dataset Information

28 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

From Crystalline to Amorphous Germania Bilayer Films at the Atomic Scale: Preparation and Characterization.

ABSTRACT: A new two-dimensional (2D) germanium dioxide film has been prepared. The film consists of interconnected germania tetrahedral units forming a bilayer structure, weakly coupled to the supporting Pt(111) metal-substrate. Density functional theory calculations predict a stable structure of 558-membered rings for germania films, while for silica films 6-membered rings are preferred. By varying the preparation conditions the degree of order in the germania films is tuned. Crystalline, intermediate ordered and purely amorphous film structures are resolved by analysing scanning tunnelling microscopy images.

SUBMITTER: Lewandowski AL

PROVIDER: S-EPMC6771709 | biostudies-literature | 2019 Aug

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Publications

From Crystalline to Amorphous Germania Bilayer Films at the Atomic Scale: Preparation and Characterization.

Lewandowski Adrián L AL Tosoni Sergio S Gura Leonard L Schlexer Philomena P Marschalik Patrik P Schneider Wolf-Dieter WD Heyde Markus M Pacchioni Gianfranco G Freund Hans-Joachim HJ

Angewandte Chemie (International ed. in English) 20190701 32

A new two-dimensional (2D) germanium dioxide film has been prepared. The film consists of interconnected germania tetrahedral units forming a bilayer structure, weakly coupled to the supporting Pt(111) metal-substrate. Density functional theory calculations predict a stable structure of 558-membered rings for germania films, while for silica films 6-membered rings are preferred. By varying the preparation conditions the degree of order in the germania films is tuned. Crystalline, intermediate or ...[more]

PMID: 31050096

Similar Datasets

Atomic-scale study of the amorphous-to-crystalline phase transition mechanism in GeTe thin films.

Project description:The underlying mechanism driving the structural amorphous-to-crystalline transition in Group VI chalcogenides is still a matter of debate even in the simplest GeTe system. We exploit the extreme sensitivity of 57Fe emission Mössbauer spectroscopy, following dilute implantation of 57Mn (T½ = 1.5 min) at ISOLDE/CERN, to study the electronic charge distribution in the immediate vicinity of the 57Fe probe substituting Ge (FeGe), and to interrogate the local environment of FeGe over the amorphous-crystalline phase transition in GeTe thin films. Our results show that the local structure of as-sputtered amorphous GeTe is a combination of tetrahedral and defect-octahedral sites. The main effect of the crystallization is the conversion from tetrahedral to defect-free octahedral sites. We discover that only the tetrahedral fraction in amorphous GeTe participates to the change of the FeGe-Te chemical bonds, with a net electronic charge density transfer of ~ 1.6 e/a0 between FeGe and neighboring Te atoms. This charge transfer accounts for a lowering of the covalent character during crystallization. The results are corroborated by theoretical calculations within the framework of density functional theory. The observed atomic-scale chemical-structural changes are directly connected to the macroscopic phase transition and resistivity switch of GeTe thin films.

| S-EPMC5558007 | biostudies-literature

Atomic-scale insights into the interfacial instability of superlubricity in hydrogenated amorphous carbon films.

Project description:The origin of instability or even disappearance of the superlubricity state in hydrogenated amorphous carbon (a-C:H) film in the presence of oxygen or water molecules is still controversial. Here, we address this puzzle regarding the tribochemical activities of sliding interfaces at the nanoscale. The results reveal that gaseous oxygen molecules disable the antifriction capacity of a-C:H by surface dehydrogenation of tribo-affected hydrocarbon bonds. In comparison, oxygen incorporation into the hydrocarbon matrix induces the formation of a low-density surface shear band, owing to which the friction state depends on the oxygen content. High friction of a-C:H film in humid environment originates from the "tumor-like" heterogeneous structures as formed in the highly oxidized tribolayer. Notably, an appropriate doping of silicon can completely shield the moisture effect by forming a silica-like tribolayer. These outcomes shed substantial lights upon the roadmap for achieving robust superlubricity of carbon films in a wide range of environments.

| S-EPMC7101219 | biostudies-literature

Atomic-scale disproportionation in amorphous silicon monoxide.

Project description:Solid silicon monoxide is an amorphous material which has been commercialized for many functional applications. However, the amorphous structure of silicon monoxide is a long-standing question because of the uncommon valence state of silicon in the oxide. It has been deduced that amorphous silicon monoxide undergoes an unusual disproportionation by forming silicon- and silicon-dioxide-like regions. Nevertheless, the direct experimental observation is still missing. Here we report the amorphous structure characterized by angstrom-beam electron diffraction, supplemented by synchrotron X-ray scattering and computer simulations. In addition to the theoretically predicted amorphous silicon and silicon-dioxide clusters, suboxide-type tetrahedral coordinates are detected by angstrom-beam electron diffraction at silicon/silicon-dioxide interfaces, which provides compelling experimental evidence on the atomic-scale disproportionation of amorphous silicon monoxide. Eventually we develop a heterostructure model of the disproportionated silicon monoxide which well explains the distinctive structure and properties of the amorphous material.

| S-EPMC4869258 | biostudies-literature

Ductile crystalline-amorphous nanolaminates.

Project description:It is known that the room-temperature plastic deformation of bulk metallic glasses is compromised by strain softening and shear localization, resulting in near-zero tensile ductility. The incorporation of metallic glasses into engineering materials, therefore, is often accompanied by complete brittleness or an apparent loss of useful tensile ductility. Here we report the observation of an exceptional tensile ductility in crystalline copper/copper-zirconium glass nanolaminates. These nanocrystalline-amorphous nanolaminates exhibit a high flow stress of 1.09 +/- 0.02 GPa, a nearly elastic-perfectly plastic behavior without necking, and a tensile elongation to failure of 13.8 +/- 1.7%, which is six to eight times higher than that typically observed in conventional crystalline-crystalline nanolaminates (<2%) and most other nanocrystalline materials. Transmission electron microscopy and atomistic simulations demonstrate that shear banding instability no longer afflicts the 5- to 10-nm-thick nanolaminate glassy layers during tensile deformation, which also act as high-capacity sinks for dislocations, enabling absorption of free volume and free energy transported by the dislocations; the amorphous-crystal interfaces exhibit unique inelastic shear (slip) transfer characteristics, fundamentally different from those of grain boundaries. Nanoscale metallic glass layers therefore may offer great benefits in engineering the plasticity of crystalline materials and opening new avenues for improving their strength and ductility.

| S-EPMC1899185 | biostudies-literature

In Situ Observation of Crystalline Silicon Growth from SiO2 at Atomic Scale.

Project description:The growth of crystalline Si (c-Si) via direct electron beam writing shows promise for fabricating Si nanomaterials due to its ultrahigh resolution. However, to increase the writing speed is a major obstacle, due to the lack of systematic experimental explorations of the growth process and mechanisms. This paper reports a systematic experimental investigation of the beam-induced formation of c-Si nanoparticles (NPs) from amorphous SiO2 under a range of doses and temperatures by in situ transmission electron microscopy at the atomic scale. A three-orders-of-magnitude writing speed-up is identified under 80 keV irradiation at 600°C compared with 300 keV irradiation at room temperature. Detailed analysis reveals that the self-organization of c-Si NPs is driven by reduction of c-Si effective free energy under electron irradiation. This study provides new insights into the formation mechanisms of c-Si NPs during direct electron beam writing and suggests methods to improve the writing speed.

| S-EPMC6944520 | biostudies-literature

Atomic-scale viscoplasticity mechanisms revealed in high ductility metallic glass films.

Project description:The fundamental plasticity mechanisms in thin freestanding Zr65Ni35 metallic glass films are investigated in order to unravel the origin of an outstanding strength/ductility balance. The deformation process is homogenous until fracture with no evidence of catastrophic shear banding. The creep/relaxation behaviour of the films was characterized by on-chip tensile testing, revealing an activation volume in the range 100-200?Å3. Advanced high-resolution transmission electron microscopy imaging and spectroscopy exhibit a very fine glassy nanostructure with well-defined dense Ni-rich clusters embedded in Zr-rich clusters of lower atomic density and a ~2-3?nm characteristic length scale. Nanobeam electron diffraction analysis reveals that the accumulation of plastic deformation at room-temperature correlates with monotonously increasing disruption of the local atomic order. These results provide experimental evidences of the dynamics of shear transformation zones activation in metallic glasses. The impact of the nanoscale structural heterogeneities on the mechanical properties including the rate dependent behaviour is discussed, shedding new light on the governing plasticity mechanisms in metallic glasses with initially heterogeneous atomic arrangement.

| S-EPMC6749058 | biostudies-literature

Atomic-scale compositional mapping reveals Mg-rich amorphous calcium phosphate in human dental enamel.

Project description:Human dental enamel, the hardest tissue in the body, plays a vital role in protecting teeth from wear as a result of daily grinding and chewing as well as from chemical attack. It is well established that the mechanical strength and fatigue resistance of dental enamel are derived from its hierarchical structure, which consists of periodically arranged bundles of hydroxyapatite (HAP) nanowires. However, we do not yet have a full understanding of the in vivo HAP crystallization process that leads to this structure. Mg(2+) ions, which are present in many biological systems, regulate HAP crystallization by stabilizing its precursor, amorphous calcium phosphate (ACP), but their atomic-scale distribution within HAP is unknown. We use atom probe tomography to provide the first direct observations of an intergranular Mg-rich ACP phase between the HAP nanowires in mature human dental enamel. We also observe Mg-rich elongated precipitates and pockets of organic material among the HAP nanowires. These observations support the postclassical theory of amelogenesis (that is, enamel formation) and suggest that decay occurs via dissolution of the intergranular phase. This information is also useful for the development of more accurate models to describe the mechanical behavior of teeth.

| S-EPMC5014466 | biostudies-literature

Preparation and Characterization of PHBV/PCL-Diol Blend Films.

Project description:Biodegradable thin films based on poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) and poly(caprolactone diol) (PCL-diol) blend were developed using the solution casting method. PHBV is biodegradable, biocompatible, and produced naturally by bacterial activity, but its use is restricted by high crystallinity and low resistance to thermal degradation with melting temperatures close to degradation thus narrowing the processing window. Solution casting was chosen as a cost-effective method reducing energy consumption and avoiding thermal degradation during processing. The increase in PCL-diol in blend composition (40-60 wt%) enhances the film-forming ability of PHBV and the wettability along with the decrease in the roughness of the resulting materials as revealed by contact angle measurements, scanning electron microscopy (SEM), and atomic force microscopy (AFM). Optimal composition in terms of filmogenity and surface structure has been achieved by the addition of PCL-diol in the amount of 60 wt%. FTIR confirmed the expected chemical structures with no evidence of chemical interactions between the two polymers.

| S-EPMC10747782 | biostudies-literature

Preparation and Characterization of Amorphous Solid Dispersions for the Solubilization of Fenretinide.

Project description:Fenretinide (4-HPR), a retinoid derivative, has shown high antitumor activity, a low toxicological profile, and no induction of resistance. Despite these favorable features, the variability in oral absorption due to its low solubility combined with the high hepatic first pass effect strongly reduce clinical outcomes. To overcome the solubility and dissolution challenges of poorly water-soluble 4-HPR, we prepared a solid dispersion of the drug (4-HPR-P5) using a hydrophilic copolymer (P5) previously synthesized by our team as the solubilizing agent. The molecularly dispersed drug was obtained by antisolvent co-precipitation, an easy and up-scalable technique. A higher drug apparent solubility (1134-fold increase) and a markedly faster dissolution were obtained. In water, the colloidal dispersion showed a mean hydrodynamic diameter of 249 nm and positive zeta potential (+41.3 mV), confirming the suitability of the formulation for intravenous administration. The solid nanoparticles were also characterized by a high drug payload (37%), as was also evidenced by a chemometric-assisted Fourier transform infrared spectroscopy (FTIR) investigation. The 4-HPR-P5 exhibited antiproliferative activity, with IC50 values of 1.25 and 1.93 µM on IMR-32 and SH-SY5Y neuroblastoma cells, respectively. Our data confirmed that the 4-HPR-P5 formulation developed herein was able to increase drug apparent aqueous solubility and provide an extended release over time, thus suggesting that it represents an efficient approach to improve 4-HPR bioavailability.

| S-EPMC10052200 | biostudies-literature