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Crystallisation of water in a series of precious opal samples with opal-A and opal-CT morphologies has been characterised using low-temperature differential scanning calorimetry (DSC) and temperature-dependent terahertz/far-infrared (THz/Far-IR) spectroscopy. The melting temperature for the crystallisable water in the opals was observed to be depressed reflecting a microporous environment and was found to be consistent for both DSC and THz spectroscopy. Based on melt temperature depression, the size range of the pores for the opal-CT was estimated to be in the range 3–6 nm while for opal-A the range was 4 to >50 nm, indicating differing microstructures between opal-A and -CT. The THz/Far-IR spectroscopy indicated the presence of both crystalline and amorphous ice on solidification of the water, although phase identification of the crystalline ice was not possible. Notably, to the authors knowledge, this paper represents the first use of THz/Far-IR spectroscopy in the temperature-dependent characterisation of water and ice encapsulated in micropores.

In 2016, an extensive fossil forest was discovered near Meshgin Shahr, northwest Iran. Silicified tree trunks occur in Miocene fluvial sediments and at multiple stratigraphic levels within a 27-m thick sequence of Pleistocene volcaniclastics. The Miocene trunks likely represent stream transport. Pleistocene examples originated during repeated eruptive events when volcaniclastic sediments buried a standing forest. The site, informally named Meshgin Shahr Fossil Forest, was registered in 2017 as a national natural monument by the Iranian Cultural, Handicraft and Tourism Organization. To date, 16 fossilized trunks have been found, all but one of them representing gymnosperms. The ancient coniferous forest was very different from modern forests in Iran and adjacent Azerbaijan, a result of climatic changes that were principally caused by the demise of the Paratethys Sea and by rain shadow effects caused by the uplift of the Alborz and Zagros mountain ranges. X-ray diffraction patterns reveal that woods from the fossil forest contain three types of silica: opal-CT, pure quartz, and a mixture of opal-CT and quartz. In addition, optical photomicrographs show the abundant presence of amorphous opal-A. Mineralogic variations occur among different fossil trees and within a single trunk. These silica polymorphs resulted from a combination of processes: silica minerals precipitated in multiple episodes under differing geochemical conditions and the diagenetic transformation of an opaline parent material.

Whereas considerable interest exists in self-assembly of well-ordered, porous \"inverse opal\" structures for optical, electronic, and (bio)chemical applications, uncontrolled defect formation has limited the scale-up and practicality of such approaches. Here we demonstrate a new method for assembling highly ordered, crack-free inverse opal films over a centimeter scale. Multilayered composite colloidal crystal films have been generated via evaporative deposition of polymeric colloidal spheres suspended within a hydrolyzed silicate sol-gel precursor solution. The coassembly of a sacrificial colloidal template with a matrix material avoids the need for liquid infiltration into the preassembled colloidal crystal and minimizes the associated cracking and inhomogeneities of the resulting inverse opal films. We discuss the underlying mechanisms that may account for the formation of large-area defect-free films, their unique preferential growth along the 〈110〉 direction and unusual fracture behavior. We demonstrate that this coassembly approach allows the fabrication of hierarchical structures not achievable by conventional methods, such as multilayered films and deposition onto patterned or curved surfaces. These robust SiO₂ inverse opals can be transformed into various materials that retain the morphology and order of the original films, as exemplified by the reactive conversion into Si or TiO₂ replicas. We show that colloidal coassembly is available for a range of organometallic sol-gel and polymer matrix precursors, and represents a simple, low-cost, scalable method for generating high-quality, chemically tailorable inverse opal films for a variety of applications.

Natural opal is a widespread mineral formed by the aqueous alteration of silicate rocks. It occurs as a mixture of silica nano-to-micro-structures (e.g., nanograins, spheres) and silica hydrogel cement, with variations in the proportions of these components leading to significant differences in the physico-chemical properties of opals. However, the detailed process of their formation in nature and the influence of the mixing ratio are not fully understood, as opal has not been yet synthesized under geologically relevant conditions. This study aims to develop a method of opal synthesis in conditions close to continental weathering conditions (<50 °C, ambient pressure) using relevant chemicals that could be employed to gain insight into the processes that give rise to opal on Earth and Mars. Our synthesis method enabled us to synthesize opal-A with different mixing ratios, of which four were then studied to determine the effect on the material’s properties. Changes in the proportion of the hydrogel cement affect the porosity and the total water content, as well as the proportion of “water” species (H2O and OH). Moreover, the synthetic opal obtained with a 1:1 ratio shows the closest similarity to natural opal-AG. Finally, our results support the hypothesized multistage process for opal formation in nature.

Here, we present a physiologically relevant model of the human pulmonary alveoli. This alveolar lung-on-a-chip platform is composed of a three-dimensional porous hydrogel made of gelatin methacryloyl with an inverse opal structure, bonded to a compartmentalized polydimethylsiloxane chip. The inverse opal hydrogel structure features well-defined, interconnected pores with high similarity to human alveolar sacs. By populating the sacs with primary human alveolar epithelial cells, functional epithelial monolayers are readily formed. Cyclic strain is integrated into the device to allow biomimetic breathing events of the alveolar lung, which, in addition, makes it possible to investigate pathological effects such as those incurred by cigarette smoking and severe acute respiratory syndrome coronavirus 2 pseudoviral infection. Our study demonstrates a unique method for reconstitution of the functional human pulmonary alveoli in vitro, which is anticipated to pave the way for investigating relevant physiological and pathological events in the human distal lung.

Biologically inspired self-healing structural color hydrogels were developed by adding a glucose oxidase (GOX)- and catalase (CAT)-filled glutaraldehyde cross-linked BSA hydrogel into methacrylated gelatin (GelMA) inverse opal scaffolds. The composite hydrogel materials with the polymerized GelMA scaffold could maintain the stability of an inverse opal structure and its resultant structural colors, whereas the protein hydrogel filler could impart self-healing capability through the reversible covalent attachment of glutaraldehyde to lysine residues of BSA and enzyme additives. A series of unprecedented structural color materials could be created by assembling and healing the elements of the composite hydrogel. In addition, as both the GelMA and the protein hydrogels were derived from organisms, the composite materials presented high biocompatibility and plasticity. These features of self-healing structural color hydrogels make them excellent functional materials for different applications.

Silicified wood occurs abundantly in Middle Miocene flows and sedimentary interbeds of the Columbia River Basalt Group (CRBG) in central Washington State, USA. These fossil localities are well-dated based on radiometric ages determined for the host lava. Paleoenvironments include wood transported by lahars (Ginkgo Petrified Forest State Park), fluvial and palludal environments (Saddle Mountain and Yakima Canyon fossil localities), and standing forests engulfed by advancing lava (Yakima Ridge fossil forest). At all of these localities, the mineralogy of fossil wood is diverse, with silica minerals that include opal-A, opal-CT, chalcedony, and macrocrystalline quartz. Some specimens are composed of only a single form of silica; more commonly, specimens contain multiple phases. Opal-A and Opal-CT often coexist. Some woods are mineralized only with chalcedony; however, chalcedony and macrocrystalline quartz are common as minor constituents in opal wood. In these specimens, crystalline silica filling fractures, rot pockets, and cell lumen may occur. These occurrences are evidence that silicification occurred as a sequential process, where changes in the geochemical environment or anatomical structures affected the precipitation of silica. Fossilization typically began with precipitation of amorphous silica within cell walls, leaving cell lumen and conductive vessels open. Diagenetic transformation of opal-A to opal-CT in fossil wood has long been a widely accepted hypothesis; however, in opaline CRBG specimens, the two silica polymorphs usually appear to have formed independently, e.g., woods in which cell walls are mineralized with opal-A but in which lumen contain opal-CT. Similarly, opal-CT has been inferred to sometimes transform to chalcedony; however, in CRBG, these mixed assemblages commonly resulted from multiple mineralization episodes.

Sediment cores recently collected from the Chilean Margin during D/V JOIDES Resolution Expedition 379T (JR100) document variability in shipboard-generated records of the green/blue (G/B) ratio. These changes show a strong coherence with benthic foraminiferal δ18O, Antarctic ice core records, and sediment lithology (e.g., higher diatom abundances in greener sediment intervals), suggesting a climate-related control on the G/B. Here, we test the utility of G/B as a proxy for diatom productivity at Sites J1002 and J1007 by calibrating G/B to measured biogenic opal. Strong exponential correlations between measured opal% and the G/B were found at both sites. We use the empirical regressions to generate high-resolution records of opal contents (opal%) on the Chilean Margin. Higher productivity tends to result in more reducing sedimentary conditions. Redox-sensitive sedimentary U/Th generally co-varies with the reconstructed opal% at both sites, supporting the association between sediment color, sedimentary U/Th, and productivity. Lastly, we calculated opal mass accumulation rate (MAR) at Site J1007 over the last ∼150,000 years. The G/B-derived opal MAR record from Site J1007 largely tracks existing records derived from traditional wet-alkaline digestion from the south and eastern equatorial Pacific (EEP) Ocean, with a common opal flux peak at ∼50 ka suggesting that increased diatom productivity in the EEP was likely driven by enhanced nutrient supply from the Southern Ocean rather than dust inputs as previously suggested. Collectively, our results identify the G/B ratio as a useful tool with the potential to generate reliable, high-resolution paleoceanographic records that circumvent the traditionally laborious methodology.

A decrease in atmospheric CO 2 partial pressure ( p CO 2 ) is considered an important prerequisite for the onset and intensification of Northern Hemisphere Glaciation (NHG). However, how the ocean sequestered missing CO 2 during the NHG is still uncertain. Changes in surface productivity and deep ventilation in the Southern Ocean (SO) have been proposed to explain the variations in atmospheric p CO 2 over the last eight glacial cycles, but it is unclear whether these mechanisms contributed to the decrease in atmospheric p CO 2 during the NHG. Using titanium-normalized contents and mass accumulation rates of biogenic opal and total organic carbon from the International Ocean Discovery Program (IODP) Expedition 374 Site U1524A, we reconstruct the productivity in the Ross Sea, Antarctica, from 3.3 Ma to 2.4 Ma. The productivity records exhibit a long-term decreasing trend and several distinct phased evolutionary features. Specifically, the local productivity fluctuated dramatically during 3.3–3.0 Ma, decreased gradually during 3.0–2.6 Ma, and remained relatively constant during 2.6–2.4 Ma. By comparing productivity with its potential influences, we infer that the phased and long-term evolutions of productivity were mainly controlled by changes in deep ocean ventilation. Sea ice expansion might have decreased productivity during 3.3–3.0 Ma by light attenuation. Changes in eolian dust input have little effect on productivity. Further analysis revealed no coupling linkage between productivity and atmospheric p CO 2 , indicating that the productivity in the SO Antarctic Zone (AZ) was not the main factor controlling the atmospheric CO 2 decrease during the NHG. To improve our understanding of the role of SO processes in the NHG, further studies should focus on the potential influences of deep ocean ventilation on atmospheric p CO 2 in the AZ, and similar studies should also be extended to the sea area in the Subantarctic Zone.

For many decades, wood silicification has been viewed as a relatively simple process of permineralization that occurs when silica dissolved in groundwater precipitates to fill vacant spaces within the porous tissue. The presence of specific silica minerals is commonly ascribed to diagenetic changes. The possibility of rapid silicification is inferred from evidence from modern hot springs. Extensive examination of silicified wood from worldwide localities spanning long geologic time suggests that these generalizations are not dependable. Instead, wood silicification may occur via multiple pathways, permineralization being relatively rare. Mineralization commonly involves silica precipitation in successive episodes, where changes in the geochemical environment cause various polymorphs to coexist in a single specimen. Diagenetic changes may later change the mineral composition, but for many specimens diagenesis is not the dominant process that controls mineral distribution. Rates of silicification are primarily related to dissolved silica levels and permeability of sediment that encloses buried wood. Rapid silica deposition takes place on wood in modern hot springs, but these occurrences have dissimilar physical and chemical conditions compared to those that exist in most geologic environments. The times required for silicification are variable, and cannot be described by any generalization.