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At least 73 records · Page 4

Tailoring Nanoporous Silica and Natural Straw Structural Insulation Composites

Nanoporous silica exhibits ultralow thermal conductivity as a result of its nanoscale pore size, high pore volume, and specific surface area. In this study, we report the self-assembled surfactant-templated synthesis of nanoporous silica, which is integrated with cellulose fibers derived from natural straw to manufacture high thermal insulation and mechanically robust nanocomposites. The nanocomposite shows a low thermal conductivity of 22.5 mW/(m·K), a compressive modulus of 0.93 MPa, and a hydrophobicity with a water contact angle of 125°. Moreover, we observed a marked reduction in water absorption capacity and a carbon footprint of 0.21 kg CO 2 equiv/kg. Here, this study provides a pathway toward the development of nanoporous structural insulation materials for energy-efficient building applications.

36 MATERIALS SCIENCE↗

Feasibility of Algal Biochar, a Byproduct of Biofuel Production, as a Supplemental Cementitious Material

Algal biochar, as the solid residue of biofuel production from algal biomass, is reported to explore disposition options, aiming to lessen the liability or obstacles to biofuel production processes. However, landfills and open combustion lead to adverse environmental impacts. One way to add value to such wastes is to use them as admixtures in cementitious construction materials. This study aims to investigate the feasibility of algae-derived biochar as supplementary cementitious materials (SCM) at different water contents and mixture ratios. Algal biochar-cement composites were prepared with different algal biochar content as well as different water-to-cement (w/c) ratios, and the surface area, morphology, elemental, and mineralogical composition were characterized. To compensate for the high-water absorption of algal biochar, a small concentration of a superplasticizer was used since higher w/c ratios negatively impact strength. The mechanical performance of algal biochar-cement composites is compared with control composites using commercial silica fume as a typical commercial SCM. The findings suggest that algal biochar is a promising candidate to replace commercial SCM, like silica fume, since algal biochar-cement composites can reach comparable compressive strength and Young’s modulus to commercial pozzolan-cement materials with the same w/c ratio, though at later curing times, 33 days. Although the tensile strength of algal biochar-cement composites is statistically similar at 7 days, it is significantly lower at later curing times, and further investigation is required to improve this property. Algal biochar-based cement binders showed comparable embodied carbon to silica fume-based cement binders based on a cradle-to-gate lifecycle analysis. However, the ability of algal biochar to absorb large volumes of CO 2 over short periods of time, as measured in this study, makes this novel SCM an excellent alternative to reduce the embodied carbon of concrete structures cradle-to-grave at 1/10 of the cost. In conclusion, valorization of algae-derived solid waste provides great potential to reduce embodied carbon and brings credit to biofuel production and concrete-based construction.

algae-derived↗

Design new epoxy nanocomposite coatings based on metal vanadium oxy-phosphate M 0.5 VOPO 4 for anti-corrosion applications

Epoxy nanocomposite coatings are an essential way to protect petroleum storage tanks from corrosion. For this purpose, the new nanocomposite epoxy coatings (P-M/epoxy composites) have been successfully designed. The P-M/epoxy composites are based on the metal vanadium oxy-phosphate M 0.5 VOPO 4 (where M = Mg, Ni, and Zn). The function of P-M/epoxy composites as anti-corrosion coatings was explored using electrochemical and mechanical tests. Using electrochemical impedance spectroscopy (EIS), it has been noticed that the pore resistance and polarization resistance of the P-M/epoxy composites remain higher as compared to the neat epoxy. The P-M/epoxy composites have the greatest impact on the cathodic dis-bonded area and water absorption. Besides, P-M/epoxy composites exhibit a very high order of mechanical properties. Further, Mg 0.5 VOPO 4 has the greatest effect on the anti-corrosion properties of epoxy coating followed by Zn 0.5 VOPO 4 and Ni 0.5 VOPO 4 . All these properties lead to developing effective anti-corrosion coatings. Thus, the net result from this research work is highly promising and provides a potential for future works on the anti-corrosion coating.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Covalently integrated silica nanoparticles in poly(ethylene glycol)-based acrylate resins: thermomechanical, swelling, and morphological behavior

Nanocomposites integrate functional nanofillers into viscoelastic matrices for electronics, lightweight structural materials, and tissue engineering. Herein, the effect of methacrylate-functionalized (MA-SiO 2 ) and vinyl-functionalized (V-SiO 2 ) silica nanoparticles on the thermal, mechanical, physical, and morphological characteristics of poly(ethylene glycol) (PEG) nanocomposites was investigated. The gel fraction of V-SiO 2 composites decreases upon addition of 3.8 wt% but increases with further addition (>7.4 wt%) until it reaches a plateau at 10.7 wt%. The MA-SiO 2 induced no significant changes in gel fraction and both V-SiO 2 and MA-SiO 2 nanoparticles had a negligible impact on the nanocomposite glass transition temperature and water absorption. The Young's modulus and ultimate compressive stress increased with increasing nanoparticle concentration for both nanoparticles. Due to the higher crosslink density, MA-SiO 2 composites reached a maximum mechanical stress at a concentration of 7.4 wt%, while V-SiO 2 composites reached a maximum at a concentration of 10.7 wt%. Scanning electron microscopy, transmission electron microscopy, and small-angle X-ray scattering revealed a bimodal size distribution for V-SiO 2 and a monomodal size distribution for MA-SiO 2 . Although aggregates were observed for both nanoparticle surface treatments, V-SiO 2 dispersion was poor while MA-SiO 2 were generally well-dispersed. Finally, these findings lay the framework for silica nanofillers in PEG-based nanocomposites for advanced manufacturing applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effects of soybean 7S protein on the quality and digestibility of dry rice noodles under twin‐screw extrusion process

Summary Starch and protein are important components of food, the mixed system formed between them (complexes, gels, mixtures, etc.) can improve the physical and chemical properties of starch and protein, and its potential application in the food industry has also attracted widespread attention. In this study, indica rice flour and soybean 7S protein (β‐Conglycinin) were used as the experimental materials to explore the effect of soybean 7S protein addition on the quality and digestibility of rice noodles. Aims to develop rice noodles with high protein and low GI, so that people can take care of their health while satisfying their appetites. The results showed that with the increase of soybean 7S protein addition, the starch digestibility decreased, resulting in the estimated glycaemic index (eGI) and glycaemic load (GL) decreasing. However, the cooking loss rate and breakage rate of rice noodles gradually increased, the water absorption first increased and then decreased, and the taste of rice noodles is acceptable when the 7S protein addition amount is within 9%. The interaction between starch and soybean 7S protein was mediated by weak interactions such as hydrogen bonds and hydrophobic forces indicated by Fourier transform infrared spectroscopy (FTIR) and X‐ray diffraction (XRD).

Qiao, Fan↗

Intense infrared lasers for strong-field science

The advent of chirped-pulse amplification in the 1980s and femtosecond Ti:sapphire lasers in the 1990s enabled transformative advances in intense laser–matter interaction physics. Whereas most of experiments have been conducted in the limited near-infrared range of 0.8–1 μm, theories predict that many physical phenomena such as high harmonic generation in gases favor long laser wavelengths in terms of extending the high-energy cutoff. Significant progress has been made in developing few-cycle, carrier-envelope phase-stabilized, high-peak-power lasers in the 1.6–2 μm range that has laid the foundation for attosecond X ray sources in the water window. Even longer wavelength lasers are becoming available that are suitable to study light filamentation, high harmonic generation, and laser–plasma interaction in the relativistic regime. Long-wavelength lasers are suitable for sub-bandgap strong-field excitation of a wide range of solid materials, including semiconductors. In the strong-field limit, bulk crystals also produce high-order harmonics. In this review, we first introduce several important wavelength scaling laws in strong-field physics, then describe recent breakthroughs in short- (1.4–3 μm), mid- (3–8 μm), and long-wave (8–15 μm) infrared laser technology, and finally provide examples of strong-field applications of these novel lasers. Furthermore, some of the broadband ultrafast infrared lasers will have profound effects on medicine, environmental protection, and national defense, because their wavelengths cover the water absorption band, the molecular fingerprint region, as well as the atmospheric infrared transparent window.

43 PARTICLE ACCELERATORS↗

Characterization of wood fiber insulation for the development of wood fiber-insulated panels (WIPs) for use in building envelope

Wood fiber insulation (WFI) was studied as an eco-friendly alternative for fossil-based building insulation, focusing on its use in new wood fiber-insulated panels (WIPs). Rigid WFI boards with densities of 110, 140, and 180 kg/m³, including a 140 kg/m³ variant without paraffin wax, were evaluated. Key properties investigated included porosity, water vapor transmission, liquid water adsorption, and thermal conductivity. The porosity ranged between 85 and 92%, primarily influenced by density. Water vapor permeability ranged from 65 to 90 ng·s-1m-1Pa-1, while liquid water absorption was between 2.5 and 20% by volume, influenced by both wax and density. The thermal conductivity coefficient ranged from 0.038 to 0.055 W/(m·K). Bond strength tests with WFI (140 kg/m³ with wax) laminated to various materials using structural adhesives showed tensile perpendicular-to-grain strengths of 10 to 16 kPa and shear strengths of 60 to 90 kPa, with failure only occurring within the WFI. It was concluded that WFI is a promising material for novel WIPs, offering competitive hygrothermal properties and compatibility with structural adhesives. However, its bio-based nature suggests variability and complexity, necessitating further rigorous testing in various climates and in more complex assemblies.

Materials Science↗

Coal-based Bricks & Blocks (CBBs): Process Development to Prototype Fabrication Coupled with Techno-Economic Analysis and Market Survey

The decline of coal use for energy production provides an abundance of local feedstock for new innovative uses and value-added products. Expanding the U.S. coal-value chain to manufacture high-value carbon products can strengthen the nation’s energy and mineral security, enhance the U.S. national defense security, increase the United States’ economic prosperity, while achieving U.S. environmental objectives. The primary project goal is a relatively light-weight composite product with superior (or comparable) compressive strength. Both virgin and, where available, post-consumer recycled thermoplastic versions are tested for each thermoplastic species. A useful attribute of thermoplastics as binders is that they can be heated to their melting point, cooled, and reheated again without significant degradation. A key advantage of thermoset CBBs is that they require only mixing and molding. CBB advantages include low cost, availability, binding ability and processability. Coal-based bricks and blocks (CBBs) weigh about 50% less than clay bricks and can be manufactured with an interlocking design to promote ease of use for the novice builder. CBB formulation is evaluated according to a design-of-experiments (DoE) approach. DoE variables are a) relative weight fractions of binder, b) relative proportions of large versus small (milled) anthracite size fractions, and c) additive percentage. Fabrication methods include hot-press molding and extrusion, the later being the most commercially viable. CBBs are tested for compressive strength, modulus of rupture (by flexure test) and water absorption per ASTM C67, with density determined by the Archimedes drainage method. Fractured interfaces are examined by SEM (Scanning Electron Microscopy) to resolve fracture dynamics and interior microstructure uniformity. Differential scanning calorimetry (DSC) is used to compare plastic transition temperatures i.e., glass and melting temperatures to contrast virgin with post-consumer recycled thermoplastics and optimize their usage. These results are used in the DoE analysis to identify the binder and relative weight percentages for optimum strength, density, and porosity. Overall, CBBs possess strength comparable to clay-based bricks but are non-permeable and hydrophobic, and hence resistant to degradation by freeze-fracturing, corrosion, and efflorescence. The strongest composites have been made with the following thermoplastic binders (in order of strength): thermoset, high-density polyethylene crosslink resin, high-density polyethylene, nylon 6/6, and polypropylene. Results from a techno-economic analysis TEA show economy of scale for CBBs by modularization and reveal the binder as the cost driver for material costs. Ideally, the incorporation of post-consumer recycled thermoplastic will decrease material acquisition costs and increase product sustainability. Notably, CBBs do not require the high temperature calcination needed to produce cement, nor do they require firing in the 1600-2400 °F range for three days using natural gas, as do clay brick equivalents. Instead, CBBs are heated to a modest <600 °F according to the melt flow index of the thermoplastic binder. Existing anthracite mines can be expanded to produce CBBs to reduce aggregate transportation costs and emissions that exist for clay bricks. TEA reflects this reduced energy cost while a comparative CO2 emission analysis quantifies the reduced environmental footprint. The market survey identifies several commercialization opportunities, dependent upon the brick classification.

01 COAL, LIGNITE, AND PEAT↗

Yield stress and flow behavior of enzyme liquefied slurries from corn cobs and corn stover pellets

With the increase in population, the world will depend on renewable sources to meet the increasing energy needs. The use of lignocellulosic biomass as a renewable source has been proven efficient for conversion to cellulosic ethanol and capable of contributing to thresholds for energy demand while reducing greenhouse gases by 90% when compared with fossil fuels. However, limitations in feeding and flow within biorefineries is encountered when system plugging occurs due to biomass compaction and a high yield stress for slurries formed during its processing, thereby preventing transport of biomass materials between plant unit operations. In some cases, this leads to unexpected plant shutdowns increasing industrial operational costs. As an alternative, enzyme-assisted liquefaction for slurry creation from corn stover at solids loadings up to 30% is reported in this work. Two different kinds of biomass (pelleted corn stover and cobs) were liquefied in a fed-batch process using commercial enzymes Celluclast 1.5L or Ctec-2 at 1FPU or 3 FPU per gram of dry solids in 10 mM sodium citrate buffer solution (pH 4.8). Pellets were fed into a 1 L stirred bioreactor according to a pre-defined fed-batch protocol over the first 5 hours until reaching 30% of solids loading. After 6, 24 and 96 hours, samples were taken and characterized with respect to their sugar composition, rheology and water absorption. Successful slurry creation with dramatically reduced yield stress was achieved for corn stover for both assessed enzymes. Yield stresses of 178±7 Pa (3 FPU, Celluclast 1.5L) and 79±6 Pa (3 FPU, Ctec-2) were measured for corn stover at 24 hours, compared to 6,000 Pa for samples without enzyme. Yield stress was 155± 29 Pa (3FPU, Ctec-2) and 257 ± 72 Pa (1 FPU,Celluclast 1.5L) for corn cobs at 24 hours. Yield stress decreased when residence time increased with an enhanced fluidity noted for higher enzyme concentrations. A profile for 6, 24 and 96h of yield stress measurements is presented.

Guitierrez, Diana↗

Enzyme-assisted liquefaction for different fractions of corn stover pellets

With an increase in population, the world will depend on renewable sources to meet the increasing energy needs. The use of lignocellulosic biomass as a renewable source has been proven efficient for conversion to cellulosic ethanol and capable of contributing to thresholds for energy demand while reducing greenhouse gases by 90% when compared with fossil fuels. However, limitations in feeding and flow within biorefineries are encountered when system plugging occurs due to biomass compaction and a high yield stress for slurries formed during its processing. Furthermore, differences in the biomass source present a challenge to the continuity of operations and reliability in the process. This work explores enzyme-assisted liquefaction for solid loadings up to 30% as an alternative for the creation of slurry from two different types of biomass (pelleted corn stover and cobs) that were liquefied in a fed-batch process using commercial enzymes Celluclast 1.5L or Ctec-2 at 1FPU/g or 3 FPU/g of dry solids in a 10 mM sodium citrate buffer solution (pH 4.8). Pellets were fed into a 1 L stirred bioreactor according to a predefined fed-batch protocol during the first 5 hours until 30% solid loading was reached. After 6, 24 and 96 hours, samples were taken and characterized with respect to their composition, rheology, and water absorption. Successful slurry creation with dramatically reduced yield stress was achieved for corn stover for both enzymes assessed. Yield stresses of 178±7 Pa (3 FPU, Celluclast 1.5L) and 79±6 Pa (3 FPU, Ctec-2) were measured for corn stover at 24 hours, compared to 6,000 Pa for samples without enzyme. Yield stress was 155± 29 Pa (3FPU, Ctec-2) and 257 ± 72 Pa (1 FPU, Celluclast 1.5L) for corn cobs at 24 hours. A profile for 6, 24 and 96h of yield stress measurements and sugar conversion is presented.

Gutierrez, Diana↗

Liquefaction of different corn stover fractions assisted by enzyme-biomass deconstruction

Recalcitrant properties of different sources of lignocellulosic biomass represent challenges in materials processing within a biorefinery, as well as enzyme efficient deconstruction to fermentable sugars. Limitations include lignin derived enzyme inhibitors, enzyme inhibition by hydrolysis products, and resistance to mixing due to rheological properties of lignocellulosic particulates at high solids loadings. Consequently, we examined conditions that might be used to achieve liquid slurries (i.e., liquefaction) at solids loadings of 300 g/L before the material enters the biorefinery through a pretreatment step. This work explores enzyme-assisted liquefaction in a fed-batch process using the commercial enzymes Celluclast 1.5L or Ctec-2 at 1FPU/g or 3 FPU/g of dry solids, basis. Corn stover pellets were fed into a 1 L stirred bioreactor containing enzyme solution over a 5-hour period until reaching 30% solids loading (dry wgt / vol basis). After 6, 24 and 96 hours from the start of the run, samples were taken and characterized with respect to their sugar composition, rheology, water absorption and enzyme activity. Slurries with dramatically reduced yield stresses were achieved for corn stover. Yield stresses of 178±7 Pa (3 FPU, Celluclast 1.5L) and 79±6 Pa (3FPU, Ctec-2) were measured for corn stover at 24 hours, compared to 6,000 Pa for samples without enzyme.Yield stress was 155± 29 Pa (3FPU, Ctec-2) and 257 ± 72 Pa (1 FPU, Celluclast 1.5L) for corn cobs at 24 hours.A profile based on 6, 24 and 96h of yield stress measurements and sugar conversion is presented. Enzyme activity is measured and the impact of liquefaction on an integrated processing in a biorefinery operation is discussed.

Gutierrez, Diana↗

High Solids Loading Aqueous Slurry Formation of Corn Stover Before Pretreatment in a Fed-batch Bioreactor

With the increase on population the world will depend on renewable sources to meet the increasingly energy needs. Use of lignocellulosic biomass as a renewable source has been proven efficient for conversion to cellulosic ethanol and capable of contributing to achieve the threshold on energy demand while reducing greenhouse gases in 90% when compared with fossil fuels (Wang et al., 2007, 2012). However, the processing of biomass encounters limitations in feeding and flow within biorefineries due to the system plugging by compaction and slurry high yield stress, preventing transport of biomass materials and in some cases unexpected plant shutdowns that results in high operational costs (dos Santos et al., 2021; Ximenes et al., 2021). Different solutions for biomass handling and slurry formation from densified materials like pellets have been studied. Cellulosic biomass residues are typically processed in pretreatment reactors to which acid or base is added (Humbird et al., 2002). Other pretreatments such as liquid hot water (LHW) and steam explosion that act without the addition of chemicals use pressures above the saturation vapor of water, to disrupt biomass structure (Ruiz et al., 2021). Although these methods are widely known, the use of pretreatments like acid digestion and LHW present challenges like waste disposal and could be energy inefficient (Mosier et al., 2005). Alternatively other approaches like enzymatic liquefaction have been applied for biomass transformation into slurries with promising results and without the use of pretreatments (dos Santos et al., 2021). Nevertheless, enzymatic liquefaction implementation faces difficulties due to the recalcitrant properties of biomass, its variability, and the release of enzyme inhibitors. While it has been proven that chemical composition properties in biomass have effects on enzyme inhibition (Huang et al., 2022; Kim et al., 2011; Zhai et al., 2018), hindering the efficiency of the liquefaction, not ample research has been conducted in understanding the physical properties as particle size, porosity, water adsorption retention and their effect in the ability to form a slurry at high solids concentration (Yan et al., 2020). In order to improve lignocellulosic biomass handling and formation of biomass slurries, enzyme assisted liquefaction for slurry creation from corn stover at solids loadings up to 30% is reported in this work. Two different kinds of biomass (pelleted corn stover and cobs) were liquefied in a fed-batch process using commercial enzymes Celluclast 1.5L or Ctec-2 at 1FPU or 3 FPU per gram of dry solids in 10 mM sodium citrate buffer solution (pH 4.8). Pellets were fed into a 1 L stirred bioreactor according to a predefined fed-batch protocol over the first 5 hours until reaching 30% of solids loading. After 6, 24 and 96 hours, samples were taken and characterized with respect to their sugar composition, rheology and water absorption. Successful slurry creation with dramatically reduced yield stress was achieved for corn stover for both assessed enzymes. Yield stresses of 178±7 Pa (3 FPU, Celluclast 1.5L) and 79±6 Pa (3 FPU, Ctec-2) were measured for corn stover at 24 hours, compared to 6,000 Pa for samples without enzyme. Yield stress was 155± 29 Pa (3FPU, Ctec-2) and 257 ± 72 Pa (1 FPU, Celluclast 1.5L) for corn cobs at 24 hours. Yield stress decreased when residence time increased with an enhanced fluidity noted for higher enzyme concentrations. A profile for 6, 24 and 96h of yield stress measurements is presented.

Gutierrez, Diana↗

Rice Bran Stabilisation and Oil Extraction Using the Microwave-Assisted Method and Its Effects on GABA and Gamma-Oryzanol Compounds

Rice bran oil (RBO) is a valuable ingredient extracted from rice bran (RB), a side stream of polishing rice grain in the milling process. RBO is rich in bioactive ingredients with potential health benefits, such as gamma-oryzanol (GO) and gamma-aminobutyric acid (GABA). Despite its benefits, the quality of RBO depends on the degree of stabilisation of the RB, which is easily affected by lipase enzymes, and thus needs an effective treatment prior to RBO production. To assess the potential of the microwave-assisted method for RB stabilisation and RBO extraction, three Carolino rice varieties (Ariete, Teti, Luna) were tested. The effect of RB stabilisation was evaluated via acid value, water absorption, and GO and GABA levels. The RBO yield was optimised by solvent, temperature, and solvent-to-sample ratio, and the GO and fatty acid levels were determined. The RB stabilisation for the Luna variety did not affect the GO and GABA; for the Ariete and Teti varieties, the GO decreased by 34.4% and 24.2%, and the GABA increased by 26.5% and 47.0%, respectively. The GO levels in RBO samples were not affected by RB stabilisation. The RBO nutritional value was confirmed by the suitable ratio (>2) between polyunsaturated (PUFA) and saturated fatty acids (SFA), with the Teti variety presenting the highest ratio.

Reis, Núria (ORCID:0000000194339109)↗

Bacterial-Retted Hemp Fiber/PLA Composites

The push for sustainability in all facets of manufacturing has led to an increased interest in biomass as an alternative to non-renewable materials. Hemp bast fiber mats were produced from a bacterial retting process, named BFM, as the fiber reinforcement. The objective of this study was to evaluate the feasibility of laminating BFM with polylactic acid (PLA) for a composite panel product. Since both BFM and PLA are biodegradable, the resulting BFM-PLA composites will be 100% biodegradable. PLA pallets were processed into thin polymer sheets which served as the matrix. The BFM and PLA plates were laminated in five layers and compression-molded into composite panels. Experiments were conducted on the three BFM-to-PLA ratios (35/65, 45/55, and 50/50). Mechanical properties (tensile and bending properties) and physical properties (thickness swell and water absorption) were tested and compared to the currently commercial sheet molding compound (SMC) from fiber glass. The thermal behavior of the BFM/PLA composites was characterized using dynamic mechanical analysis (DMA) and differential scanning calorimetry (DSC). The developed BFM/PLA composite product is a sustainable alternative to existing synthetical fiber-reinforced polymer (FRP) that is biodegradable in landfill at the end of life.

Smith, Lee M. (ORCID:0000000264390357)↗

Optical Absorption Spectroscopy Probes Water Wire and Its Ordering in a Hydrogen-Bond Network

Water wires, quasi-one-dimensional chains composed of hydrogen-bonded (H-bonded) water molecules, play a fundamental role in numerous chemical, physical, and physiological processes. Yet direct experimental detection of water wires has been elusive so far. Based on advanced many-body theory that includes electron-hole interactions, we report that optical absorption spectroscopy can serve as a sensitive probe of water wires and their ordering. In both liquid and solid water, the main peak of the spectrum is discovered to be a charge-transfer exciton. In water, the charge-transfer exciton is strongly coupled to the H-bonding environment where the exciton is excited between H-bonded water molecules with a large spectral intensity. In regular ice, the spectral weight of the charge-transfer exciton is enhanced by a collective excitation occurring on proton-ordered water wires, whose spectral intensity scales with the ordering length of water wire. The spectral intensity and excitonic interaction strength reaches its maximum in ice XI, where the long-range ordering length yields the most pronounced spectral signal. Our findings suggest that water wires, which widely exist in important physiological and biological systems and other phases of ice, can be directly probed by this approach. Published by the American Physical Society 2025

Tang, Fujie (ORCID:0000000197615359)↗

Isotope effects in x-ray absorption spectra of liquid water

The isotope effects in x-ray absorption spectra of liquid water are studied by a many-body approach within electron-hole excitation theory. The molecular structures of both light and heavy water are modeled by path-integral molecular dynamics based on the advanced deep-learning technique. The neural network is trained on ab initio data obtained with SCAN density functional theory. The experimentally observed isotope effect in x-ray absorption spectra is reproduced semiquantitatively in theory. Compared to the spectrum in normal water, the blueshifted and less pronounced pre- and main-edge in heavy water reflect that the heavy water is more structured at short- and intermediate-range of the hydrogen-bond network. In contrast, we find the isotope effect on the spectrum is negligible at post-edge, which is consistent with the identical long-range ordering in both liquids as observed in the diffraction experiment.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Role of water vapour in the absorption of nanosecond 266-nm laser pulses by atmospheric air

The absorption of the Nd : YAG fourth harmonic in air and binary mixtures of water vapour with nitrogen and oxygen at atmospheric pressure has been measured as a function of pulse energy (peak intensity). The mixtures obtained by adding equal amounts of water vapour to dry nitrogen and oxygen have been found to differ significantly in absorption. Preliminary quantitative data have been obtained for two- and three-photon absorption cross sections of water and oxygen molecules: σ{sup (2)}(H{sub 2}O) = (4 ± 1) ± 10{sup –49} cm{sup 4} s and σ{sup (3)}(O{sub 2}) = (5.6 ± 1.4) ± 10{sup –78} cm{sup 6} s{sup 2}. The absorption of 266-nm pulses with peak intensities from 0.05 to 2 GW cm{sup –2} in the near-surface atmosphere has been shown to be determined by two-photon absorption in water vapour and three-photon absorption in oxygen. In moist air containing 1 % water vapour, the absorption coefficient for 266-nm laser pulses exceeds that in dry air by four to five times. There is no absorption in nitrogen. We have developed a technique for photoacoustic measurements of multiphoton absorption cross sections in single-component gases and gas mixtures. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Many-body effects in the X-ray absorption spectra of liquid water

Significance In X-ray absorption spectroscopy, an electron–hole excitation probes the local atomic environment. The interpretation of the spectra requires challenging theoretical calculations, particularly in a system like liquid water, where quantum many-body effects and molecular disorder play an important role. Recent advances in theory and simulation make possible new calculations that are in good agreement with experiment, without recourse to commonly adopted approximations. Based on these calculations, the three features observed in the experimental spectra are unambiguously attributed to excitonic effects with different characteristic correlation lengths, which are distinctively affected by perturbations of the underlying H-bond structure induced by temperature changes and/or by isotopic substitution. The emerging picture of the water structure is fully consistent with the conventional tetrahedral model.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗