Bayesian Maximum Entropy Integration of Ozone Observations and Model Predictions: A National Application

To improve ozone exposure estimates for ambient concentrations at a national scale, we introduce our novel Regionalized Air Quality Model Performance (RAMP) approach to integrate chemical transport model (CTM) predictions with the available ozone observations using the Bayesian Maximum Entropy (BME) framework. The framework models the nonlinear and nonhomoscedastic relation between air pollution observations and CTM predictions and for the first time accounts for variability in CTM model performance. A validation analysis using only noncollocated data outside of a validation radius <i>r</i>_<i>v</i> was performed and the <i>R</i>² between observations and re-estimated values for two daily metrics, the daily maximum 8-h average (DM8A) and the daily 24-h average (D24A) ozone concentrations, were obtained with the OBS scenario using ozone observations only in contrast with the RAMP and a Constant Air Quality Model Performance (CAMP) scenarios. We show that, by accounting for the spatial and temporal variability in model performance, our novel RAMP approach is able to extract more information in terms of <i>R</i>² increase percentage, with over 12 times for the DM8A and over 3.5 times for the D24A ozone concentrations, from CTM predictions than the CAMP approach assuming that model performance does not change across space and time

Data_Sheet_1_Characteristics of soil microbiota and organic carbon distribution in jackfruit plantation under different fertilization regimes.docx

Manure amendment to improve soil organic carbon (SOC) content is an important strategy to sustain ecosystem health and crop production. Here, we utilize an 8-year field experiment to evaluate the impacts of organic and chemical fertilizers on SOC and its labile fractions as well as soil microbial and nematode communities in different soil depths of jackfruit (Artocarpus heterophyllus Lam.). Three treatments were designed in this study, including control with no amendment (CK), organic manure (OM), and chemical fertilizer (CF). Results showed that OM significantly increased the abundance of total nematodes, bacterivores, bacteria, and fungi as well as the value of nematode channel ratio (NCR) and maturity index (MI), but decreased plant-parasites and Shannon diversity (H′). Soil microbial and nematode communities in three soil depths were significantly altered by fertilizer application. Acidobacteria and Chloroflexi dominated the bacterial communities of OM soil, while Nitrospira was more prevalent in CF treatment. Organic manure application stimulated some functional groups of the bacterial community related to the C cycle and saprotroph-symbiotroph fungi, while some groups related to the nitrogen cycle, pathotroph-saprotroph-symbiotroph and pathotroph-saprotroph fungi were predominated in CF treatment. Furthermore, OM enhanced the soil pH, contents of total soil N, P, K, and SOC components, as well as jackfruit yield. Chemical fertilizers significantly affected available N, P, and K contents. The results of network analyses show that more significant co-occurrence relationships between SOC components and nematode feeding groups were found in CK and CF treatments. In contrast, SOC components were more related to microbial communities than to nematode in OM soils. Partial least-squares-path modeling (PLS-PM) revealed that fertilization had significant effects on jackfruit yield, which was composed of positive direct (73.6%) and indirect effects (fertilization → fungal community → yield). It was found that the long-term manure application strategy improves soil quality by increasing SOM, pH, and nutrient contents, and the increased microbivorous nematodes abundance enhanced the grazing pressure on microorganisms and concurrently promoted microbial-derived SOC turnover.</p

Charge Transport Behavior in Solution-Grown Methylammonium Lead Tribromide Perovskite Single Crystal Using α Particles

Methylammonium (MA) lead hybrid perovskite single crystal recently received attention as a potential radiation detection material. Here, we report the MAPbBr₃ bulk crystals grown by the modified antisolvent vapor-assisted crystallization method. The growth rate is determined by diluting the antisolvent, which results in the average size of MAPbBr₃ crystals to significantly increase from 2 × 2 × 1 to 15 × 15 × 5 mm³. The morphology evolution of MAPbBr₃ crystals, which is contributed by the growth anisotropy, has been discussed according to the molar ratios of precursors and the bond theory. The resulting centimeter-sized MAPbBr₃ crystals exhibit high resistivity (5.6 × 10⁸ Ω·cm) at room temperature. The mobility–lifetime (μτ) products are measured under ²⁴¹Am (5.48 MeV) α particles irradiation, with the values of 2.2 × 10^–4 and 4.2 × 10^–4 cm²/V for electrons and holes, respectively. Simultaneously, the electrons and holes mobility are estimated to be 24.6 and 59.7 cm²/(V·s), respectively, using the α-source-induced transient waveforms

Ligand-Free, Quantum-Confined Cs₂SnI₆ Perovskite Nanocrystals

Tin-halide perovskite nanocrystals are a viable precursor for lead-free, high-efficiency active layers for photovoltaic cells. We describe a new synthetic procedure for quantum-confined Cs₂SnI₆ nanocrystals with size-dependent band gaps in the long-visible to near-infrared (1.38–1.47 eV). Hot injection synthesis produces particles with no organic capping ligands, with average diameters that increase from 12 ± 2.8 nm to 38 ± 4.1 nm with increasing reaction temperature. The band gap, energies of the first excitonic peak, ground-state bleach peak (in the transient absorption spectrum), and photoluminescence peak depend linearly on the inverse square of diameter, consistent with quantum-confined excitons with an effective mass of (0.12 ± 0.02)<i>m</i>₀, where <i>m</i>₀ is the mass of an electron, a factor of 4.6 smaller than that in the bulk material. Transient absorption measurements show that approximately 90% of the bleach amplitude decays within 30 ps, probably because of carrier trapping on unpassivated surface sites. The films made by simple drop-casting of Cs₂SnI₆ nanocrystal solutions, with no postsynthetic ligand exchange or removal, are smooth and uniform, resist delamination, and have no visible gaps at the film–substrate interface

Gradient Structure Design of Flexible Waterborne Polyurethane Conductive Films for Ultraefficient Electromagnetic Shielding with Low Reflection Characteristic

Highly efficient electromagnetic shielding materials entailing strong electromagnetic wave absorption and low reflection have become an increasing requirement for next-generation communication technologies and high-power electronic instruments. In this study, a new strategy is employed to provide flexible waterborne polyurethane composite films with an ultra-efficient electromagnetic shielding effectiveness (EMI SE) and low reflection by constructing gradient shielding layers with a magnetic ferro/ferric oxide deposited on reduced graphene oxide (rGO@Fe₃O₄) and silver-coated tetraneedle-like ZnO whisker (T-ZnO/Ag) functional nanoparticles. Because of the differences in density between rGO@Fe₃O₄ and T-ZnO/Ag, a gradient structure is automatically formed during the film formation process. The gradient distribution of rGO@Fe₃O₄ over the whole thickness range forms an efficient electromagnetic wave absorption network that endows the film with a strong absorption ability on the top side, while a thin layer of high-density T-ZnO/Ag at the bottom constructs a highly conductive network that provides an excellent electromagnetic reflection ability for the film. This specific structure results in an “absorb–reflect–reabsorb” process when electromagnetic waves penetrate into the composite film, leading to an excellent EMI shielding performance with an extremely low reflection characteristic at a very low nanofiller content (0.8 vol % Fe₃O₄@rGO and 5.7 vol % T-ZnO/Ag): the EMI SE reaches 87.2 dB against the X band with a thickness of only 0.5 mm, while the shielding effectiveness of reflection (SE_R) is only 2.4 dB and the power coefficient of reflectivity (<i>R</i>) is as low as 0.39. This result means that only 39% of the microwaves are reflected in the propagation process when 99.9999998% are attenuated, which is the lowest value among the reported references. This composite film with remarkable performance is suitable for application in portable and wearable smart electronics, and this method offers an effective strategy for absorption-dominated EMI shielding

Self-Assembly of Nanoporous ZIF-8-Based Superstructures for Robust Chemical Sensing of Solvent Vapors

Self-assembly of metal–organic frameworks (MOFs) to construct optical sensors has been proposed to detect chemicals by acclimating colors in response to analytes that adsorbed on the surface of MOF nanoparticles and in the interspaces between particles. However, the instability of the weakly assembled optical structures held together by van der Waals forces limits their active sensing application. Here, we propose full-color tunable superstructures that are constructed by self-assembled ZIF-8 nanoparticles and postsynthetic poly(dimethylsiloxane) (PDMS) coating, which behave as robust optical sensors. The optical band was tuned by controlling the size of the ZIF-8 particles and also responded to the adsorption of chemicals with different refractive indexes in the micropores of the ZIF-8 particles. In addition, PDMS-coated ZIF-8 superstructures (ZIF-8@PDMS) were fabricated by thermal evaporation to optimize the optical quality and improve the robustness and solvent resistance during chemical sensing. Static and dynamic sensing results showed that the hierarchical porous structures endow the ZIF-8@PDMS superstructure with higher optical saturation and faster response in comparison to their counterparts configured with a ZIF-8 superstructure

Geochronology and petrogenesis of the early Silurian Zeluo mafic-ultramafic intrusion, eastern Tibet: implications for the tectonic setting and evolution of the eastern Proto-Tethys Ocean

The Tibetan Plateau is a key region to understand the evolution of the Tethys Oceans. To better constrain the tectonic evolution of the Proto-Tethys Ocean on the western margin of the Yangtze plate, we present an integrated petrography, geochemistry, and zircon U-Pb-Lu-Hf isotope study on newly recognized early Silurian gabbro and serpentinite rocks from the eastern Yidun terrane of the Tibetan Plateau. Zircon U-Pb dating of the gabbro yields an Early Silurian age of 438.2 ± 2.8 Ma. Zircon εHf(t) values of 5.4 to 8.5 suggest a single-stage model age (TDM1) ranging from 729 to 858 Ma. The gabbros exhibit low total rare earth element abundances but are moderately enriched in the light rare earth elements and the large-ion lithophile elements (e.g. Rb, Ba, and Sr), and display representative negative high-field strength elemental anomalies for Nb, Ta, Zr, and Hf on spidergrams. The gabbro and serpentinites were derived from a depleted mantle-like source made of garnet-spinel lherzolite composition, from a sub-arc mantle wedge that was metasomatized by slab dehydration. Thus, the gabbro and serpentinites record an Early Silurian subduction event of the Proto-Tethys Ocean under the Yangtze plate. Furthermore, this study confirms that the Yidun terrane on the western margin of the Yangtze plate is underlined by a Precambrian crystalline basement.</p

Role of Stoichiometry in the Growth of Large Pb₂P₂Se₆ Crystals for Nuclear Radiation Detection

Pb₂P₂Se₆ as a heavy element, chemically robust semiconductor, has been identified as a promising material for cost-effective room temperature X/γ-ray detection. Here, we report the properties of Pb₂P₂Se₆ crystals grown by a vertical Bridgman method under off-stoichiometric Se-rich and Pb-rich conditions. Regardless of the conditions the resulting single crystals exhibited high bulk resistivity on the order of 10¹¹ Ω·cm. However, the photoconductivity and charge transport properties varied based on growth condition indicating the different dominant defects associated with the type of stoichiometric deviation. The formation and nature of intrinsic defects in Pb₂P₂Se₆ crystals were also studied by first-principles density functional theory (DFT) calculations as well as thermally stimulated current (TSC) spectroscopy. The TSC results indicated that four traps were common to both Se-rich and Pb-rich Pb₂P₂Se₆, while a higher density of shallow defects were observed in Se-rich Pb₂P₂Se₆. DFT calculations predict that the antisite defects P_Pb⁺, P_Se^– and Pb_P^– are the dominant deep donors and acceptors in Se-rich and Pb-rich Pb₂P₂Se₆, respectively, which leads to the degradation of mobility lifetime product (μτ) on the order of 10^–5 cm²·V^–1 as measured under ²⁴¹Am (5.48 MeV) alpha particles irradiation. Nevertheless, Pb₂P₂Se₆ detectors with a thickness of 2 mm show reliable linear response under a series of radiation sources, including ²⁴¹Am and ⁵⁷Co γ-ray sources. A high X-ray sensitivity comparable to that of amorphous Se for Pb-rich Pb₂P₂Se₆ detectors was realized, with the value of 68.3 μC·Gy_air^–1 cm^–2 under 40 kVp Ag X-rays at an electrical field of 50 V·cm^–1

Cu₂I₂Se₆: A Metal–Inorganic Framework Wide-Bandgap Semiconductor for Photon Detection at Room Temperature

Cu₂I₂Se₆ is a new wide-bandgap semiconductor with high stability and great potential toward hard radiation and photon detection. Cu₂I₂Se₆ crystallizes in the rhombohedral <i>R</i>3̅<i>m</i> space group with a density of <i>d</i> = 5.287 g·cm^–3 and a wide bandgap <i>E</i>_g of 1.95 eV. First-principles electronic band structure calculations at the density functional theory level indicate an indirect bandgap and a low electron effective mass <i>m</i>_e* of 0.32. The congruently melting compound was grown in centimeter-size Cu₂I₂Se₆ single crystals using a vertical Bridgman method. A high electric resistivity of ∼10¹² Ω·cm is readily achieved, and detectors made of Cu₂I₂Se₆ single crystals demonstrate high photosensitivity to Ag Kα X-rays (22.4 keV) and show spectroscopic performance with energy resolutions under ²⁴¹Am α-particles (5.5 MeV) radiation. The electron mobility is measured by a time-of-flight technique to be ∼46 cm²·V^–1·s^–1. This value is comparable to that of one of the leading γ-ray detector materials, TlBr, and is a factor of 30 higher than mobility values obtained for amorphous Se for X-ray detection

Stoichiometric Effects on the Photoelectric Properties of LiInSe₂ Crystals for Neutron Detection

⁶LiInSe₂ is a promising semiconductor candidate for thermal neutron detection due to its large capture cross-section. However, the charge collection efficiency is still insufficient for high resolution for the grown-in defects induced by the stoichiometric deviation. In this work, we report photoelectric properties of stoichiometric LiInSe₂ crystal boules up to 70 mm in length and 20 mm in diameter grown by the vertical Bridgman method. Inductively coupled plasma measurements demonstrate that the ratio of Li, In, and Se of the as-grown crystal is very close to 1:1:2, which is optimized by low temperature synthesis processing. The obtained single crystals display high bulk resistivity in the range of 10¹¹–10¹² Ω·cm and a direct band gap of 2.01–2.83 eV with a changeable color from red to yellow. The electronic structure of LiInSe₂ was studied using first-principles density functional theory calculations, which predicts that the antisite defects of In_Li and Li_In are the dominant factor for the different crystal colors observed. The stoichiometric LiInSe₂ crystal gives an improved energy resolution, for a semiconductor detector when illuminated with a ²⁴¹[email protected] MeV α source, of 23.3%. The electron mobility-lifetime product (<i>μτ</i>) is ∼2.5 × 10^–5 cm² V^–1