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  1. Free, publicly-accessible full text available June 1, 2024
  2. Abstract With the motivation to study how non-magnetic ion site disorder affects the quantum magnetism of Ba 3 CoSb 2 O 9 , a spin-1/2 equilateral triangular lattice antiferromagnet, we performed DC and AC susceptibility, specific heat, elastic and inelastic neutron scattering measurements on single crystalline samples of Ba 2.87 Sr 0.13 CoSb 2 O 9 with Sr doping on non-magnetic Ba 2+ ion sites. The results show that Ba 2.87 Sr 0.13 CoSb 2 O 9 exhibits (i) a two-step magnetic transition at 2.7 K and 3.3 K, respectively; (ii) a possible canted 120 degree spin structure at zero field with reduced ordered moment as 1.24 μ B /Co; (iii) a series of spin state transitions for both H ∥ ab -plane and H ∥ c -axis. For H ∥ ab -plane, the magnetization plateau feature related to the up–up–down phase is significantly suppressed; (iv) an inelastic neutron scattering spectrum with only one gapped mode at zero field, which splits to one gapless and one gapped mode at 9 T. All these features are distinctly different from those observed for the parent compound Ba 3 CoSb 2 O 9 , which demonstrates that the non-magnetic ion site disorder (the Sr doping) plays a complex role on the magnetic properties beyond the conventionally expected randomization of the exchange interactions. We propose the additional effects including the enhancement of quantum spin fluctuations and introduction of a possible spatial anisotropy through the local structural distortions. 
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  3. null (Ed.)
  4. We present a novel source attribution approach that incorporates satellite data into GEOS-Chem adjoint simulations to characterize the species-specific, regional, and sectoral contributions of daily emissions for 3 air pollutants: fine particulate matter (PM2.5), ozone (O3), and nitrogen dioxide (NO2). This approach is implemented for Washington, DC, first for 2011, to identify urban pollution sources, and again for 2016, to examine the pollution response to changes in anthropogenic emissions. In 2011, anthropogenic emissions contributed an estimated 263 (uncertainty: 130–444) PM2.5- and O3-attributable premature deaths and 1,120 (391–1795) NO2 attributable new pediatric asthma cases in DC. PM2.5 exposure was responsible for 90% of these premature deaths. On-road vehicle emissions contributed 51% of NO2-attributable new asthma cases and 23% of pollution-attributable premature deaths, making it the largest contributing individual sector to DC’s air pollution–related health burden. Regional emissions, originating from Maryland, Virginia, and Pennsylvania, were the most responsible for pollution-related health impacts in DC, contributing 57% of premature deaths impacts and 89% of asthma cases. Emissions from distant states contributed 34% more to PM2.5 exposure in the wintertime than in the summertime, occurring in parallel with strong wintertime westerlies and a reduced photochemical sink. Emission reductions between 2011 and 2016 resulted in health benefits of 76 (28–149) fewer pollution-attributable premature deaths and 227 (2–617) fewer NO2-attributable pediatric asthma cases. The largest sectors contributing to decreases in pollution-related premature deaths were energy generation units (26%) and on-road vehicles (20%). Decreases in NO2-attributable pediatric asthma cases were mostly due to emission reductions from on-road vehicles (63%). Emission reductions from energy generation units were found to impact PM2.5 more than O3, while on-road vehicle emission reductions impacted O3 proportionally more than PM2.5. This novel method is capable of capturing the sources of urban pollution at fine spatial and temporal scales and is applicable to many urban environments, globally. 
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  5. null (Ed.)
    Abstract Spin-valley locking in monolayer transition metal dichalcogenides has attracted enormous interest, since it offers potential for valleytronic and optoelectronic applications. Such an exotic electronic state has sparsely been seen in bulk materials. Here, we report spin-valley locking in a Dirac semimetal BaMnSb 2 . This is revealed by comprehensive studies using first principles calculations, tight-binding and effective model analyses, angle-resolved photoemission spectroscopy measurements. Moreover, this material also exhibits a stacked quantum Hall effect (QHE). The spin-valley degeneracy extracted from the QHE is close to 2. This result, together with the Landau level spin splitting, further confirms the spin-valley locking picture. In the extreme quantum limit, we also observed a plateau in the z -axis resistance, suggestive of a two-dimensional chiral surface state present in the quantum Hall state. These findings establish BaMnSb 2 as a rare platform for exploring coupled spin and valley physics in bulk single crystals and accessing 3D interacting topological states. 
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  6. Peracetic acid (PAA) is a sanitizer with increasing use in food, medical and water treatment industries. Amino acids are important components in targeted foods for PAA treatment and ubiquitous in natural waterbodies and wastewater effluents as the primary form of dissolved organic nitrogen. To better understand the possible reactions, this work investigated the reaction kinetics and transformation pathways of selected amino acids towards PAA. Experimental results demonstrated that most amino acids showed sluggish reactivity to PAA except cysteine (CYS), methionine (MET), and histidine (HIS). CYS showed the highest reactivity with a very rapid reaction rate. Reactions of MET and HIS with PAA followed second-order kinetics with rate constants of 4.6 ± 0.2, and 1.8 ± 0.1 M−1s−1 at pH 7, respectively. The reactions were faster at pH 5 and 7 than at pH 9 due to PAA speciation. Low concentrations of H2O2 coexistent with PAA contributed little to the oxidation of amino acids. The primary oxidation products of amino acids with PAA were [O] addition compounds on the reactive sites at thiol, thioether and imidazole groups. Theoretical calculations were applied to predict the reactivity and regioselectivity of PAA electrophilic attacks on amino acids and improved mechanistic understanding. As an oxidative disinfectant, the reaction of PAA with organics to form byproducts is inevitable; however, this study shows that PAA exhibits lower and more selective reactivity towards biomolecules such as amino acids than other common disinfectants, causing less concern of toxic disinfection byproducts. This attribute may allow greater stability and more targeted actions of PAA in various applications. 
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