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1. Summertime Airborne Measurements of Ammonia Emissions From Cattle Feedlots and Dairies in Northeastern Colorado

   https://doi.org/10.1029/2023JD039043  

   Juncosa_Calahorrano, Julieta F; Pollack, Ilana B; Sullivan, Amy P; Roscioli, J Robert; Caulton, Dana R; McCabe, Megan E; Li, En; Pierce, Jeffrey R; Fischer, Emily V (December 2023, Journal of Geophysical Research: Atmospheres)

   Abstract Phase One of the Transportation and Transformation of Ammonia (TRANS²Am) field campaign took place in northeastern Colorado during the summer of 2021. One of the goals of TRANS²Am was to measure ammonia (NH₃) emissions from cattle feedlots and dairies. Most of these animal husbandry facilities are co‐located within oil and gas development, an important source of methane (CH₄) and ethane (C₂H₆) in the region. Phase One of TRANS²Am included 12 near‐source research flights. We present estimates of NH₃emissions ratios with respect to CH₄(NH₃EmR), with and without correction of CH₄from oil and gas, for 29 feedlots and dairies in the region. The data shows larger emissions ratios than previously reported in the literature with a large range of values (i.e., 0.1–2.6 ppbv ppbv⁻¹). Facilities housing cattle and dairy had a mean (std) of 1.20 (0.63) and 0.29 (0.08) ppbv ppbv⁻¹, respectively. We also found that only 15% of the total ammonia (NH_x) is in the particle phase (i.e., ) near major sources during the warm summertime months. We examined the evolution of NH₃in one plume that was sampled at different distances and altitudes up to 25 km downwind and estimated the NH₃lifetime against deposition and partitioning to the particle phase to be 87–120 min. Finally, we calculated estimates of NH₃emission rates from four optimally sampled facilities. These ranged from 4 to 29 g NH₃ · h⁻¹ · hd⁻¹. 

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2. Investigation of coastal ammonium aerosol sources in the Northwest Pacific Ocean

   https://doi.org/10.1016/j.atmosenv.2023.120034  

   MacFarland, Alexandra B; Joyce, Emily E; Wang, Xuchen; Walters, Wendell W; Altieri, Katye E; Schiebel, Hayley N; Hastings, Meredith G (November 2023, Atmospheric Environment)

   Determining the magnitude and origins of nitrogen (N) deposition in the open ocean is vital for understanding how anthropogenic activities influence oceanic biogeochemical cycles. Excess N in the North Pacific Ocean(NPO) is suggested to reflect recent anthropogenic atmospheric deposition from the Asian continent, changes in nutrient dynamics due to marine N-fixation, and/or lateral transport of nutrients. We investigate the impact of anthropogenic and marine sources on reactive N deposition in the NPO, with a focus on ammonium (NH4+), an important bioavailable nutrient, using aerosol samples (n =108) collected off the coast of China (Changdao Island). This study site is used as a proxy for continental emissions that can be exported and subsequently deposited to the ocean. The NH4+concentration of aerosol samples varied seasonally (p < 0.05), with a higher average value in winter (2.8 ±1.1 μg/m3) and spring (1.9 ±0.8 μg/m3) compared to autumn (0.7 ±0.6 μg/m3) and summer (1.4 ±0.4 μg/m3). The isotopic composition of aerosol NH4+ varied seasonally, with higher averages in spring (13.3 ±7.9‰) and summer (15.6 ±6.2‰) compared to autumn (3.2 ±2.5 ‰) and winter (3.8 ±11.4‰). These seasonal patterns in the isotopic composition of NH4+ are investigated based on correlations of aerosol chemical species, seasonal shifts in transport patterns, partitioning of ammonia/ammonium between the gas and particle phase, and continental versus marine sources of ammonia. We find that anthropogenic activities, mainly agricultural practices (e.g., volatilization, fertilizer, animal husbandry), are the primary sources of NH4+ deposited to the NPO. 

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3. Organic aerosol formation from the reactive uptake of isoprene epoxydiols (IEPOX) onto non-acidified inorganic seeds

   https://doi.org/10.5194/acp-14-3497-2014  

   Nguyen, T. B.; Coggon, M. M.; Bates, K. H.; Zhang, X.; Schwantes, R. H.; Schilling, K. A.; Loza, C. L.; Flagan, R. C.; Wennberg, P. O.; Seinfeld, J. H. (January 2014, Atmospheric Chemistry and Physics)

   The reactive partitioning of cis and trans β-IEPOX was investigated on hydrated inorganic seed particles, without the addition of acids. No organic aerosol (OA) formation was observed on dry ammonium sulfate (AS); however, prompt and efficient OA growth was observed for the cis and trans β-IEPOX on AS seeds at liquid water contents of 40–75% of the total particle mass. OA formation from IEPOX is a kinetically limited process, thus the OA growth continues if there is a reservoir of gas-phase IEPOX. There appears to be no differences, within error, in the OA growth or composition attributable to the cis / trans isomeric structures. Reactive uptake of IEPOX onto hydrated AS seeds with added base (NaOH) also produced high OA loadings, suggesting the pH dependence for OA formation from IEPOX is weak for AS particles. No OA formation, after particle drying, was observed on seed particles where Na⁺ was substituted for NH₄⁺. The Henry's Law partitioning of IEPOX was measured on NaCl particles (ionic strength ~9 M) to be 3 × 10⁷ M atm⁻¹ (−50 / +100%). A small quantity of OA was produced when NH₄⁺ was present in the particles, but the chloride (Cl^-) anion was substituted for sulfate (SO₄^2-), possibly suggesting differences in nucleophilic strength of the anions. Online time-of-flight aerosol mass spectrometry and offline filter analysis provide evidence of oxygenated hydrocarbons, organosulfates, and amines in the particle organic composition. The results are consistent with weak correlations between IEPOX-derived OA and particle acidity or liquid water observed in field studies, as the chemical system is nucleophile-limited and not limited in water or catalyst activity. 

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4. Secondary organic aerosol formation from the β-pinene+NO₃ system: effect of humidity and peroxy radical fate

   https://doi.org/10.5194/acp-15-7497-2015  

   Boyd, C. M.; Sanchez, J.; Xu, L.; Eugene, A. J.; Nah, T.; Tuet, W. Y.; Guzman, M. I.; Ng, N. L. (January 2015, Atmospheric Chemistry and Physics)

   Abstract. The formation of secondary organic aerosol (SOA) from the oxidation of β-pinene via nitrate radicals is investigated in the Georgia Tech Environmental Chamber (GTEC) facility. Aerosol yields are determined for experiments performed under both dry (relative humidity (RH) < 2 %) and humid (RH = 50 % and RH = 70 %) conditions. To probe the effects of peroxy radical (RO₂) fate on aerosol formation, "RO₂ + NO₃ dominant" and "RO₂ + HO₂ dominant" experiments are performed. Gas-phase organic nitrate species (with molecular weights of 215, 229, 231, and 245 amu, which likely correspond to molecular formulas of C₁₀H₁₇NO₄, C₁₀H₁₅NO₅, C₁₀H₁₇NO₅, and C₁₀H₁₅NO₆, respectively) are detected by chemical ionization mass spectrometry (CIMS) and their formation mechanisms are proposed. The NO⁺ (at m/z 30) and NO₂⁺ (at m/z 46) ions contribute about 11 % to the combined organics and nitrate signals in the typical aerosol mass spectrum, with the NO⁺ : NO₂⁺ ratio ranging from 4.8 to 10.2 in all experiments conducted. The SOA yields in the "RO₂ + NO₃ dominant" and "RO₂ + HO₂ dominant" experiments are comparable. For a wide range of organic mass loadings (5.1–216.1 μg m^&minus;3), the aerosol mass yield is calculated to be 27.0–104.1 %. Although humidity does not appear to affect SOA yields, there is evidence of particle-phase hydrolysis of organic nitrates, which are estimated to compose 45–74 % of the organic aerosol. The extent of organic nitrate hydrolysis is significantly lower than that observed in previous studies on photooxidation of volatile organic compounds in the presence of NO_x. It is estimated that about 90 and 10 % of the organic nitrates formed from the β-pinene+NO₃ reaction are primary organic nitrates and tertiary organic nitrates, respectively. While the primary organic nitrates do not appear to hydrolyze, the tertiary organic nitrates undergo hydrolysis with a lifetime of 3–4.5 h. Results from this laboratory chamber study provide the fundamental data to evaluate the contributions of monoterpene + NO₃ reaction to ambient organic aerosol measured in the southeastern United States, including the Southern Oxidant and Aerosol Study (SOAS) and the Southeastern Center for Air Pollution and Epidemiology (SCAPE) study. 

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5. Airborne and ground-based observations of ammonium-nitrate-dominated aerosols in a shallow boundary layer during intense winter pollution episodes in northern Utah

   https://doi.org/10.5194/acp-18-17259-2018  

   Franchin, Alessandro; Fibiger, Dorothy L.; Goldberger, Lexie; McDuffie, Erin E.; Moravek, Alexander; Womack, Caroline C.; Crosman, Erik T.; Docherty, Kenneth S.; Dube, William P.; Hoch, Sebastian W.; et al (January 2018, Atmospheric Chemistry and Physics)

   Abstract. Airborne and ground-based measurements of aerosol concentrations, chemicalcomposition, and gas-phase precursors were obtained in three valleys innorthern Utah (USA). The measurements were part of the Utah Winter FineParticulate Study (UWFPS) that took place in January–February 2017. Totalaerosol mass concentrations of PM₁ were measured from a Twin Otteraircraft, with an aerosol mass spectrometer (AMS). PM₁ concentrationsranged from less than 2µgm⁻³ during clean periods to over100µgm⁻³ during the most polluted episodes, consistent withPM_2.5 total mass concentrations measured concurrently at groundsites. Across the entire region, increases in total aerosol mass above∼2µgm⁻³ were associated with increases in theammonium nitrate mass fraction, clearly indicating that the highest aerosolmass loadings in the region were predominantly attributable to an increase inammonium nitrate. The chemical composition was regionally homogenous fortotal aerosol mass concentrations above 17.5µgm⁻³, with 74±5% (average±standard deviation) ammonium nitrate, 18±3%organic material, 6±3% ammonium sulfate, and 2±2%ammonium chloride. Vertical profiles of aerosol mass and volume in the regionshowed variable concentrations with height in the polluted boundary layer.Higher average mass concentrations were observed within the first few hundredmeters above ground level in all three valleys during pollution episodes. Gas-phase measurements of nitric acid (HNO₃) and ammonia (NH₃) duringthe pollution episodes revealed that in the Cache and Utah valleys, partitioningof inorganic semi-volatiles to the aerosol phase was usually limited by theamount of gas-phase nitric acid, with NH₃ being in excess. The inorganicspecies were compared with the ISORROPIA thermodynamic model. Total inorganicaerosol mass concentrations were calculated for various decreases in totalnitrate and total ammonium. For pollution episodes, our simulations of a50% decrease in total nitrate lead to a 46±3% decrease in totalPM₁ mass. A simulated 50% decrease in total ammonium leads to a36±17%µgm⁻³ decrease in total PM₁ mass, over the entirearea of the study. Despite some differences among locations, ourresults showed a higher sensitivity to decreasing nitric acid concentrationsand the importance of ammonia at the lowest total nitrate conditions. In theSalt Lake Valley, both HNO₃ and NH₃ concentrations controlledaerosol formation. 

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