This study examines major wildfires in the western United States between 2005 and 2015 to determine which species exhibit the highest percent change in mass concentration on day of peak fire influence relative to preceding nonfire days. Forty‐one fires were examined using the Environmental Protection Agency (EPA) Interagency Monitoring of Protected Visual Environments (IMPROVE) data set. Organic carbon (OC) and elemental carbon (EC) constituents exhibited the highest percent change increase. The sharpest enhancements were for the volatile (OC1) and semivolatile (OC2) OC fractions, suggestive of secondary organic aerosol formation during plume transport. Of the noncarbonaceous constituents, Cl, P, K, NO₃⁻, and Zn levels exhibited the highest percent change. Dust was significantly enhanced in wildfire plumes, based on significant enhancements in fine soil components (i.e., Si, Ca, Al, Fe, and Ti) and PM_coarse (i.e., PM₁₀–PM_2.5). A case study emphasized how transport of wildfire plumes significantly impacted downwind states, with higher levels of fine soil and PM_coarse at the downwind state (Arizona) as compared to the source of the fires (California). A global model (Navy Aerosol Analysis and Prediction System, NAAPS) did not capture the dust influence over California or Arizona during this case event because it is not designed to resolve dust dynamics in fires, which motivates improved treatment of such processes. Significant chloride depletion was observed on the peak EC day for almost a half of the fires examined. Size‐resolved measurements during two specific fires at a coastal California site revealed significant chloride reductions for particle aerodynamic diameters between 1 and 10 μm.

This paper presents novel results from size-resolved particulate matter (PM) mass, composition, and morphology measurements conducted during the 2018 southwest monsoon (SWM) season in Metro Manila, Philippines. Micro-orifice uniform deposit impactors (MOUDIs) were used to collect PM sample sets composed of size-resolved measurements at the following aerodynamic cut-point diameters (D_p): 18, 10, 5.6, 3.2, 1.8, 1.0, 0.56, 0.32, 0.18, 0.10, and 0.056 µm. Each sample set was analyzed for composition of the water-soluble fraction. Analysis for mass was carried out on two sample sets, whereas black carbon (BC) and morphology analysis were analyzed on a single sample set. The bulk of the PM mass was between 0.18 and 1.0 µm with a dominant mode between 0.32 and 0.56 µm. Similarly, most of the black carbon (BC) mass was found between 0.10 and 1.0 µm, peaking between 0.18 and 0.32 µm. These peaks are located in the Greenfield gap, or the size range between 0.10 and 1.0 µm, where wet scavenging by rain is relatively inefficient. In the range between 0.10 and 0.18 µm, BC constituted 78.1 % of the measured mass. Comparable contributions of BC (26.9 %) and the water-soluble fraction (33.4 %) to total PM were observed and most of the unresolved mass, which amounted to 39.6 % in total, was for diameters exceeding 0.32 µm. The water-soluble ions and elements exhibited an average combined concentration of 8.53 µg m⁻³, with ${\mathrm{SO}}_{\mathrm{4}}^{\mathrm{2}-}$ , ${\mathrm{NH}}_{\mathrm{4}}^{+}$ , ${\mathrm{NO}}_{\mathrm{3}}^{-}$ , Na⁺, and Cl⁻ as the major contributors. Positive matrix factorization (PMF) was applied to identify the possible aerosol sources and estimate their contribution to the water-soluble fraction of collected PM. The factor with the highest contribution was attributed to “aged aerosol” (48.0 %), while “sea salt” (22.5 %) and “combustion” emissions (18.7 %) had comparable contributions. “Vehicular/resuspended dust” (5.6 %) and “waste processing” emissions (5.1 %) were also identified. Microscopy analysis highlighted the ubiquity of nonspherical particles regardless of size, which is significant when considering calculations of parameters such as single scattering albedo, the asymmetry parameter, and the extinction efficiency. The significant influence from aged aerosol to Metro Manila during the SWM season indicates that local sources in this megacity do not fully govern this coastal area's aerosol properties. The fact that the majority of the regional aerosol mass burden is accounted for by BC and other insoluble components has important downstream effects on the aerosol hygroscopic properties, which depend on composition. The results are relevant for understanding the impacts of monsoonal features on size-resolved aerosol properties, notably aqueous processing and wet scavenging. Finally, the results of this work provide contextual data for future sampling campaigns in Southeast Asia such as the airborne component of the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP²Ex) planned for the SWM season in 2019.

Leveraging aerosol data from multiple airborne and surface‐based field campaigns encompassing diverse environmental conditions, we calculate statistics of the oxalate‐sulfate mass ratio (median: 0.0217; 95% confidence interval: 0.0154–0.0296; R = 0.76; N = 2,948). Ground‐based measurements of the oxalate‐sulfate ratio fall within our 95% confidence interval, suggesting the range is robust within the mixed layer for the submicrometer particle size range. We demonstrate that dust and biomass burning emissions can separately bias this ratio toward higher values by at least one order of magnitude. In the absence of these confounding factors, the 95% confidence interval of the ratio may be used to estimate the relative extent of aqueous processing by comparing inferred oxalate concentrations between air masses, with the assumption that sulfate primarily originates from aqueous processing.

Cloud droplet chemical composition is a key observable property that can aid understanding of how aerosols and clouds interact. As part of the Clouds, Aerosols and Monsoon Processes – Philippines Experiment (CAMP²Ex), three case studies were analyzed involving collocated airborne sampling of relevant clear and cloudy air masses associated with maritime warm convection. Two of the cases represented a polluted marine background, with signatures of transported East Asian regional pollution, aged over water for several days, while the third case comprised a major smoke transport event from Kalimantan fires. Sea salt was a dominant component of cloud droplet composition, in spite of fine particulate enhancement from regional anthropogenic sources. Furthermore, the proportion of sea salt was enhanced relative to sulfate in rainwater and may indicate both a propensity for sea salt to aid warm rain production and an increased collection efficiency of large sea salt particles by rain in subsaturated environments. Amongst cases, as precipitation became more significant, so too did the variability in the sea salt to (non-sea salt) sulfate ratio. Across cases, nitrate and ammonium were fractionally greater in cloud water than fine-mode aerosol particles; however, a strong covariability in cloud water nitrate and sea salt was suggestive of prior uptake of nitrate on large salt particles. A mass-based closure analysis of non-sea salt sulfate compared the cloud water air-equivalent mass concentration to the concentration of aerosol particles serving as cloud condensation nuclei for droplet activation. While sulfate found in cloud was generally constrained by the sub-cloud aerosol concentration, there was significant intra-cloud variability that was attributed to entrainment – causing evaporation of sulfate-containing droplets – and losses due to precipitation. In addition, precipitation tended to promote mesoscale variability in the sub-cloud aerosol through a combination of removal, convective downdrafts, and dynamically driven convergence. Physical mechanisms exerted such strong control over the cloud water compositional budget that it was not possible to isolate any signature of chemical production/loss using in-cloud observations. The cloud-free environment surrounding the non-precipitating smoke case indicated sulfate enhancement compared to convective mixing quantified by a stable gas tracer; however, this was not observed in the cloud water (either through use of ratios or the mass closure), perhaps implying that the warm convective cloud timescale was too short for chemical production to be a leading-order budgetary term and because precursors had already been predominantly exhausted. Closure of other species was truncated by incomplete characterization of coarse aerosol (e.g., it was found that only 10 %–50 % of sea salt mass found in cloud was captured during clear-air sampling) and unmeasured gas-phase abundances affecting closure of semi-volatile aerosol species (e.g., ammonium, nitrate and organic) and soluble volatile organic compound contributions to total organic carbon in cloud water.

This study uses airborne cloud water composition measurements to characterize the vertical structure of air‐equivalent mass concentrations of water‐soluble species in marine stratocumulus clouds off the California coast. A total of 385 cloud water samples were collected in the months of July and August between 2011 and 2016 and analyzed for water‐soluble ionic and elemental composition. Three characteristic profiles emerge: (i) a reduction of concentration with in‐cloud altitude for particulate species directly emitted from sources below cloud without in‐cloud sources (e.g., Cl⁻ and Na⁺), (ii) an increase of concentration with in‐cloud altitude (e.g., NO₂⁻ and formate), and (iii) species exhibiting a peak in concentration in the middle of cloud (e.g., non–sea‐salt SO₄²⁻, NO₃⁻, and organic acids). Vertical profiles of rainout parameters such as loss frequency, lifetime, and change in concentration with respect to time show that the scavenging efficiency throughout the cloud depth depends strongly on the thickness of the cloud. Thin clouds exhibit a greater scavenging loss frequency at cloud top, while thick clouds have a greater scavenging loss frequency at cloud base. The implications of these results for treatment of wet scavenging in models are discussed.

This study characterizes in situ airborne properties associated with biomass burning (BB) plumes in the vicinity of the California coast. Out of 231 total aircraft soundings in July–August 2013 and 2016, 81 were impacted by BB layers. A number of vertical characteristics of BB layers are summarized in this work (altitude, location relative to cloud top height, thickness, number of vertically adjacent layers, interlayer distances) in addition to differences in vertical aerosol concentration profiles due to either surface type (e.g., land or ocean) or time of day. Significant BB layer stratification occurred, especially over ocean versus land, with the majority of layers in the free troposphere and within 100 m of the boundary layer top. Heating rate profiles demonstrated the combined effect of cloud and BB layers and their mutual interactions, with enhanced heating in BB layers with clouds present underneath. Aerosol size distribution data are summarized below and above the boundary layer, with a notable finding being enhanced concentrations of supermicrometer particles in BB conditions. A plume aging case study revealed the dominance of organics in the free troposphere, with secondary production of inorganic and organic species and coagulation as a function of distance from fire source up to 450 km. Rather than higher horizontal and vertical resolution, a new smoke injection height method was the source of improved agreement for the vertical distribution of BB aerosol in the Navy Aerosol Analysis and Prediction System model when compared to airborne data.