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 PMcoarse (i.e., PM10–PM2.5). A case study emphasized how transport of wildfire plumes significantly impacted downwind states, with higher levels of fine soil and PMcoarse 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.

Abstract. 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 (Dp): 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 SO42-, NH4+, NO3-, 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.

We report on a multiyear set of airborne field campaigns (2005–16) off the California coast to examine aerosols, clouds, and meteorology, and how lessons learned tie into the upcoming NASA Earth Venture Suborbital (EVS-3) campaign: Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE; 2019–23). The largest uncertainty in estimating global anthropogenic radiative forcing is associated with the interactions of aerosol particles with clouds, which stems from the variability of cloud systems and the multiple feedbacks that affect and hamper efforts to ascribe changes in cloud properties to aerosol perturbations. While past campaigns have been limited in flight hours and the ability to fly in and around clouds, efforts sponsored by the Office of Naval Research have resulted in 113 single aircraft flights (>500 flight hours) in a fixed region with warm marine boundary layer clouds. All flights used nearly the same payload of instruments on a Twin Otter to fly below, in, and above clouds, producing an unprecedented dataset. We provide here i) an overview of statistics of aerosol, cloud, and meteorological conditions encountered in those campaigns and ii) quantification of model-relevant metrics associated with aerosol–cloud interactions leveraging the high data volume and statistics. Based on lessons learned from those flights, we describe the pragmatic innovation in sampling strategy (dual-aircraft approach with combined in situ and remote sensing) that will be used in ACTIVATE to generate a dataset that can advance scientific understanding and improve physical parameterizations for Earth system and weather forecasting models, and for assessing next-generation remote sensing retrieval algorithms.

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. Key Points: • Significant biomass burning (BB) layer stratification with majority of layers in the free troposphere within 100 m of the boundary layer top • A new smoke injection height method improved agreement for the vertical distribution of BB aerosol in the NAAPS model versus in situ data • Shortwave heating rate profiles demonstrate the combined effect of stratocumulus cloud and BB layers and their mutual interactions Supporting Information:• Supporting Information S1• Data Set S1

Airborne measurements of meteorological, aerosol, and stratocumulus cloud properties have been harmonized from six field campaigns during July-August months between 2005 and 2016 off the California coast. A consistent set of core instruments was deployed on the Center for Interdisciplinary Remotely-Piloted Aircraft Studies Twin Otter for 113 flight days, amounting to 514 flight hours. A unique aspect of the compiled data set is detailed measurements of aerosol microphysical properties (size distribution, composition, bioaerosol detection, hygroscopicity, optical), cloud water composition, and different sampling inlets to distinguish between clear air aerosol, interstitial in-cloud aerosol, and droplet residual particles in cloud. Measurements and data analysis follow documented methods for quality assurance. The data set is suitable for studies associated with aerosol-cloud-precipitation-meteorology-radiation interactions, especially owing to sharp aerosol perturbations from ship traffic and biomass burning. The data set can be used for model initialization and synergistic application with meteorological models and remote sensing data to improve understanding of the very interactions that comprise the largest uncertainty in the effect of anthropogenic emissions on radiative forcing.

This work examines particulate chloride (Cl) and bromide (Br) depletion in marine aerosol particles influenced by wildfires at a coastal California site in the summers of 2013 and 2016. Chloride exhibited a dominant coarse mode due to sea salt influence, with substantially diminished concentrations during fire periods as compared to nonfire periods. Bromide exhibited a peak in the submicrometer range during fire and nonfire periods, with an additional supermicrometer peak in the latter periods. Chloride and Br depletions were enhanced during fire periods as compared to nonfire periods. The highest observed %Cl depletion occurred in the submicrometer range, with maximum values of 98.9% (0.32-0.56 μm) and 85.6% (0.56-1 μm) during fire and nonfire periods, respectively. The highest %Br depletion occurred in the supermicrometer range during fire and nonfire periods with peak depletion between 1.8-3.2 μm (78.8% and 58.6%, respectively). When accounting for the neutralization of sulfate by ammonium, organic acid particles showed the greatest influence on Cl depletion in the submicrometer range. These results have implications for aerosol hygroscopicity and radiative forcing in areas with wildfire influence owing to depletion effects on composition.

Cloud adiabaticity (α) is defined as the ratio of the actual liquid water path (LWPmeasured) in a cloud to its corresponding adiabatic value (LWPad). Processes such as drizzle and entrainment can lead to subadiabatic LWPmeasured. This study examines α and its relationship to microphysical properties for 86 cloud events over the Northeast Pacific Ocean based on data collected during four separate summertime airborne campaigns. For the study region, α was found to be 0.766 ± 0.134. For most cases, clouds with a low value of α were found to have lower droplet number concentration (Nd), higher droplet effective radius (re), higher relative dispersion (d), and higher rain rate (R). The subcloud aerosol concentration (Na) was often less for the low‐α cases. The relationship between α and the vertical profiles and cloud‐top characteristics for both the cloud droplet‐only spectrum and full spectrum (cloud and rain droplets) is also examined. Inclusion of rain droplets produced a larger change in d for the low‐α clouds as compared to the high‐α clouds. On average, R increased at cloud top for high‐α clouds but decreased at cloud top for low‐α clouds. Accounting for α when estimating Nd from Moderate Resolution Imaging Spectroradiometer retrievals results in better agreement with in situ Nd values. Results of this work motivate the need for additional focus on the factors governing α, such as cloud type, and implications of its value, especially for remote‐sensing retrievals.

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