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.

No abstract

This study reports a characterization of the real part of dry particle refractive index (n) at 532 nm based on airborne measurements over the United States, Canada, the Pacific Ocean, and the Gulf of Mexico from the 2012 Deep Convective Clouds and Chemistry (DC3) and 2013 Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC 4 RS) campaigns. Effective n values are reported, with the limitations and uncertainties discussed. Eight air mass types were identified based on criteria related to gas-phase tracer concentrations, location, and altitude. Average values of n for these air types ranged from 1.50 to 1.53. Values of n for the organic aerosol (OA) fraction (n OA ) were calculated using a linear mixing rule for each air mass type, with 1.52 shown to be a good approximation for all OA. Case studies detailing vertical structure revealed that n and n OA increased with altitude, simultaneous with enhancements in the mass fraction of OA. Values of n OA were positively (negatively) correlated with the O:C (H:C) ratio in the absence of biomass burning influence; in contrast, the cumulative data set revealed a slight decrease in n OA as a function of the O:C ratio. The performance of parametric (multiple linear regression) and nonparametric (Gaussian process regression) methods in predicting n based on aerosol composition data is discussed. It is shown that even small perturbations in n values significantly impact aerosol optical depth retrievals, radiative forcing, and optical sizing instruments, emphasizing the importance of further improving the understanding of this important aerosol property.

Abstract. A 16-month (July 2018–October 2019) dataset of size-resolved aerosol composition is used to examine the sources and characteristics of five organic acids (oxalate, succinate, adipate, maleate, phthalate) and methanesulfonate (MSA) in Metro Manila, Philippines. As one of the most polluted megacities globally, Metro Manila offers a view of how diverse sources and meteorology impact the relative amounts and size distributions of these species. A total of 66 sample sets were collected with a Micro-Orifice Uniform Deposit Impactor (MOUDI), of which 54 sets were analyzed for composition. Organic acids and MSA surprisingly were less abundant than in other global regions that are also densely populated. The combined species accounted for an average of 0.80 ± 0.66 % of total gravimetric mass between 0.056 and 18 µm, still leaving 33.74 % of mass unaccounted for after considering black carbon and water-soluble ions and elements. The unresolved mass is suggested to consist of non-water-soluble metals as well as both water-soluble and non-water-soluble organics. Oxalate was approximately an order of magnitude more abundant than the other five species (149 ± 94 ng m−3 versus others being < 10 ng m−3) across the 0.056–18 µm size range. Both positive matrix factorization (PMF) and correlation analysis are conducted with tracer species to investigate the possible sources of organic acids and MSA. Enhanced biomass burning influence in the 2018 southwest monsoon resulted in especially high levels of submicrometer succinate, MSA, oxalate, and phthalate. Peculiarly, MSA had negligible contributions from marine sources but instead was linked to biomass burning and combustion. Enhanced precipitation during the two monsoon seasons (8 June–4 October 2018 and 14 June–7 October 2019) coincided with a stronger influence from local emissions rather than long-range transport, leading to notable concentration enhancements in both the sub- and supermicrometer ranges for some species (e.g., maleate and phthalate). While secondary formation via gas-to-particle conversion is consistent with submicrometer peaks for the organic acids and MSA, several species (i.e., phthalate, adipate, succinate, oxalate) exhibited a prominent peak in the coarse mode, largely owing to their association with crustal emissions (i.e., more alkaline aerosol type) rather than sea salt. Oxalate's strong association with sulfate in the submicrometer mode supports an aqueous-phase formation pathway for the study region. However, high concentrations during periods of low rain and high solar radiation suggest photo-oxidation is an important formation pathway.

This study analyzes long-range transport of aerosol and aerosol chemical characteristics based on instances of high-and low-aerosol-loading events determined via ground-based size-resolved aerosol measurements collected at the Manila Observatory in Metro Manila, Philippines, from July to October 2018. Multiple data sources, including models, remote sensing, and in situ measurements, are used to analyze the impacts of long-range aerosol transport on Metro Manila and the conditions at the local and synoptic scales facilitating this transport. Through the use of case studies, evidence of long-range transport of biomass burning aerosol and continental emissions is identified in Metro Manila. Long-range transport of biomass burning aerosol from the Maritime Continent, bolstered by southwesterly flow and permitted by low rainfall, was identified through model results and the presence of biomass burning tracers (e.g., K, Rb) in the ground-based measurements. The impacts of emissions transported from continental East Asia on the aerosol characteristics in Metro Manila are also identified; for one of the events analyzed, this transport was facilitated by the nearby passage of a typhoon. Changes in the aerosol size distributions, water-soluble chemical composition, and contributions of various organic aerosol species to the total water-soluble organic aerosol were examined for the different cases. The events impacted by biomass burning transport had the overall highest concentration of water-soluble organic acids, while the events impacted by long-range transport from continental East Asia showed high percent contributions from shorter-chain dicarboxylic acids (i.e., oxalate) that are often representative of photochemical and aqueous processing in the atmosphere. The low-aerosolloading event was subject to a larger precipitation accumulation than the high-aerosol events, indicative of wet scavenging as an aerosol sink in the study region. This low-aerosol event was characterized by a larger relative contribution from supermicrometer aerosols and had a higher percent contribution from longer-chain dicarboxylic acids (i.e., maleate) to the water-soluble organic aerosol fraction, indicating the importance of both primary aerosol emissions and local emissions.