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This work focuses on total organic carbon (TOC) and contributing species in cloud water over Southeast Asia using a rare airborne dataset collected during NASA's Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex), in which a wide variety of maritime clouds were studied, including cumulus congestus, altocumulus, altostratus, and cumulus. Knowledge of TOC masses and their contributing species is needed for improved modeling of cloud processing of organics and to understand how aerosols and gases impact and are impacted by clouds. This work relies on 159 samples collected with an axial cyclone cloud-water collector at altitudes of 0.2–6.8 km that had sufficient volume for both TOC and speciated organic composition analysis. Species included monocarboxylic acids (glycolate, acetate, formate, and pyruvate), dicarboxylic acids (glutarate, adipate, succinate, maleate, and oxalate), methanesulfonic acid (MSA), and dimethylamine (DMA). TOC values range between 0.018 and 13.66 ppm C with a mean of 0.902 ppm C. The highest TOC values are observed below 2 km with a general reduction aloft. An exception is samples impacted by biomass burning for which TOC remains enhanced at altitudes as high as 6.5 km (7.048 ppm C). Estimated total organic matter derived from TOC contributes a mean of 30.7 % to total measured mass (inorganics + organics). Speciated organics contribute (on a carbon mass basis) an average of 30.0 % to TOC in the study region and account for an average of 10.3 % to total measured mass. The order of the average contribution of species to TOC, in decreasing contribution of carbon mass, is as follows (±1 standard deviation): acetate (14.7 ± 20.5 %), formate (5.4 ± 9.3 %), oxalate (2.8 ± 4.3 %), DMA (1.7 ± 6.3 %), succinate (1.6 ± 2.4 %), pyruvate (1.3 ± 4.5 %), glycolate (1.3 ± 3.7 %), adipate (1.0 ± 3.6 %), MSA (0.1 ± 0.1 %), glutarate (0.1 ± 0.2 %), and maleate (< 0.1 ± 0.1 %). Approximately 70 % of TOC remains unaccounted for, highlighting the complex nature of organics in the study region; in samples collected in biomass burning plumes, up to 95.6 % of TOC mass is unaccounted for based on the species detected. Consistent with other regions, monocarboxylic acids dominate the speciated organic mass (∼ 75 %) and are about 4 times more abundant than dicarboxylic acids. Samples are categorized into four cases based on back-trajectory history, revealing source-independent similarity between the bulk contributions of monocarboxylic and dicarboxylic acids to TOC (16.03 %–23.66 % and 3.70 %–8.75 %, respectively). Furthermore, acetate, formate, succinate, glutarate, pyruvate, oxalate, and MSA are especially enhanced during biomass burning periods, which is attributed to peat emissions transported from Sumatra and Borneo. Lastly, dust (Ca2+) and sea salt (Na+/Cl-) tracers exhibit strong correlations with speciated organics, supporting how coarse aerosol surfaces interact with these water-soluble organics.

Fireworks degrade air quality, reduce visibility, alter atmospheric chemistry, and cause short-term adverse health effects. However, there have not been any comprehensive physicochemical and optical measurements of fireworks and their associated impacts in a Southeast Asia megacity, where fireworks are a regular part of the culture. Size-resolved particulate matter (PM) measurements were made before, during, and after New Year 2019 at the Manila Observatory in Quezon City, Philippines, as part of the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex). A high-spectral-resolution lidar (HSRL) recorded a substantial increase in backscattered signal associated with high aerosol loading ∼440 m above the surface during the peak of firework activities around 00:00 (local time). This was accompanied by PM2.5 concentrations peaking at 383.9 µg m−3. During the firework event, water-soluble ions and elements, which affect particle formation, growth, and fate, were mostly in the submicrometer diameter range. Total (>0.056 µm) water-soluble bulk particle mass concentrations were enriched by 5.7 times during the fireworks relative to the background (i.e., average of before and after the firework). The water-soluble mass fraction of PM2.5 increased by 18.5 % above that of background values. This corresponded to increased volume fractions of inorganics which increased bulk particle hygroscopicity, kappa (κ), from 0.11 (background) to 0.18 (fireworks). Potassium and non-sea-salt (nss) SO42- contributed the most (70.9 %) to the water-soluble mass, with their mass size distributions shifting from a smaller to a larger submicrometer mode during the firework event. On the other hand, mass size distributions for NO3-, Cl−, and Mg2+ (21.1 % mass contribution) shifted from a supermicrometer mode to a submicrometer mode. Being both uninfluenced by secondary aerosol formation and constituents of firework materials, a subset of species were identified as the best firework tracer species (Cu, Ba, Sr, K+, Al, and Pb). Although these species (excluding K+) only contributed 2.1 % of the total mass concentration of water-soluble ions and elements, they exhibited the highest enrichments (6.1 to 65.2) during the fireworks. Surface microscopy analysis confirmed the presence of potassium/chloride-rich cubic particles along with capsule-shaped particles in firework samples. The results of this study highlight how firework emissions change the physicochemical and optical properties of water-soluble particles (e.g., mass size distribution, composition, hygroscopicity, and aerosol backscatter), which subsequently alters the background aerosol's respirability, influence on surroundings, ability to uptake gases, and viability as cloud condensation nuclei (CCN).

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-aerosol-loading 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.

The South China Sea (SCS) is a receptor of numerous natural and anthropogenic aerosol species from throughout greater Asia. A combination of several developing countries, archipelagic and peninsular terrain, a strong Asian monsoon climate, and a host of multi-scale meteorological phenomena make the SCS one of the most complex aerosol–meteorological systems in the world. However, aside from the well-known biomass burning emissions from Indonesia and Borneo, the current understanding of aerosol sources is limited, especially in remote marine environments. In September 2011, a 2-week research cruise was conducted near Palawan, Philippines, to sample the remote SCS environment. Size-segregated aerosol data were collected using a Davis Rotating Uniform size-cut Monitor (DRUM) sampler and analyzed for concentrations of 28 elements measured via X-ray fluorescence (XRF). Positive matrix factorization (PMF) was performed separately on the coarse, fine, and ultrafine size ranges to determine possible sources and their contributions to the total elemental particulate matter mass. The PMF analysis resolved six sources across the three size ranges: biomass burning, oil combustion, soil dust, a crustal–marine mixed source, sea spray, and fly ash. Additionally, size distribution plots, time series plots, back trajectories and satellite data were used in interpreting factors. The multi-technique source apportionment revealed the presence of biogenic sources such as soil dust, sea spray, and a crustal–marine mixed source. Anthropogenic sources were also identified: biomass burning, oil combustion, and fly ash. Mass size distributions showed elevated aerosol concentrations towards the end of the sampling period, which coincided with a shift of air mass back trajectories to southern Kalimantan. Covariance between coarse-mode soil dust and fine-mode biomass burning aerosols were observed. Agreement between the PMF and the linear regression analyses indicates that the PMF solution is robust. While biomass burning is indeed a key source of aerosol, this study shows the presence of other important sources in the SCS. Identifying these sources is not only key for characterizing the chemical profile of the SCS but, by improving our picture of aerosol sources in the region, also a step forward in developing our understanding of aerosol–meteorology feedbacks in this complex environment.

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.