Biomass Burning Particles Research Articles

Case study of the effects of aerosol chemical composition and hygroscopicity on the scattering coefficient in summer, Xianghe, southeast of Beijing, China

The aerosol scattering coefficient is mainly affected by various factors, such as aerosol chemical composition, hygroscopicity and relative humidity. A comprehensive observation of the chemical and physical properties of aerosols was conducted in Xianghe, southeast of Beijing, from June 15 to 26, 2018. Five specific cases were analysed during this observation: (1) rainy (RA); (2) low visibility during the day (LD); (3) high visibility during the day (HD); (4) low visibility at night (LN); and (5) high visibility at night (HN). The mass percentages of a secondary inorganic aerosol (nitrate, sulfate and ammonium) measured with a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) were 64.5% and 68.3% during LD and LN, which were higher than those (63.6% and 46.1%) observed during HD and HN, respectively. The mass percentages of secondary organic aerosol (SOA) and primary organic aerosol (POA) to organic aerosol were 76.6% and 23.4%, respectively, during LD. The hygroscopic parameters κ were 0.59 and 0.60 during LD and LN, which were slightly higher than those (0.57 and 0.58) observed during HD and HN, respectively, indicating that the variation of aerosol chemical composition had a limited impact on hygroscopicity. The average proportion, measured with a single particle aerosol mass spectrometer (SPAMS), of biomass burning, dust, heavy metal, soot-like, sea salt, secondary aerosols and other particles were 12.3%, 2.9%, 16.2%, 36.1%, 8.8%, 21.0% and 2.7%. The average proportions of soot-like and secondary aerosols were 42.4% and 19.2% from 0.2 to 1.0 μm. Although the variation and height of the mixing layer were similar between LD and HD, clouds reduced the solar radiation during LD, which caused a higher relative humidity (RH) (67.5%) than that (45.9%) observed during HD. A larger wind speed below 850 hpa during HN caused the mixing layer height (MLH) to reach 1910 m, which resulted in a lower RH (64.8%) than that (68.0%) observed during LN. The light scattering enhancement factors f(RH) during low visibility events were almost greater than those observed during high visibility events, regardless of they were measured during the day (0–9.7%) or night (0–13.1%). The aerosol hygroscopic growth factor (GF) maintained a similar trend with RH, indicating that RH was the main factor affecting the hygroscopic growth of the aerosol, resulting in the decrease in visibility.

Seasonal study of stable carbon and nitrogen isotopic composition in fine aerosols at a Central European rural background station

Abstract. A study of the stable carbon isotope ratios (δ13C) of total carbon (TC) and the nitrogen isotope ratios (δ15N) of total nitrogen (TN) was carried out for fine aerosol particles (PM1) and was undertaken every 2 days with a 24 h sampling period at a rural background site in Košetice (Central Europe) from 27 September 2013 to 9 August 2014 (n=146). We found a seasonal pattern for both δ13C and δ15N. The seasonal variation in δ15N was characterized by lower values (average of 13.1±4.5 ‰) in winter and higher values (25.0±1.6 ‰) in summer. Autumn and spring were transition periods when the isotopic composition gradually changed due to the changing sources and ambient temperature. The seasonal variation in δ13C was less pronounced but more depleted in 13C in summer (-27.8±0.4 ‰) as compared to winter (-26.7±0.5 ‰). A comparative analysis with water-soluble ions, organic carbon, elemental carbon, trace gases and meteorological parameters (mainly ambient temperature) has shown major associations with the isotopic compositions, which has provided greater knowledge and understanding of the corresponding processes. A comparison of δ15N with NO3-, NH4+ and organic nitrogen (OrgN) revealed that although a higher content of NO3- was associated with a decrease in the δ15N of TN, NH4+ and OrgN caused increases. The highest concentrations of nitrate, mainly represented by NH4NO3 related to the emissions from biomass burning leading to an average δ15N of TN (13.3 ‰) in winter. During spring, the percentage of NO3- in PM1 decreased. An enrichment of 15N was probably driven by the equilibrium exchange between the gas and aerosol phases (NH3(g) ↔ NH4+(p)), which is supported by the increased ambient temperature. This equilibrium was suppressed in early summer when the molar ratios of NH4+/SO42- reached 2, and the nitrate partitioning in aerosol was negligible due to the increased ambient temperature. Summertime δ15N values were among the highest, suggesting the aging of ammonium sulfate and OrgN aerosols. Such aged aerosols can be coated by organics in which 13C enrichment takes place by the photooxidation process. This result was supported by a positive correlation of δ13C with ambient temperature and ozone, as observed in the summer season. During winter, we observed an event with the lowest δ15N and highest δ13C values. The winter event occurred in prevailing southeast air masses. Although the higher δ13C values probably originated from biomass-burning particles, the lowest δ15N values were probably associated with agriculture emissions of NH3 under low-temperature conditions (< 0 ∘C).

Characteristics of single atmospheric particles in a heavily polluted urban area of China: size distributions and mixing states

To investigate the chemical composition, size distribution, and mixing state of aerosol particles on heavy pollution days, single-particle aerosol mass spectrometry was conducted during 9-26 October 2015 in Xi'an, China. The measured particles were classified into six major categories: biomass burning (BB) particles, K-secondary particles, elemental carbon (EC)-related particles, metal-containing particles, dust, and organic carbon (OC) particles. BB and EC-related particles were the dominant types during the study period and mainly originated from biomass burning, vehicle emissions, and coal combustion. According to the ambient air quality index, two typical episodes were defined: clean days (CDs) and polluted days (PDs). Accumulation of BB particles and EC-related particles was the main reason for the pollution in Xi'an. Most types of particle size were larger on PDs than CDs. Each particle type was mixed with secondary species to different degrees on CDs and PDs, indicating that atmospheric aging occurred. The mixing state results demonstrated that the primary tracers were oxidized or vanished and that the amount of secondary species was increased on PDs. This study provides valuable information and a dataset to help control air pollution in the urban areas of Xi'an. Graphical abstract.

Construction and Characterization of an Indoor Smog Chamber for Measuring the Optical and Physicochemical Properties of Aging Biomass Burning Aerosols

ABSTRACT We describe here the construction and characterization of a new combustion-chamber system (the NCAT chamber) for studying the optical and physicochemical properties of biomass burning (BB) aerosols. This system is composed of a ~9 m3 fluorinated ethylene propylene (FEP) film reactor placed in a temperature-controlled room that uses a tube furnace to combust biomass fuel samples under controlled conditions. The optical properties are measured using a cavity ring-down spectrometer and nephelometer. Aerosol number density and size classification used condensation particle counter, and differential mobility analyzer. Other analytical instruments, used include NOx, O3, CO, and CO2 analyzers, a gas chromatograph, and particle filter samples for determining the physicochemical and morphological properties. The construction details and characterization experiments are described, including measurements of the BB particulate size distribution and deposition rate, gas wall loss rates, dilution rate, light intensity, mixing speed, temperature and humidity variations, and air purification method. The wall loss rates for NO, NO2, and O3 were found to be (7.40 ± 0.01) × 10–4, (3.47 ± 0.01) × 10–4, and (5.90 ± 0.08) × 10–4 min–1, respectively. The NO2 photolysis rate constant was 0.165 ± 0.005 min–1, which corresponds to a flux of (7.72 ± 0.25) × 1017 photons nm cm–2 s–1 for 296.0–516.8 nm, and the particle deposition rate was (9.46 ± 0.18) × 10–3 min–1 for 100 nm mobility diameter BB particles from pine. Preliminary results of the single scattering albedo of fresh and aged BB aerosols are also reported.

Differential toxicities of fine particulate matters from various sources

Fine particulate matters less than 2.5 µm (PM2.5) in the ambient atmosphere are strongly associated with adverse health effects. However, it is unlikely that all fine particles are equally toxic in view of their different sizes and chemical components. Toxicity of fine particles produced from various combustion sources (diesel engine, gasoline engine, biomass burning (rice straw and pine stem burning), and coal combustion) and non-combustion sources (road dust including sea spray aerosols, ammonium sulfate, ammonium nitrate, and secondary organic aerosols (SOA)), which are known major sources of PM2.5, was determined. Multiple biological and chemical endpoints were integrated for various source-specific aerosols to derive toxicity scores for particles originating from different sources. The highest toxicity score was obtained for diesel engine exhaust particles, followed by gasoline engine exhaust particles, biomass burning particles, coal combustion particles, and road dust, suggesting that traffic plays the most critical role in enhancing the toxic effects of fine particles. The toxicity ranking of fine particles produced from various sources can be used to better understand the adverse health effects caused by different fine particle types in the ambient atmosphere, and to provide practical management of fine particles beyond what can be achieved only using PM mass which is the current regulation standard.

Cloud Condensation Nuclei Activity and Hygroscopicity of Fresh and Aged Biomass Burning Particles

Biomass burning particles are one of the largest aerosol sources worldwide and contribute a significant fraction of the global cloud condensation nuclei (CCN) burden. Chemical aging experiments of sawgrass burning particles took place in a smog chamber by turning on the UV light after HONO or H2O2 injection. The CCN activity and corresponding hygroscopicity of fresh and aged particles were measured. Most of the fresh particles can serve as reasonable CCN, and the average activation diameters at 0.2% supersaturation were 114–125 nm in the experiments. The aging process caused that the mass fraction of organic aerosols decrease and condensed phase nitrate NO3− increase, and also the average atomic oxygen to carbon (O:C) ratios increase, which were the main reasons that the aged particles were more CCN active and hygroscopic. The average activation diameters decreased by 8–15% at 0.2% supersaturation after aging, and hygroscopic parameter κ increased by 30–42%. The chemical aging productions were a little different in experiments, but the CCN property and hygroscopicity change trends were quite similar.

Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition

Abstract. Secondary organic aerosol (SOA) accounts for a large fraction of submicron particles in the atmosphere. SOA can occur in amorphous solid or semi-solid phase states depending on chemical composition, relative humidity (RH), and temperature. The phase transition between amorphous solid and semi-solid states occurs at the glass transition temperature (Tg). We have recently developed a method to estimate Tg of pure compounds containing carbon, hydrogen, and oxygen atoms (CHO compounds) with molar mass less than 450 g mol−1 based on their molar mass and atomic O : C ratio. In this study, we refine and extend this method for CH and CHO compounds with molar mass up to ∼ 1100 g mol−1 using the number of carbon, hydrogen, and oxygen atoms. We predict viscosity from the Tg-scaled Arrhenius plot of fragility (viscosity vs. Tg∕T) as a function of the fragility parameter D. We compiled D values of organic compounds from the literature and found that D approaches a lower limit of ∼ 10 (±1.7) as the molar mass increases. We estimated the viscosity of α-pinene and isoprene SOA as a function of RH by accounting for the hygroscopic growth of SOA and applying the Gordon–Taylor mixing rule, reproducing previously published experimental measurements very well. Sensitivity studies were conducted to evaluate impacts of Tg, D, the hygroscopicity parameter (κ), and the Gordon–Taylor constant on viscosity predictions. The viscosity of toluene SOA was predicted using the elemental composition obtained by high-resolution mass spectrometry (HRMS), resulting in a good agreement with the measured viscosity. We also estimated the viscosity of biomass burning particles using the chemical composition measured by HRMS with two different ionization techniques: electrospray ionization (ESI) and atmospheric pressure photoionization (APPI). Due to differences in detected organic compounds and signal intensity, predicted viscosities at low RH based on ESI and APPI measurements differ by 2–5 orders of magnitude. Complementary measurements of viscosity and chemical composition are desired to further constrain RH-dependent viscosity in future studies.

Investigation of K*, Na* and Ca* flame emission during single biomass particle combustion

ABSTRACTNowadays biomass is widely used to produce electricity and heat. The growing demand for these stocks and their price results in the usage of low-quality biomass. In some cases, such biomass is mixed with herbaceous fuels and supplied to the heating plants. As such mix contains higher levels of volatile K, Na and Ca, there occurs ash-related problems such as slagging, fouling and agglomeration during combustion process.The aim of this work was to investigate the possibility to detect alkali-metals emission by chemiluminescence analysis during combustion in purpose to reduce the risk of ash-related problems. For experimental investigation, wood particle, wood pellet and wheat straw pellet were used. The chemiluminescence intensities of alkali species Na*, K* and Ca* and its variation during combustion of different biomass particle were evaluated. Results revealed that when fuel is changing during combustion, it is possible to predict the emissions of aforementioned radicals of different fuels and adjust appropriate regime of combustion.

Ubiquitous influence of wildfire emissions and secondary organic aerosol on summertime atmospheric aerosol in the forested Great Lakes region

Abstract. Long-range aerosol transport affects locations hundreds of kilometers from the point of emission, leading to distant particle sources influencing rural environments that have few major local sources. Source apportionment was conducted using real-time aerosol chemistry measurements made in July 2014 at the forested University of Michigan Biological Station near Pellston, Michigan, a site representative of the remote forested Great Lakes region. Size-resolved chemical composition of individual 0.5–2.0 µm particles was measured using an aerosol time-of-flight mass spectrometer (ATOFMS), and non-refractory aerosol mass less than 1 µm (PM1) was measured with a high-resolution aerosol mass spectrometer (HR-AMS). The field site was influenced by air masses transporting Canadian wildfire emissions and urban pollution from Milwaukee and Chicago. During wildfire-influenced periods, 0.5–2.0 µm particles were primarily aged biomass burning particles (88 % by number). These particles were heavily coated with secondary organic aerosol (SOA) formed during transport, with organics (average O∕C ratio of 0.8) contributing 89 % of the PM1 mass. During urban-influenced periods, organic carbon, elemental carbon–organic carbon, and aged biomass burning particles were identified, with inorganic secondary species (ammonium, sulfate, and nitrate) contributing 41 % of the PM1 mass, indicative of atmospheric processing. With current models underpredicting organic carbon in this region and biomass burning being the largest combustion contributor to SOA by mass, these results highlight the importance for regional chemical transport models to accurately predict the impact of long-range transported particles on air quality in the upper Midwest, United States, particularly considering increasing intensity and frequency of Canadian wildfires.

Volatization & combustion of biomass particles in random media: Mathematical modeling and analyze the effect of Lewis number

In this work, a mathematical model is proposed to model volatilization and combustion of micro organic dust particles. In contrast with previous studies, random combustion of Biomass particles (Lycopodium) and analyze the effect of different Lewis number on the combustion properties is investigated. It is assumed that flame structure is consisted of preheat or volatilization zone, reaction zone and post flame zone. Also, different Lewis numbers are applied in governing equations. For modeling random combustion, the source term in energy equation has been modeled by use of random states for volatilization of particles in preheat zone. For this regard, different groups which contains random number of particles and sense a random temperature in the preheat zone has been considered. In this analysis, the impact of random combustion, Lewis number and size of particles on the combustion properties of Biomass particles such as: burning velocity, flame temperature and effective equivalence ratio are studied. Consequently, comparison made between results obtained from random model by experimental data, showed that the random model have a better agreement with experimental data than non-random model.

Examining the chemical composition of black carbon particles from biomass burning with SP-AMS

We present laboratory measurements of the chemical speciation of black carbon particles produced from burning a series of biomass fuels during FLAME III (2009). A soot particle aerosol mass spectrometer (SP-AMS) was utilized to study the chemical composition of refractory black carbon particles and the associated nonrefractory components. We examine the effect of source fuel and combustion efficiency on the chemical composition of the emitted black carbon aerosol particles. Fifteen different source fuel types were examined. Two distinct types of black carbon spectra were observed: Low mass to charge (C1+-C5+) black carbon cluster ions were observed for all fuels while high mass to charge (>C32+) black carbon cluster ions with distinctive fullerene structure were found for turkey oak and pine species. The relative ratios between the mass concentrations of non-refractory organic species and black carbon varied between fuel types and displayed an inverse correlation with the modified combustion efficiency (MCE) of the burns. Finally, positive matrix factorization (PMF) was conducted on the SP-AMS mass spectra in order to examine the variability in the chemical composition of the observed biomass burning particles and to identify potential signatures of different fuel types.

Modification of Local Urban Aerosol Properties by Long-Range Transport of Biomass Burning Aerosol

During August 2016, a quasi-stationary high-pressure system spreading over Central and North-Eastern Europe, caused weather conditions that allowed for 24/7 observations of aerosol optical properties by using a complex multi-wavelength PollyXT lidar system with Raman, polarization and water vapour capabilities, based at the European Aerosol Research Lidar Network (EARLINET network) urban site in Warsaw, Poland. During 24–30 August 2016, the lidar-derived products (boundary layer height, aerosol optical depth, Ångström exponent, lidar ratio, depolarization ratio) were analysed in terms of air mass transport (HYSPLIT model), aerosol load (CAMS data) and type (NAAPS model) and confronted with active and passive remote sensing at the ground level (PolandAOD, AERONET, WIOS-AQ networks) and aboard satellites (SEVIRI, MODIS, CATS sensors). Optical properties for less than a day-old fresh biomass burning aerosol, advected into Warsaw’s boundary layer from over Ukraine, were compared with the properties of long-range transported 3–5 day-old aged biomass burning aerosol detected in the free troposphere over Warsaw. Analyses of temporal changes of aerosol properties within the boundary layer, revealed an increase of aerosol optical depth and Ångström exponent accompanied by an increase of surface PM10 and PM2.5. Intrusions of advected biomass burning particles into the urban boundary layer seem to affect not only the optical properties observed but also the top height of the boundary layer, by moderating its increase.

Morphologies and elemental compositions of local biomass burning particles at urban and glacier sites in southeastern Tibetan Plateau: Results from an expedition in 2010

Many studies indicate that the atmospheric environment over the southern part of the Tibetan Plateau is influenced by aged biomass burning particles that are transported over long distances from South Asia. However, our knowledge of the particles emitted locally (within the plateau region) is poor. We collected aerosol particles at four urban sites and one remote glacier site during a scientific expedition to the southeastern Tibetan Plateau in spring 2010. Weather and backward trajectory analyses indicated that the particles we collected were more likely dominated by particles emitted within the plateau. The particles were examined using an electron microscope and identified according to their sizes, shapes and elemental compositions. At three urban sites where the anthropogenic particles were produced mainly by the burning of firewood, soot aggregates were in the majority and made up >40% of the particles by number. At Lhasa, the largest city on the Tibetan Plateau, tar balls and mineral particles were also frequently observed because of the use of coal and natural gas, in addition to biofuel. In contrast, at the glacier site, large numbers of chain-like soot aggregates (~25% by number) were noted. The morphologies of these aggregates were similar to those of freshly emitted ones at the urban sites; moreover, physically or chemically processed ageing was rarely confirmed. These limited observations suggest that the biomass burning particles age slowly in the cold, dry plateau air. Anthropogenic particles emitted locally within the elevated plateau region may thus affect the environment within glaciated areas in Tibet differently than anthropogenic particles transported from South Asia.

Characteristics, Sources, and Health Risk Assessment of Trace Elements in PM10 at an Urban Site in Chengdu, Southwest China

To investigate trace element pollution of PM10 in urban Chengdu, a Southwest megacity of China, as well as to assess the human health risks caused by exposure to PM10, we analyzed ambient PM10 samples collected at an urban site in Chengdu from November, 2014 to October, 2015. The annual mean concentration of PM10 in the sampling period was 173.6 ± 77.9 µg m–3, which is 2.5 times higher than the national recommended standard of 70 µg m–3. The mean metals content in PM10 was in the following order: iron (Fe) > zinc (Zn) > titanium (Ti) > copper (Cu) > manganese (Mn) > lead (Pb) > barium (Ba) > chromium (Cr) > strontium (Si) > nickel (Ni) > arsenic (As) > vanadium (V) > antimony (Sb) > cobalt (Co) > cadmium (Cd) > bismuth (Bi). The concentration of As in PM10 was observed to be 2.9 times higher than the secondary level recommended by the China National Ambient Air Quality Standard (GB3095-2012), whereas the concentrations of other metals were within the limit. Enrichment factor analysis indicated that As, Pb, Zn, Cu, Cd, and Sb mainly originated from anthropogenic sources. Five factors were identified by positive matric factorization (PMF) model. The sources identified were soil dust (48.4%), road dust (19.4%), fossil fuel combustion (14.9%), electroplating industry (13.8%), and metallurgy industry (3.5%). Particle morphology and chemical composition analysis revealed six major particle types, namely aluminosilicate, sulfur-containing, carbon-containing, chlorine-containing, biomass burning, and metal particles. The results of the health risk assessment indicated that Cr can be carcinogenic to both children and adults, and other trace elements were determined to be below the legislation threshold (Environmental Protection Agency limit values), except for As, which was observed to be above the threshold.

Insight into the in-cloud formation of oxalate based on in situ measurement by single particle mass spectrometry

Abstract. While ground-based works suggest the significance of in-cloud production (or aqueous formation) to oxalate, direct evidence is rare. With the in situ measurements performed at a remote mountain site (1690 m above sea level) in southern China, we first reported the size-resolved mixing state of oxalate in the cloud droplet residual (cloud RES), the cloud interstitial (cloud INT), and ambient (cloud-free) particles by single particle mass spectrometry. The results support the growing evidence that in-cloud aqueous reactions promote the formation of oxalate, with ∼ 15 % of the cloud RES and cloud INT particles containing oxalate in contrast to only ∼ 5 % of the cloud-free particles. Furthermore, individual particle analysis provides unique insight into the formation of oxalate during in-cloud processing. Oxalate was predominantly (> 70 % in number) internally mixed with the aged biomass-burning particles, highlighting the impact of biomass burning on the formation of oxalate. In contrast, oxalate was underrepresented in aged elemental carbon particles, although they represented the largest fraction of the detected particles. It can be interpreted by the individual particle mixing state that the aged biomass-burning particles contained an abundance of organic components serving as precursors for oxalate. Through the analysis of the relationship between oxalate and organic acids (−45[HCO2]−, −59[CH3CO2]−, −71[C2H3CO2]−, −73[C2HO3]−), the results show that in-cloud aqueous reactions dramatically improved the conversion of organic acids to oxalate. The abundance of glyoxylate associated with the aged biomass-burning particles is a controlling factor for the in-cloud production of oxalate. Since only limited information on oxalate is available in the free troposphere, the results also provide an important reference for future understanding of the abundance, evolution, and climate impacts of oxalate.

Biomass burning particles in the Brazilian Amazon region: Mutagenic effects of nitro and oxy-PAHs and assessment of health risks.

Emissions from burning of biomass in the Amazon region have adverse effects on the environment and human health. Herein, particulate matter (PM) emitted from biomass burning in the Amazon region during two different periods, namely intense and moderate, was investigated. This study focused on: i) organic characterization of nitro- and oxy-polycyclic aromatic hydrocarbons (PAHs); ii) assessment of the excess lifetime cancer risk (LCR); and iii) assessment of the invitro mutagenic effects of extractable organic matter (EOM). Further, we compared the sensitivity of two mutagenicity tests: Salmonella/microsome test and cytokinesis-block micronucleus (CBMN) with human lung cells. Among the nitro-PAHs, 2-nitrofluoranthene, 7-nitrobenz[a]anthracene, 1-nitropyrene, and 3-nitrofluoranthene showed the highest concentrations, while among oxy-PAHs, 2-metylanthraquinone, benz[a]anthracene-7,12-dione, and 9,10-anthraquinone were the most abundant. The LCR calculated for nitro-PAH exposure during intense biomass burning period showed a major contribution of 6-nitrochrysene to human carcinogenic risk. The EOM from intense period was more mutagenic than that from moderate period for both TA98 and YG1041 Salmonella strains. The number of revertants for YG1041 was 5-50% higher than that for TA98, and the most intense responses were obtained in the absence of metabolic activation, suggesting that nitroaromatic compounds with direct-acting frameshift mutagenic activity are contributing to the DNA damage. Treatment of cells with non-cytotoxic doses of EOM resulted in an increase in micronuclei frequencies. The minimal effective dose showed that Salmonella/microsome test was considerably more sensitive in comparison with CBMN mainly for the intense burning period samples. This was the first study to assess the mutagenicity of EOM associated with PM collected in the Amazon region using Salmonella/microsome test. The presence of compounds with mutagenic effects, particularly nitro- and oxy-PAHs, and LCR values in the range of 10-5 indicate that the population is potentially exposed to an increased risk of DNA damage, mutation, and cancer.

Simulations of the effect of intensive biomass burning in July 2015 on Arctic radiative budget

The impact of biomass burning (BB) on aerosol optical properties and radiative budget in the polar region following an intense boreal fire event in North America in July 2015 is explored in this paper. Presented data are obtained from the Navy Aerosol Analysis and Prediction System (NAAPS) reanalysis and the Fu-Liou radiative transfer model. NAAPS provides particle concentrations and aerosol optical depth (AOD) at 1° x 1° spatial and 6-hourly temporal resolution, its AOD and vertical profiles were validated with field measurements for this event. Direct aerosol radiative forcings (ARF) at the surface, the top of the atmosphere (TOA) and within the atmosphere are calculated for clear-sky and all-sky conditions, with the surface albedo and cloud properties constrained by satellite retrievals. The mean ARFs at the surface, the TOA, and within the atmosphere averaged for the north pole region (latitudes north of 75.5N) and the study period (July 5–15, 2015) are −13.1 ± 2.7, 0.3 ± 2.1, and 13.4 ± 2.7 W/m2 for clear-sky and −7.3 ± 1.8, 5.0 ± 2.6, and 12.3 ± 1.6 W/m2 for all-sky conditions respectively. Local ARFs can be a several times larger e.g. the clear-sky surface and TOA ARF reach over Alaska −85 and −30 W/m2 and over Svalbard −41 and −20 W/m2 respectively. The ARF is found negative at the surface (almost zero over high albedo region though) with the maximum forcing over the BB source region, and weaker forcing under all-sky conditions compared to the clear-sky conditions. Unlike the ARFs at the surface and within the atmosphere, which have consistent forcing signs all over the polar region, the ARF at the TOA changes signs from negative (cooling) over the source region (Alaska) to positive (heating) over bright surfaces (e.g., Greenland) because of strong surface albedo effect. NAAPS simulations also show that the transported BB particle over the Arctic are in the low-to-middle troposphere and above low-level clouds, resulting in little difference in ARFs at the TOA between clear- and all-sky conditions over the regions with high surface albedo. Over dark surfaces, the negative TOA forcing increases with AOD about 50% slower under all-sky conditions compared to clear-sky case. The boreal BB event resulted in large magnitude of ARFs and the high variabilities of the forcings over the polar region has a significant impact on the polar weather conditions and important implications for the polar climate.

Distinct high molecular weight organic compound (HMW-OC) types in aerosol particles collected at a coastal urban site

Organic oligomers were discovered in laboratory-generated atmospheric aerosol over a decade ago. However, evidence for the presence of oligomers in ambient aerosols is scarce and mechanisms for their formation have yet to be fully elucidated. In this work, three unique aerosol particle types internally mixed with High molecular weight organic compounds (HMW-OC) species - likely oligomers - were detected in ambient air using single particle Aerosol Time-Of-Flight Mass Spectrometry (ATOFMS) in Cork (Ireland) during winter 2009. These particle types can be described as follows: (1) HMW-OCs rich in organic nitrogen - possibly containing nitrocatechols and nitroguaiacols - originating from primary emissions of biomass burning particles during evening times; (2) HMW-OCs internally mixed with nitric acid, occurring in stagnant conditions during night time; and (3) HMW-OCs internally mixed with sea salt, likely formed via photochemical reactions during day time. The study exemplifies the power of methodologies capable of monitoring the simultaneous formation of organic and inorganic particle-phase reaction products. Primary emissions and atmospheric aging of different types of HMW-OC contributes to aerosol with a range of acidity, hygroscopic and optical properties, which can have different impacts on climate and health.

Water uptake by fresh Indonesian peat burning particles is limited by water-soluble organic matter

Abstract. The relationship between hygroscopic properties and chemical characteristics of Indonesian biomass burning (BB) particles, which are dominantly generated from peatland fires, was investigated using a humidified tandem differential mobility analyzer. In addition to peat, acacia (a popular species at plantation) and fern (a pioneering species after disturbance by fire) were used for experiments. Fresh Indonesian peat burning particles are almost non-hygroscopic (mean hygroscopicity parameter, κ < 0.06) due to predominant contribution of water-insoluble organics. The range of κ spans from 0.02 to 0.04 (dry diameter = 100 nm, hereinafter) for Riau peat burning particles, while that for Central Kalimantan ranges from 0.05 to 0.06. Fern combustion particles are more hygroscopic (κ = 0. 08), whereas the acacia burning particles have a mediate κ value (0.04). These results suggest that κ is significantly dependent on biomass types. This variance in κ is partially determined by fractions of water-soluble organic carbon (WSOC), as demonstrated by a correlation analysis (R = 0.65). κ of water-soluble organic matter is also quantified, incorporating the 1-octanol–water partitioning method. κ values for the water extracts are high, especially for peat burning particles (A0 (a whole part of the water-soluble fraction): κ = 0.18, A1 (highly water-soluble fraction): κ = 0.30). This result stresses the importance of both the WSOC fraction and κ of the water-soluble fraction in determining the hygroscopicity of organic aerosol particles. Values of κ correlate positively (R = 0.89) with the fraction of m∕z 44 ion signal quantified using a mass spectrometric technique, demonstrating the importance of highly oxygenated organic compounds to the water uptake by Indonesian BB particles. These results provide an experimentally validated reference for hygroscopicity of organics-dominated particles, thus contributing to more accurate estimation of environmental and climatic impacts driven by Indonesian BB particles on both regional and global scales.

Temporal variations in optical and microphysical properties of mineral dust and biomass burning aerosol derived from daytime Raman lidar observations over Warsaw, Poland

In July 2013, favorable weather conditions caused a severe events of advection of biomass burning particles of Canadian forest fires to Europe. The smoke layers were widely observed, especially in Western Europe. An unusual atmospheric aerosol composition was measured at the EARLINET site in Warsaw, Central Poland, during a short event that occurred between 11 and 21 UTC on 10th July 2013. Additionally to the smoke layer, mineral dust was detected in a separate layer. The long-range dust transport pathway followed an uncommon way; originating in Western Sahara, passing above middle Atlantic, and circulating over British Islands, prior to its arrival to Poland. An effective radius of 560 nm was obtained for Saharan dust over Warsaw. This relatively small effective radius is likely due to the long time of the transport. The aerosol-polarization-Raman PollyXT-UW lidar was used for a successful daytime Raman retrieval of the aerosol optical properties at selected times during this short event. The aerosol vertical structure during the inflow over Warsaw in terms of optical properties and depolarization was analyzed, indicating clear distinction of the layers. The microphysical properties were inverted from the lidar derived optical data for selected ranges as representing the smoke and the mineral dust. For smoke, the effective radius was in the range of 0.29–0.36 μm and the complex refractive index 1.36 + 0.008i, on average. For dust, the values of 0.33–0.56 μm and 1.56 + 0.004i were obtained. An evolution of the aerosol composition over Warsaw during the day was analyzed.