Ambient Aerosol Research Articles

Unveiling the Molecular Characteristics, Origins, and Formation Mechanism of Reduced Nitrogen Organic Compounds in the Urban Atmosphere of Shanghai Using a Versatile Aerosol Concentration Enrichment System.

Reduced nitrogen-containing organic compounds (NOCs) in aerosols play a crucial role in altering their light-absorption properties, thereby impacting regional haze and climate. Due to the low concentration levels of individual NOCs in the air, the utilization of accurate detection and quantification technologies becomes essential. For the first time, this study investigated the diurnal variation, chemical characteristics, and potential formation pathways of NOCs in urban ambient aerosols in Shanghai using a versatile aerosol concentration enrichment system (VACES) coupled with HPLC-Q-TOF-MS. The results showed that NOCs accounted over 60% of identified components of urban organic aerosols, with O/N < 3 compounds being the major contributors (>70%). The predominance of the positive ionization mode suggested the prevalence of reduced NOCs. Higher relative intensities and number fractions of NOCs were observed during nighttime, while CHO compounds showed an opposite trend. Notably, a positive correlation between the intensity of NOCs and ammonium during the nighttime was observed, suggesting that the reaction of ammonium to form imines may be a potential pathway for the formation of reduced NOCs during the nighttime. Seven prevalent types of reduced NOCs in autumn and winter were identified and characterized by an enrichment of CH2 long-chain homologues. These NOCs included alkyl, cyclic, and aromatic amides in CHON compounds, as well as heterocyclic or cyclic amines and aniline homologue series in CHN compounds, which were associated with anthropogenic activities and may be capable of forming light-absorbing chromophores or posing harm to human health. The findings highlight the significant contributions of both primary emissions and ammonium chemistry, particularly amination processes, to the pollution of reduced NOCs in Shanghai's atmosphere.

Short-Term Effects of Primary and Secondary Particulate Matter on Ceramide Metabolism, Pro-Inflammatory Response, and Blood Coagulation.

Evidence of the precise biological pathway responsible for acute cardiovascular events triggered by particulate matter (PM) exposure from anthropogenic emissions is sparse. We investigated the associations of biomarkers relevant to the pathophysiology of atherothrombosis (ceramide metabolism, pro-inflammatory response, and blood coagulation) with primary and secondary components in particulate matter with aerodynamic diameters less than 2.5 μm (PM2.5). A total of 152 healthy participants were followed with four repeated clinical visits between September 2019 and January 2020 in Beijing. Exposure to ambient inorganic aerosols (sulfate, nitrate, ammonium, and chloride), as well as organic aerosols (OA) in PM2.5, was measured by a real-time aerosol chemical speciation monitor, and sources of OA were performed by positive matrix factorization. We found significant increases of 101.9-397.9% in ceramide indicators associated with interquartile-range increases in inorganic aerosols and OA prior to 72 h of exposure. Higher levels of organic and inorganic aerosols in PM2.5 were associated with increases of 3.1-6.0% in normal T cells regulated upon activation and expressed and secreted relevant to the pro-inflammatory response; increases of 276.9-541.5% were observed in D-dimers relevant to coagulation. Detrimental effects were further observed following OA exposure from fossil fuel combustion. Mediation analyses indicated that ceramide metabolism could mediate the associations of PM2.5 components with pro-inflammatory responses. Our findings expand upon the current understanding of potential pathophysiological pathways of cardiovascular events posed by ambient particulates and highlight the importance of reducing primary and secondary PM from anthropogenic combustions.

New measurements reveal a large contribution of nitrogenous molecules to ambient organic aerosol

AbstractNitrogen is a significant element that constitutes ambient organic aerosol. Individual N-containing organic molecules are known to have both natural and anthropogenic sources and implicated in a wide-ranging health and environmental effects. Yet, unlike carbon (C), the total quantity of aerosol organic nitrogen (ON) remains largely unquantified, hindering a quantitative understanding of their major sources and impacts. Here, aerosol ON is quantitatively surveyed in hundreds of aerosol filter samples collected from sites of varying urban influence in China using our recently developed method that permits simple, and yet sensitive, simultaneous detection of inorganic and organic nitrogen. Annual average ON concentration was in the range of 0.4–1.4 μg N m−3, representing 17–31% of aerosol total nitrogen. Monte Carlo simulations constrained by paired ON and OC measurements suggest N-containing organic molecules contributed typically 37–50%, with a 95% confidence interval of [12%, 94%], to ambient organic aerosols. Source apportionment analysis reveals that biomass burning and secondary formation are dominant ON sources, accounting for 21–24% and ~ 30% of ON, respectively. Primary biological aerosol is also a significant source of ON (7–18%), with its contribution more prominent in non-urban atmospheres. The results provide the quantitative data for the extent of presence of organic nitrogenous aerosol and the origin of their major sources. Such data, we anticipate, would bring forth a breakthrough in our ability to describe and model organic aerosols and to assess their environmental impacts, such as atmospheric nitrogen nutrient inputs to ecosystems.

Quantification of NOx sources contribution to ambient nitrate aerosol, uncertainty analysis and sensitivity analysis in a megacity

Dual isotopes of nitrogen and oxygen of NO3− are crucial tools for quantifying the formation pathways and precursor NOx sources contributing to atmospheric nitrate. However, further research is needed to reduce the uncertainty associated with NOx proportional contributions. The acquisition of nitrogen isotopic composition from NOx emission sources lacks regulation, and its impact on the accuracy of contribution results remains unexplored. This study identifies key influencing factors of source isotopic composition through statistical methods, based on a detailed summary of δ15N-NOx values from various sources. NOx emission sources are classified considering these factors, and representative means, standard deviations, and 95 % confidence intervals are determined using the bootstrap method. During the sampling period in Tianjin in 2022, the proportional nitrate formation pathways varied between sites. For suburban and coastal sites, the ranking was fP1(NO2 + OH radical) >fP2(N2O5 + H2O) >fP3(NO3 + DMS/HC), while the rural site exhibited similar fractional contributions from all three formation pathways. Fossil fuel NOx sources consistently contributed more than non-fossil NOx sources in each season among three sites. The uncertainties in proportional contributions varied among different sources, with coal combustion and biogenic soil emission showing lower uncertainties, suggesting more stable proportional contributions than other sources. The sensitivity analysis clearly identifies that the isotopic composition of 15N-enriched and 15N-reduced sources significantly influences source contribution results, emphasizing the importance of accurately characterizing the localized and time-efficient nitrogen isotopic composition of NOx emission sources. In conclusion, this research sheds light on the importance of addressing uncertainties in NOx proportional contributions and emphasizes the need for further exploration of nitrogen isotopic composition from NOx emission sources for accurate atmospheric nitrate studies.

Measurement report: Water diffusion in single suspended phase-separated aerosols

Abstract. Water diffusion is a typical thermodynamic process in ambient aerosols that plays pivotal roles in their physicochemical properties and atmospheric lifetime and influences the climate and human health. A fair amount of aerosols become phase-separated after experiencing atmospheric aging processes such as efflorescence, amorphization, and liquid–liquid phase separation. However, detecting the hygroscopicity of heterogeneous aerosols is quite intractable. Here, for the first time, we directly characterized the water diffusion in single suspended phase-separated aerosols via a self-constructed laser tweezer Raman spectroscopy (LTRS) system. The H2O–D2O isotope exchange was harnessed to trace the water diffusion in single laser-levitated homogenous/heterogeneous microdroplets. The time-resolved cavity-enhanced Raman spectra of the microdroplets were used to detect the diffusion process in real time. Two archetypes of phase-separated aerosols, i.e., partially engulfed and core–shell, were studied. Moreover, we quantified the dynamic water diffusion process by experimentally measuring the diffusion coefficients. The results showed that compared with the homogenous aerosols, water diffusion limitations existed in the phase-separated aerosols. The incomplete diffusion may stem from the formation of certain hydrated molecule clusters. This work provides possible implications for the evolutions, especially the gas–particle partition, of the actual phase-separated atmospheric aerosols.

Bridging New Observational Capabilities and Process-Level Simulation: Insights into Aerosol Roles in the Earth System

Abstract The spatial distribution of ambient aerosol particles significantly impacts aerosol–radiation–cloud interactions, which contribute to the largest uncertainty in global anthropogenic radiative forcing estimations. However, the atmospheric boundary layer and lower free troposphere have not been adequately sampled in terms of spatiotemporal resolution, hindering a comprehensive characterization of various atmospheric processes and impeding our understanding of the Earth system. To address this research data gap, we have leveraged the development of uncrewed aerial systems (UAS) and advanced measurement techniques to obtain mesoscale spatial data on aerosol microphysical and optical properties around the U.S. Southern Great Plains (SGP) atmospheric observatory. Our study also benefits from state-of-the-art laboratory facilities that include three-dimensional molecular imaging techniques enabled by secondary ion mass spectrometry and nanogram-level chemical composition analysis via micronebulization aerosol mass spectrometry. Through our study, we have developed a framework for observation–modeling integration, enabling an examination of how various assumptions about the organic–inorganic components mixing state, inferred from chemical analysis, affect clouds and radiation in observation-constrained model simulations. By integrating observational constraints (derived from offline chemical analysis of the aerosol surface using collected samples) with in situ UAS observations, we have identified a prominent role of organic-enriched nanometer layers located at the surface of aerosol particles in determining profiles of aerosol optical and hygroscopic properties over the SGP observatory. Furthermore, we have improved the agreement between predicted clouds and ground-based cloud lidar measurements. This UAS–model–laboratory integration exemplifies how these new advanced capabilities can significantly enhance our understanding of aerosol–radiation–cloud interactions.

Unlocking the Mystery of Aerosol Phase Transitions Governed by Relative Humidity History Through an Advanced Outdoor Nephelometer System

AbstractThis study introduces an innovative outdoor nephelometer system designed to monitor the dynamic hygroscopic behavior of aerosols in ambient air. Field measurements conducted in the Pearl River Delta region of China unveil significant roles of relative humidity (RH) swings on aerosol phase states. Highlighting the occurrence of aerosol crystallization in the afternoon followed by gradual deliquescence as RH increases, particularly when minimum afternoon RH drops below 35%, with no such behavior observed when it exceeds 40%. Emphasizing that aerosol phase states are shaped not only by RH and chemical composition but also by their RH history, illustrating that RH levels of 70% in the morning or evening may correspond to fully dissolved metastable or partially dissolved metastable states of ambient aerosols. These findings underscore the need to account for RH history when predicting aerosol phase states and have broader implications for comprehending aerosol behavior and its atmospheric impacts.

Contribution of black carbon and desert dust to aerosol absorption in the atmosphere of the Eastern Arabian Peninsula

Discriminating the absorption coefficients of aerosol mineral dust and black carbon (BC) in different aerosol size fractions is a challenge because of BC's large mass absorption cross-section compared to dust. Ambient aerosol wavelength dependent absorption coefficients (babs) in supermicron and submicron size fractions were determined with a high time resolution. The measurements were performed simultaneously using identical systems at an urban and a regional background site in Qatar. At each site, measurements were taken by co-located Aethalometers, one with a virtual impactor (VI) and the other with a PM1 cyclone to respectively collect super-micron-enhanced and submicron fractions. The combined measurement of aerosol absorption and scattering coefficients enabled the particles to be classified based on their optical properties' wavelength dependence. The classification reveals the presence of BC internally/externally mixed with different aerosols. Helium ion microscopy images provided information concerning the extent of mineral dust in the submicron fraction. The determination of absorption coefficients during dust storms and non-dust periods was used to establish the absorption Ångström exponent for dust and BC. Non-parametric wind regression, potential source contribution function and back-trajectory analysis reveal major regional sources of desert dust associated with north-westerly winds and a minor local dust contribution. In contrast, major BC sources found locally were associated with south-westerly winds with a smaller contribution made by offshore emissions transported by north-easterly and easterly winds. The use of a pair of Aethalometers with VI and PM1 inlets separates contributions of BC and dust to the aerosol absorption coefficient.

Study of secondary organic aerosol formation and aging using ambient air in an oxidation flow reactor during high pollution events over Delhi

Secondary aerosols constitute a significant fraction of atmospheric aerosols, yet our understanding of their formation mechanism and fate is very limited. In this work, the secondary organic aerosol (SOA) formation and aging of ambient air of Delhi are studied using a potential aerosol mass (PAM) reactor, an oxidation flow reactor (OFR), coupled with aerosol chemical speciation monitor (ACSM), proton transfer reaction time of flight mass spectrometer (PTR-ToF-MS), and scanning mobility particle sizer with counter (SMPS + C). The setup mimics atmospheric aging of up to several days with the generation of OH radicals. Variations in primary volatile organic compounds (VOCs) and oxygenated volatile organic compounds (OVOCs) as a function of photochemical age were investigated. Primary VOCs such as benzene, toluene, xylene, trimethyl benzene, etc. decrease and OVOCs like formic acid, formaldehyde, acetone, ethanol, etc. increase substantially upon oxidation in OFR. The highest organic aerosol (OA) enhancement was observed for the 4.2 equivalent photochemical days of aging i.e., 1.84 times the ambient concentration, and net OA loss was observed at very high OH exposure, typically after 8.4 days of photochemical aging due to heterogeneous oxidation followed by fragmentation/evaporation. In ambient air, OA enhancement is highest during nighttime due to the high concentrations of precursor VOCs in the atmosphere. SMPS + C results demonstrated substantial new particle formation upon aging and decrement in preexisting aerosol mass. This is the first experimental study conducting an in-situ evaluation of potential SOA mass generated from the ambient aerosols in India.

Contrail formation on ambient aerosol particles for aircraft with hydrogen combustion: a box model trajectory study

Abstract. Future air traffic using (green) hydrogen (H2) promises zero carbon emissions, but the effects of contrails from this new technology have hardly been investigated. We study contrail formation behind aircraft with H2 combustion by means of the particle-based Lagrangian Cloud Module (LCM) box model. Assuming the absence of soot and ultrafine volatile particle formation, contrail ice crystals form solely on atmospheric background particles mixed into the plume. While a recent study extended the original LCM with regard to the contrail formation on soot particles, we further advance the LCM to cover the contrail formation on ambient particles. For each simulation, we perform an ensemble of box model runs using the dilution along 1000 different plume trajectories. The formation threshold temperature of H2 contrails is around 10 K higher than for conventional contrails (which form behind aircraft with kerosene combustion). Then, contrail formation becomes primarily limited by the homogeneous freezing temperature of the water droplets such that contrails can form at temperatures down to around 234 K. The number of ice crystals formed varies strongly with ambient temperature even far away from the contrail formation threshold. The contrail ice crystal number clearly increases with ambient aerosol number concentration and decreases significantly for ambient particles with mean dry radii ⪅ 10 nm due to the Kelvin effect. Besides simulations with one aerosol particle ensemble, we analyze contrail formation scenarios with two co-existing aerosol particle ensembles with different mean dry sizes or hygroscopicity parameters. We compare them to scenarios with a single ensemble that is the average of the two aerosol ensembles. We find that the total ice crystal number can differ significantly between the two cases, in particular if nucleation-mode particles are involved. Due to the absence of soot particle emissions, the ice crystal number in H2 contrails is typically reduced by more than 80 %–90 % compared to conventional contrails. The contrail optical thickness is significantly reduced, and H2 contrails either become visible later than kerosene contrails or are not visible at all for low ambient particle number concentrations. On the other hand, H2 contrails can form at lower flight altitudes where conventional contrails would not form.

Quantifying the Chemical Composition and Real-Time Mass Loading of Nanoplastic Particles in the Atmosphere Using Aerosol Mass Spectrometry.

Plastic debris, including nanoplastic particles (NPPs), has emerged as an important global environmental issue due to its detrimental effects on human health, ecosystems, and climate. Atmospheric processes play an important role in the transportation and fate of plastic particles in the environment. In this study, a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was employed to establish the first online approach for identification and quantification of airborne submicrometer polystyrene (PS) NPPs from laboratory-generated and ambient aerosols. The fragmentation ion C8H8+ is identified as the major tracer ion for PS nanoplastic particles, achieving an 1-h detection limit of 4.96 ng/m3. Ambient PS NPPs measured at an urban location in Texas are quantified to be 30 ± 20 ng/m3 by applying the AMS data with a constrained positive matrix factorization (PMF) method using the multilinear engine (ME-2). Careful analysis of ambient data reveals that atmospheric PS NPPs were enhanced as air mass passed through a waste incinerator plant, suggesting that incineration of waste may serve as a source of ambient NPPs. The online quantification of NPPs achieved through this study can significantly improve our understanding of the source, transport, fate, and climate effects of atmospheric NPPs to mitigate this emerging global environmental issue.

Quantification and Characterization of Fine Plastic Particles as Considerable Components in Atmospheric Fine Particles.

The negative effects of air pollution, especially fine particulate matter (PM2.5, particles with an aerodynamic diameter of ≤2.5 μm), on human health, climate, and ecosystems are causing significant concern. Nevertheless, little is known about the contributions of emerging pollutants such as plastic particles to PM2.5 due to the lack of continuous measurements and characterization methods for atmospheric plastic particles. Here, we investigated the levels of fine plastic particles (FPPs) in PM2.5 collected in urban Shanghai at a 2 h resolution by using a novel versatile aerosol concentration enrichment system that concentrates ambient aerosols up to 10-fold. The FPPs were analyzed offline using the combination of spectroscopic and microscopic techniques that distinguished FPPs from other carbon-containing particles. The average FPP concentrations of 5.6 μg/m3 were observed, and the ratio of FPPs to PM2.5 was 13.2% in this study. The FPP sources were closely related to anthropogenic activities, which pose a potential threat to ecosystems and human health. Given the dramatic increase in plastic production over the past 70 years, this study calls for better quantification and control of FPP pollution in the atmosphere.

Evolution of nucleophilic high molecular-weight organic compounds in ambient aerosols: a case study

Abstract. Nucleophilic high molecular-weight organic compounds (HMWOCs) are sensitive to protons (H+) in Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis. A comprehensive evaluation of the diurnal evolution of nucleophilic HMWOCs was performed. HMWOCs aged significantly in daily cycles, accompanied by functionality shifts, particularly oxygenated and reduced nitrogen (CHON and CHN) as well as oxygenated organics. The intensities of high molecular-weight (HMW) oxygenated compounds increased during both daytime and nighttime. The daytime evolution produced more nitrogen-containing compounds with carboxylic group (–COOH) homologues with molecular weights greater than 300, while the nighttime evolution produced mostly small CHON compounds (molecular weights &lt; 300). During evolution, nighttime CHON removals were observed; meanwhile, carboxylation was also identified in CHON groups. The daytime evolution produced significantly more reduced-nitrogen-containing compounds; a day- and nighttime increase in CHN compounds with five members was also observed. This study can provide insights into the aging of less polar organic aerosols.

Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity

Abstract. Although air quality guidelines generally use the atmospheric concentration of fine particulate matter (PM2.5) as a metric for air pollution evaluation and management, the fact cannot be ignored that different particle toxicities are unequal and significantly related to their sources and chemical compositions. Therefore, judging the most harmful source and identifying the toxic component would be helpful for optimizing air quality standards and prioritizing targeted PM2.5 control strategies to protect public health more effectively. Since the combustions of fuels, including oil, coal, and biomass, are the main anthropogenic sources of environmental PM2.5, their discrepant contributions to health risks of mixed ambient aerosol pollution dominated by the respective emission intensity and unequal toxicity of chemical components need to be identified. In order to quantify the differences between these combustion primary emissions, 10 types of PM2.5 from each typical source group, i.e., vehicle exhaust, coal combustion, and plant biomass (domestic biofuel) burning, were collected for comparative study with toxicological mechanisms. In total, 30 types of individual combustion samples were intercompared with representative urban ambient air PM2.5 samples, whose chemical characteristics and biological effects were investigated by component analysis (carbon, metals, soluble ions) and in vitro toxicity assays (cell viability, oxidative stress, inflammatory response) of human lung adenocarcinoma epithelial cells (A549). Carbonaceous fractions were plenteous in automobile exhaust and biomass burning, while heavy metals were more plentiful in PM2.5 from coal combustion and automobile exhaust. The overall ranking of mass-normalized cytotoxicity for source-specific PM2.5 was automobile exhaust &gt; coal combustion &gt; domestic plant biomass burning &gt; ambient urban air, possibly with differential toxicity triggers, and showed that the carbonaceous fractions (organic carbon, OC; elemental carbon, EC) and redox-active transition metals (V, Ni, Cr) assisted by water-soluble ions (Ca2+, Mg2+, F−, Cl−) might play important roles in inducing cellular reactive organic species (ROS) production, causing oxidative stress and inflammation, resulting in cell injury and apoptosis, and thus damaging human health. Coupled with the source apportionment results of typical urban ambient air PM2.5 in eastern China, reducing toxic PM2.5 from these anthropogenic combustions will be greatly beneficial to public health. In addition to the air pollution control measures that have been implemented, like strengthening the vehicle emission standards, switching energy from coal to gas and electricity, and controlling the open incineration of agricultural straws, further methods could be considered, especially by preferentially reducing the diesel exhaust, lessening the coal combustion by replacement with low-ash clean coals, and depressing the rural crop straw biomass burning emissions.

Enhancing characterization of organic nitrogen components in aerosols and droplets using high-resolution aerosol mass spectrometry

Abstract. This study aims to enhance the understanding and application of the Aerodyne high-resolution aerosol mass spectrometer (HR-AMS) for the comprehensive characterization of organic nitrogen (ON) compounds in aerosol particles and atmospheric droplets. To achieve this goal, we analyzed 75 N-containing organic compounds, representing a diverse range of ambient non-organonitrate ON (NOON) types, including amines, amides, amino acids, N heterocycles, protein, and humic acids. Our results show that NOON compounds can produce significant levels of NHx+ and NOx+ ion fragments, which are typically recognized as ions representative of inorganic nitrogen species. We also identified the presence of CH2N+ at m/z = 28.0187, an ion fragment rarely quantified in ambient datasets due to substantial interference from N2+. As a result, the utilization of an updated calibration factor of 0.79 is necessary for accurate NOON quantification via the HR-AMS. We also assessed the relative ionization efficiencies (RIEs) for various NOON species and found that the average RIE for NOON compounds (1.52 ± 0.58) aligns with the commonly used default value of 1.40 for organic aerosol. Moreover, through a careful examination of the HR-AMS mass spectral features of various NOON types, we propose fingerprint ion series that can aid the NOON speciation analysis. For instance, the presence of CnH2n+2N+ ions is closely linked with amines, with CH4N+ indicating primary amines, C2H6N+ suggesting secondary amines, and C3H8N+ representing tertiary amines. CnH2nNO+ ions (especially for n values of 1–4) are very likely derived from amides. The co-existence of three ions, C2H4NO2+, C2H3NO+, and CH4NO+, serves as an indicator for the presence of amino acids. Additionally, the presence of CxHyN2+ ions indicates the occurrence of 2N-heterocyclic compounds. Notably, an elevated abundance of NH4+ is a distinct signature for amines and amino acids, as inorganic ammonium salts produce only negligible amounts of NH4+ in the HR-AMS. Finally, we quantified the NOON contents in submicron particles (PM1) and fog water in Fresno, California, and PM1 in New York City (NYC). Our results revealed the substantial presence of amino compounds in both Fresno and NYC aerosols, whereas concurrently collected fog water in Fresno contained a broader range of NOON species, including N-containing aromatic heterocycle (e.g., imidazoles) and amides. These findings highlight the significant potential of employing the widespread HR-AMS measurements of ambient aerosols and droplets to enhance our understanding of the sources, transformation processes, and environmental impacts associated with NOON compounds in the atmosphere.

Impacts of variations in aerosol refractive index on the retrieving of the light-absorption and hygroscopicity of ambient black carbon-containing aerosols using SP2

Black carbon (BC) aerosols directly influence the earth's climate system by absorbing the light intensity and indirectly by interacting with clouds. The microphysical properties of BC-containing aerosols were determined by their core diameter and shell thickness, which can be derived from the measurement of a single-particle soot photometer (SP2). Traditionally, a constant real part of the shell's refractive index (RRI) was employed to retrieve the shell thickness of BC-containing aerosols using the measured scattering signals from SP2. Recent field measurements in East China show that ambient aerosol RRI varies over a wide range between 1.36 and 1.56. The influences of aerosol RRI variation on the retrieving of BC-containing aerosol shell thickness from the measurements of SP2 are investigated with simulation studies. Results show that the variation in ambient aerosol RRI can lead to a variation in the coating thickness of BC-containing aerosols by 9.4%. The corresponding uncertainties in the light absorption enhancement reach up to 29% due to the influence of aerosol RRI. The critical mean supersaturation (SS) of the BC-containing aerosol varies significantly between 0.044% and 0.055% due to the uncertainties in the derived shell thickness using a constant RRI. This study highlights the demand for the real-time measurement of ambient aerosol RRI when deriving the microphysical properties of ambient BC-containing aerosols from the SP2 measurement.

Multi-section reference value for the analysis of horizontally scanning aerosol lidar observations

Abstract. The quantitative analysis of measurements with horizontally scanning aerosol lidar instruments faces two major challenges: the background correction can be affected by abnormal signal peaks, and the choice of a reference extinction coefficient αref is complicated if aerosols are ubiquitous in the sampled volume. Here, we present the newly developed multi-section method for the stable solution of extinction coefficient retrievals from horizontally scanning lidar measurements. The algorithm removes irregular peaks related to signal noise based on an experimentally derived fitting model. A representative value for αref is inferred from converging retrievals along different scan axes and over multiple scans of 10 to 15 min under the assumption that they are only related to ambient aerosols without distinct emission sources. Consequently, αref obtained through the multi-section method reflects typical atmospheric aerosols unaffected by emissions and noise. When comparing αref to the PM2.5 mass concentrations at national monitoring stations near the measurement area, a significant correlation with an r2 value exceeding 0.74 was observed. The presented case studies show that the new method allows for the retrieval and visualization of spatio-temporal aerosol distributions and subsequent products such as PM2.5 concentrations.

Mass spectrometric analysis of unprecedented high levels of carbonaceous aerosol particles long-range transported from wildfires in the Siberian Arctic

Abstract. Wildfires in Siberia generate large amounts of aerosols, which may be transported over long distances and pose a threat to the sensitive ecosystem of the Arctic. Particulate matter (PM) of aged wildfire plumes originating from Yakutia in August 2021 was collected in Nadym and on Bely Island (both in northwestern Siberia). An advanced analysis of the chemical composition of aerosol particles was conducted through a multi-wavelength thermal–optical carbon analyzer (TOCA) coupled to resonance-enhanced multiphoton ionization time-of-flight mass spectrometry (REMPI-TOFMS) as well as through ultra-high-resolution Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS). In Nadym, concentrations of organic carbon (OC) and elemental carbon (EC) peaked at 100 and 40 µg m−3, respectively, associated with Angström absorption exponents for 405 and 808 nm (AAE405/808) between 1.5 and 3.3. The weekly average on Bely Island peaked at 8.9 µg m−3 of OC and 0.3 µg m−3 of EC and AAE405/808 close to unity. In particular, ambient aerosol in Nadym had a distinct biomass burning profile with pyrolysis products from carbohydrates, such as cellulose and hemicellulose, as well as lignin and resinoic acids. However, temporarily higher concentrations of five- and six-ring polycyclic aromatic hydrocarbons (PAHs), different from the PAH signature of biomass burning, suggest a contribution of regional gas flaring. FT-ICR MS with electrospray ionization (ESI) revealed a complex mixture of highly functionalized compounds, containing up to 20 oxygen atoms, as well as nitrogen- and sulfur-containing moieties. Concentrations of biomass burning markers on Bely Island were substantially lower than in Nadym, flanked by the appearance of unique compounds with higher oxygen content, higher molecular weight, and lower aromaticity. Back-trajectory analysis and satellite-derived aerosol optical depth suggested long-range transport of aerosol from the center of a Yakutian wildfire plume to Nadym and from the plume periphery to Bely Island. Owing to lower aerosol concentrations in the plume periphery than in its center, it is demonstrated how dilution affects the chemical plume composition during atmospheric aging.

Enhanced light absorption by ambient brown carbon aerosols in the eastern Himalayas

This study investigates the light absorption properties of organic aerosols in PM10 collected at a high-altitude location (2700 m a.s.l.) in the eastern Himalayas from March 2019 to February 2020.

Exploratory measurements of ambient air quality in a residential area applying a diffusion charge based UFP monitor/Orientierende Messungen der Luftqualität in einem Wohngebiet mit einem auf Diffusionsaufladung basierten UFP-Monitor

In the context of the revision of the EU Ambient Air Qualitiy Directive (2008/50/EC), measurement of ultrafine particles (UFP) in ambient air is proposed and discussed. To investigate the local ambient UFP concentration (immis- sion), exploratory measurements of air pollution with UFPs were performed over several months in a residential area. The measurement device is based on charge detection of the measurement aerosol (AQ Guard Smart 2000 of the manufacturer Palas®). The background particle concentrations are within the typical background level for rural residential areas (3,000 to 5,000 cm-3). Increased UFP concentration levels were predominantly measured during the evening and the night. On 53 days of the total measurement duration of 101 days increased par- ticle concentrations above the background level (at least 6,000 cm-3) regarding the 15-minute average values were measured for at least one hour during the evening and night (16:00 to 0:00). The main source of the increased particle concentra- tion is the operation of woodstoves in the neighbourhood of the measuring location. This air pollution in the evening hours is not reflected in the context of daily or monthly averages. Other pollution sources (barbecue, new-years fireworks, traffic – different measurement location) were also identified and differences of the mean particle diameter of the ambient aerosol with regards to the background level (80 nm) could be determined. The device is suitable for UFP measurements and offers a lower detectable size-range compared to conventional scattered-light based optical particle counters.