Aerosol Measurements Research Articles

Free-tropospheric aerosols contribute to large aerosol optical depth at a remote, inland location with insignificant anthropogenic emissions

In-situ measurements of atmospheric aerosols from remote environments marked with negligible human activities are required to reduce the uncertainties associated with natural aerosols in pre-industrial climate forcings (particularly the aerosol-cloud interactions). In this study, we present long-term continuous aerosol measurements, carried out using ground-based and satellite observations, both close to the surface and in the vertical column, over a remote, rural, inland location in southern peninsular India. The near-surface aerosol concentrations were low, in general conformity to the typical pattern expected for a remote location, with the temporal changes being primarily governed by the background meteorology. However, the columnar aerosol optical depth (AOD) was surprisingly high and resembled that of a typical semi-urban continental location, with an yearly mean AOD of 0.47 ± 0.06. Spaceborne lidar observations in conjunction with ground-based radiometer measurements revealed that around 60% of this AOD was contributed by free-tropospheric aerosol layers during summer and monsoon seasons. Airmass back-trajectory analysis along with particle depolarisation ratio profiles indicate that these aerosol layers are mostly associated with long-range transported dust aerosols. Our findings indicate that benign surface concentration of aerosols at a location need not necessarily be sufficient to consider it as an optimal choice for studying background aerosols.

Optimization of the Polarized Imaging Nephelometer (PI-Neph) for continuous monitoring of multiwavelength aerosol phase functions in support of space polarimetry missions

This work deals with the set up and optimization of a commercial multiwavelength polarized imaging nephelometer (PI-Neph, Airphoton PIN100) designed to measure F11 (phase function) and –F12/F11 (polarized phase function) from ambient aerosol samples. Such measurements are critical for the success of upcoming satellite missions based on polarimetry measurements because they will support and validate retrieval techniques. The main novelty of the instrument with respect to previous versions consists of using only one beam instead of a mirror system to fold it, avoiding internal reflections of light and loss of energy within the laser beam. The instrument also includes the automatization of the imaging technique that makes possible continuous measurements in near real time of the aerosol phase functions at different states of linear polarization directly from ambient air. Laser emits at three different wavelengths (405, 515 and 660 nm) and the beam goes through a wire grid polarizer for linearly polarizing the light, followed by two liquid crystal retarders that control the state of linear polarization. The detector is a CMOS camera perpendicular to the beam which allows to obtain final phase functions in the range 5°–175° (losses of some angles by physical limitations and stray light). The calibration of the instrument is discussed and includes geometric calibration (to account for different light paths to the camera) plus absolute calibration (to obtain physical units). Temporal stability of calibrations is observed, and different data quality tests are presented in order to obtain reliable values of F11 and –F12/F11. For an automatic operation of the instrument that permits real time phase matrix measurements, a data quality check algorithm that avoids non-physical measurements and filters outliers has been developed. Validation of the scattering matrix elements based on monodisperse aerosol measurements is also done with polystyrene latex spheres (PSL), showing good agreement with Mie theory. Finally, first results of the instrument operating at the University of Granada (UGR) station from the Andalusian Global ObseRvatory of the Atmosphere (AGORA) since April 2022 are presented. Very good agreements of the integrated scattering coefficients with an integrating nephelometer (TSI, model 3563) were obtained with high correlation coefficients for the three wavelengths (R2 > 0.81). The calculated root-mean-square error (RMSE) reveals that the performance of the PI-Neph in the measurement of the scattering coefficient is better in the 660 nm and 515 nm wavelengths than in the 405 nm one, although differences between datasets are still low. The observed differences in phase functions and especially polarized phase functions (both in shape and spectral differences) under changing atmospheric scenarios (Saharan dust, pollution and background aerosol conditions) indicated that these variables are sensitive and reliable to classify the type of ambient aerosol. Particularly, the combined measurements of F11 and –F12/F11 shows a unique potential of the PI-Neph for aerosol typology.

Variability of ambient particulate matter loading at Henties Bay, Namibia

The Namibian coast is one of the areas of international interest for aerosol studies. This is due to the region’s importance for the global radiation budget because of the presence of a semi-permanent stratocumulus cloud along the coast. Aerosol particles may scatter/absorb radiation and directly influence how long clouds last by modifying their properties. This is all dependent on the particles’ chemical and physical properties because of the sources they were emitted from. In this study, we identified and investigated episodes of high (HAE) and low (LAE) PM concentrations and the meteorology that may favour their occurrence. Here, we investigated PM2.5 (particles with an aerodynamic diameter of 2.5 µm or less) and PM10 (particles with an aerodynamic diameter of 10 µm or less) at Henties Bay, Namibia. Daily aerosol measurements were taken with E-samplers between 15 and 29 July 2019. The Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model was used to investigate the long-range atmospheric transport of air masses that reached Henties Bay. The study found that during HAEs, the average PM2.5 concentration was 28.40 ± 18.10 µg/m3 and the average PM10 concentration was 68.20 ± 44.3 µg/m3. In contrast, during LAEs, the average PM2.5 concentration was 13.3 ± 9.52 µg/m3 and the average PM10 concentration was 30.00 ± 23.00 µg/m3. In both fractions, there was an observed dominant contribution from marine sources.

Site-specific dose conversion factors for radon progeny based on ambient aerosol characteristics in an outdoor environment and a tourist cave.

Site-specific Dose Conversion Factors (DCFs) for radon progeny were estimated based on the aerosol measurement results in an outdoor environment and a tourist cave. The Activity Median Diameter (AMD) and unattached fraction were measured and used to calculate the effective dose per unit intake of radon progeny. The AMDs in the outdoor environment was in the range of 0.24-0.71μm with the unattached fraction of 0.17. In the tourist cave, two peaks were found in the aerosol size distribution at nucleation and accumulation modes and the unattached fraction was measured to be 0.69 with a range of 0.36-0.85. The DCFs at the outdoor environment did not differ from those from the publication of the International Commission on Radiological Protection; however, the DCF in the tourist cave was significantly higher due to the discrepancy in the unattached fraction and the aerosol size distribution. It was found that these two factors would significantly affect the DCF so that we should be aware of it.

CAIPEEX: Indian Cloud Seeding Scientific Experiment

Abstract The demand for effective methods to augment precipitation over arid regions of India has been increasing over the past several decades as the changing climate brings warmer average temperatures. In the fourth phase of the Cloud Aerosol Interaction and Precipitation Enhancement Experiment (CAIPEEX IV), a scientific investigation was conducted over a rain-shadow region of the Western Ghats mountains in India. The primary objective was to investigate the efficacy of hygroscopic seeding in convective clouds and to develop a cloud seeding protocol. CAIPEEX IV followed the World Meteorological Organization (WMO) recommendations in a peer-reviewed report with physical, statistical, and numerical investigations. The initial results of the campaign in the monsoon period of 2018 and 2019 with two instrumented aircraft, a ground-based dual-polarization C-band radar, a network of rain gauges, radiosondes, and surface aerosol measurements are reported here. The hygroscopic seeding material was detected in cloud droplets and key cloud microphysical processes in the seeding hypothesis were tracked. The formidable challenges of assessing seeding impacts in convective clouds and the results from 150 seed and 122 no-seed samples of randomized experiments are illustrated. Over 5,000 cloud passes from the airborne campaign provided details about the convective cloud properties as the key indicators for a seeding strategy and the evaluation protocol. The experimental results suggest that cloud seeding can be approached scientifically to reduce uncertainty. The results from this study should interest the scientific community and policymakers concerned with climate change’s impact on precipitation and how to mitigate rainfall deficiencies.

Metrological traceable calibration of organic carbon and elemental carbon based on laboratory-generated reference materials

Carbonaceous aerosol, including organic carbon (OC) and elemental carbon (EC), has significant influence on human health, air quality and climate change. Accurate measurement of carbonaceous aerosol is essential to reduce the uncertainty of radiative forcing estimation and source apportionment. The accurate separation of OC and EC is controversial due to the charring of OC. Therefore, the development of reference materials (RM) for the validation of OC/EC separation is an important basis for further study. Previous RMs were mainly based on ambient air sampling, which could not provide traceability of OC and EC concentration. To develop traceable RMs with known OC/EC contents, our study applied an improved aerosol generation and mixing technique, providing uniform deposition of particles on quartz filters. To generate OC aerosol with similar pyrolytic property of ambient aerosol, both water soluble organic carbon (WSOC) and water insoluble organic carbon (WIOC) were used, and amorphous carbon was selected for EC surrogate. The RMs were analyzed using different protocols. The homogeneity within the filter was validated, reaching below 2%. The long-term stability of RMs has been validated with RSD ranged from 1.7%–3.2%. Good correlation was observed between nominal concentration of RMs with measured concentration by two protocols, while the difference of EC concentration was within 20%. The results indicated that the newly developed RMs were acceptable for the calibration of OC and EC, which could improve the accuracy of carbonaceous aerosol measurement. Moreover, the laboratory-generated EC-RMs could be suitable for the calibration of equivalent BC concentration by Aethalometers.

The impact of aerosols on stratiform clouds over southern West Africa: a large-eddy-simulation study

Abstract. Low-level stratiform clouds (LLSCs) covering a large area appear frequently during the wet monsoon season in southern West Africa. This region is also a place where different types of aerosols coexist, including biomass burning aerosols coming from central and southern Africa and aerosols emitted by local anthropogenic activities. We investigate the indirect and semi-direct effects of these aerosols on the life cycle of LLSCs by conducting a case study based on airborne and ground-based observations from the field campaign of Dynamic-Aerosol-Chemistry-Cloud-Interaction in West Africa (DACCIWA). This case is modeled using a large-eddy-simulation (LES) model with fine resolution and in situ aerosol measurements, including size distribution and chemical composition. The model has successfully reproduced the observed life cycle of the LLSC, from stratus formation to stabilization during the night and to upward development after sunrise until break-up of the cloud deck in the late afternoon. Additional sensitivity simulations using different measured aerosol profiles also suggest that aerosols can affect the cloud life cycle through both the indirect and semi-direct effects. As expected, modeled cloud microphysical features, including cloud droplet number concentration, mean radius, and thus cloud reflectivity, are all controlled by aerosol concentration. However, it is found that the variation in cloud reflectivity induced by different aerosol profiles is not always the only factor in determining the incoming solar radiation at the ground and thus for the cloud life cycle after sunrise. Instead, the difference in cloud fraction brought by dry-air entrainment from above and thus the speed of consequent evaporation – also influenced by aerosol concentration – is another important factor to consider. Clouds influenced by higher aerosol concentrations and thus with a higher number concentration and smaller sizes of cloud droplets are found to evaporate more easily and thus impose a lower cloud fraction. In addition, our sensitivity runs including versus excluding aerosol direct radiative effects have also demonstrated the impacts specifically of solar absorption by black carbon on the cloud life cycle. The semi-direct effect resulting from an excessive atmospheric heating of up to 12 K d−1 by black carbon in our modeled cases is found to lower the cloud top as well as the liquid water path, reducing surface incoming solar radiation and dry entrainment and increasing the cloud fraction.

Uncertainties in source allocation of carbonaceous aerosols in a Mediterranean region

Understanding the atmospheric processes involving carbonaceous aerosols (CAs) is crucial for assessing air pollution impacts on human health and climate. The sources and formation mechanisms of CAs are not well understood, making it challenging to quantify impacts in models. Studies suggest residential wood combustion (RWC) and traffic significantly contribute to CAs in Europe’s urban and rural areas.Here, we used an atmospheric chemistry model (MONARCH) and three different emission inventories (two versions of the European-scale emission inventory CAMS-REG_v4 and the HERMESv3 detailed national inventory for Spain) to assess the uncertainties in CAs simulation and source allocation (from traffic, RWC, shipping, fires and others) in Northeast Spain. For this, black carbon (BC) and organic aerosol (OA) measurements performed at three supersites representing different environments (urban, regional and remote) were used. Our findings show the importance of model resolution and detailed emission input data in accurately reproducing BC/OA observations. Even though emissions of total particulate matter are rather consistent between inventories in Spain, we found discrepancies between them mainly related to the spatiotemporal disaggregation (particularly relevant for traffic and RWC) and the treatment of the condensable fraction of CAs in RWC (changes in the speciation of elemental/organic carbon). The main source contribution to BC concentrations in the urban site is traffic, accounting for 71.1%/65.2% (January/July) in close agreement with the fossil contribution derived from observations (78.8%/84.2%), followed by RWC (12.8%/3%) and shipping emissions (5.4%/13.8%). An over-representation of RWC (winter) and shipping (summer) is obtained with CAMS-REG_v4. Noteworthy uncertainties arise in OA results due to condensables in emissions and a limited secondary aerosol production in the model.These findings offer insights into MONARCH’s effectiveness in simulating CAs concentrations and source contribution in Northeast Spain. The study highlights the benefits of combining new datasets and modeling techniques to refine emission inventories and better understand and mitigate air pollution impacts.

Overview and statistical analysis of boundary layer clouds and precipitation over the western North Atlantic Ocean

Abstract. Due to their fast evolution and large natural variability in macro- and microphysical properties, the accurate representation of boundary layer clouds in current climate models remains a challenge. One of the regions with large intermodel spread in the Coupled Model Intercomparison Project Phase 6 ensemble is the western North Atlantic Ocean. Here, statistically representative in situ measurements can help to develop and constrain the parameterization of clouds in global models. To this end, we performed comprehensive measurements of boundary layer clouds, aerosol, trace gases, and radiation in the western North Atlantic Ocean during the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) mission. In total, 174 research flights with 574 flight hours for cloud and precipitation measurements were performed with the HU-25 Falcon during three winter (February–March 2020, January–April 2021, and November 2021–March 2022) and three summer seasons (August–September 2020, May–June 2021, and May–June 2022). Here we present a statistical evaluation of 16 140 individual cloud events probed by the fast cloud droplet probe and the two-dimensional stereo cloud probe during 155 research flights in a representative and repetitive flight strategy allowing for robust statistical data analyses. We show that the vertical profiles of distributions of the liquid water content and the cloud droplet effective diameter (ED) increase with altitude in the marine boundary layer. Due to higher updraft speeds, higher cloud droplet number concentrations (Nliquid) were measured in winter compared to summer despite lower cloud condensation nucleus abundance. Flight cloud cover derived from statistical analysis of in situ data is reduced in summer and shows large variability. This seasonal contrast in cloud coverage is consistent with a dominance of a synoptic pattern in winter that favors conditions for the formation of stratiform clouds at the western edge of cyclones (post-cyclonic). In contrast, a dominant summer anticyclone is concomitant with the occurrence of shallow cumulus clouds and lower cloud coverage. The evaluation of boundary layer clouds and precipitation in the Nliquid ED phase space sheds light on liquid, mixed-phase, and ice cloud properties and helps to categorize the cloud data. Ice and liquid precipitation, often masked in cloud statistics by a high abundance of liquid clouds, is often observed throughout the cloud. The ACTIVATE in situ cloud measurements provide a wealth of cloud information useful for assessing airborne and satellite remote-sensing products, for global climate and weather model evaluations, and for dedicated process studies that address precipitation and aerosol–cloud interactions.

Quantifying the Viscosity of Individual Submicrometer Semisolid Particles Using Atomic Force Microscopy.

Atmospheric aerosols' viscosities can vary significantly depending on their composition, mixing states, relative humidity (RH) and temperature. The diffusion time scale of atmospheric gases into an aerosol is largely governed by its viscosity, which in turn influences heterogeneous chemistry and climate-relevant aerosol effects. Quantifying the viscosity of aerosols in the semisolid phase state is particularly important as they are prevalent in the atmosphere and have a wide range of viscosities. Currently, direct viscosity measurements of submicrometer individual atmospheric aerosols are limited, largely due to the inherent size limitations of existing experimental techniques. Herein, we present a method that utilizes atomic force microscopy (AFM) to directly quantify the viscosity of substrate-deposited individual submicrometer semisolid aerosol particles as a function of RH. The method is based on AFM force spectroscopy measurements coupled with the Kelvin-Voigt viscoelastic model. Using glucose, sucrose, and raffinose as model systems, we demonstrate the accuracy of the AFM method within the viscosity range of ∼104-107 Pa s. The method is applicable to individual particles with sizes ranging from tens of nanometers to several micrometers. Furthermore, the method does not require prior knowledge on the composition of studied particles. We anticipate future measurements utilizing the AFM method on atmospheric aerosols at various RH to aid in our understanding of the range of aerosols' viscosities, the extent of particle-to-particle viscosity variability, and how these contribute to the particle diversity observable in the atmosphere.

Dielectric barrier discharge as bipolar ion source for aerosol charging: Application to filtration, thin film, and aerosol size measurement

We have investigated the potentialities of dielectric barrier discharges (DBD) for aerosol electro-processing with a special focus on ion production and aerosol charging for deposition (filtration and materials) and aerosol measurement tools. The advantages and drawbacks of aerosol injection downstream or upstream of the discharge are compared according to the application. The main parameters that control ion production and transport are investigated based on post-discharge ion current measurements. Post-DBD aerosol chargers are compared for submicron particle size measurements based on aerosol bipolar charging and electrical mobility analysis. Finally, the principle of counterflow extraction of bipolar ion from an atmospheric pressure DBD is established from upstream measurements of positive and negative ion fluxes in air, without neither ozone (<0.1 ppmv) nor nanoparticles.

What Are the Similarities and Differences in Marine Boundary Layer Cloud and Drizzle Microphysical Properties During the ACE‐ENA and MARCUS Field Campaigns?

AbstractThis study compares macrophysical and microphysical properties of single‐layered, liquid‐dominant MBL clouds from the Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS) (above 60°S) and the ARM East North Atlantic (ENA) site during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE‐ENA) field campaign. A total of 1,136 (16.5% of clouds) and 6,034 5‐min cloud samples are selected from MARCUS and ARM ENA in this study. MARCUS clouds have higher cloud‐top heights, thicker cloud layers, larger liquid water path, and colder cloud temperatures than ENA. Thinner, warmer MBL clouds at ENA can contain higher layer‐mean liquid water content due to higher cloud and ocean surface temperatures along with greater precipitable water vapor (PWV). MARCUS has a higher drizzle frequency rate (71.8%) than ENA (45.1%). Retrieved cloud and drizzle microphysical properties from each field campaign show key differences. MARCUS clouds feature smaller cloud droplets, whereas ENA clouds have larger cloud droplets, especially at the upper region of the cloud. From cloud top to cloud base, drizzle drop sizes increase while number concentrations decrease. Drizzle drop radius and number concentration decrease from cloud base to drizzle base due to net evaporation, and MARCUS' lower specific humidity leads to a higher drizzle base than ENA. The broader surface pressure and lower tropospheric stability (LTS) distributions during MARCUS have demonstrated that there are different synoptic patterns for selected cases during MARCUS with less PWV, while ENA is dominated by high pressure systems with nearly doubled PWV.

Measurement and Modeling of Ship-Related Ultrafine Particles and Secondary Organic Aerosols in a Mediterranean Port City.

Maritime transport emerges as a major source of ultrafine particle (UFP) pollution in coastal regions with consequences for the health of people living in port cities. Inhalation of UFPs can cause inflammation and oxidative stress, which are starting points for further diseases. In addition to primary particles, secondary organic aerosol (SOA) may form through the photo-oxidation of volatile organic compounds emitted in ship exhaust. The characterization of size-segregated and chemical properties of particles is essential for assessing the health implications related to shipping. We applied a coupled regional-local chemistry transport modeling system to study the effects of ship emissions on atmospheric concentrations of UFP and SOA in the Mediterranean port city Marseille (France), which is characterized by the combination of high port activity, industrialized emissions, and active photochemistry in summer. Our results show that the average potential impact from local shipping in the port area was 6-9% for SOA and 27-51% for total particle number concentration in July 2020. The estimated oxidative potential of daily mean particulate organic matter related to shipping was lower than the oxidative potential reported for heavy fuel oil (HFO). The lower oxidative potential in this study is very likely due to the low share of ships using HFO during stopover.

Size-segregated aerosol measurements during Diwali festival in an elevated background location

Recent studies in the direction of identifying signatures of aerosol emission from fireworks stressed on the need of simultaneous measurements of mass, number and chemical compositional characteristics. Such an identification is tricky when the measurements are performed in an elevated background environment and/or in presence of an additional wide source term. This work studies the modifications in atmospheric aerosol characteristics due to firework induced emissions in Bathinda city of Punjab, North India. This study presents interpretations based on the results obtained from the measurements performed for 14 days covering the days of Diwali festival, 2021 as well as the baseline database gathered from a year-long campaign to measure mass concentration in different size-ranges. Highest mass concentration for the study duration was observed to be PM10- 382 μg/m3, PM2.5–299 μg/m3, PM1- 240 μg/m3, respectively in the month of November 2021. A clear increase of concentration was noted for Diwali days and the averaged concentration for PM10, PM2.5 and PM1 reached to 445 μg/m3, 363 μg/m3 and 304 μg/m3 on Diwali day, respectively. Number size distribution evolution analysis for the data measured from an optical particle counter (size range: 0.25–1 μm) showed that emissions for Diwali days occurred mostly at night times and in smaller size channels (<0.5 μm). Chemical compositional data of selected samples close to Diwali days was interpreted in terms of factor of increase of mass density of collected particles in different size-ranges. Mass density of elements K, Cl, S, Al, Zn, P, Mn, Pb, Br and Zr in PM1 samples was observed to be higher for Diwali days in comparison to their pre-Diwali levels. Few elements viz. Ba, Sr and Nb were found to be only present in the samples taken during Diwali days. In addition to Ba, Sr and Nb, elements V, Mg, Br and Se were observed to be present in PM2.5 and PM10 samples taken during the Diwali days. This study provides combined ambient aerosol characteristics during Diwali days when the air quality was affected by stubble burning as well.

Dust sources over the Arabian Peninsula

This study explores the characteristics of crucial dust sources and changes in their emissions over the Arabian Peninsula (AP) over the 2000–2022 period using high-resolution dust aerosol optical depth data from the Moderate Resolution Imagining Spectroradiometer (MODIS) aerosol measurements onboard Terra and Aqua platforms. The MODIS dust retrievals successfully unravel the hitherto-unexplored key dust source regions and spatial heterogeneity in dust emissions. Critically, MODIS-defined dust sources display a robust geomorphological signature. In Iraq, the Tigris and Euphrates River basins contain extensive dust sources; the Euphrates dust sources are stronger and more widespread. Localized dust sources are noticed over Syria. In the Kingdom of Saudi Arabia (KSA), the eastern province particularly facilitates extensive dust activity. Oman is the prominent dust source in the southern AP due to the presence of intruding sand dunes. Dust emissions in the Iraq and KSA regions exhibit a significant negative correlation with the Standardized Precipitation-Evapotranspiration Index, a drought index, establishing that the local droughts enhance the dust emissions in these regions. The recent sustained droughts from 2008 to 2013 caused a remarkable escalation in the dust emissions in these regions through the modification of land surface conditions.

Real-time characterization of chemical threat agent aerosols for improvement of inhalation studies

Objectives Deliberate or accidental release of chemical treat agents in the aerosol form can cause an inhalation hazard. Since the relationship between aerosol properties and health hazards is poorly understood, research into the toxicological consequences of exposure to aerosols is needed. The aim of the present study was to improve the characterization of particles for inhalation studies. Methods Several aerosol measurement technologies were compared for their potential to physically and chemically characterize particles in the inhalation size range in real-time. For that purpose, we compared the performance of an aerodynamic particle sizer (APS), a scanning mobility particle sizer (SMPS) and an electrical low-pressure impactor (ELPI) in an experimental set-up in which particles were generated by a Collison nebulizer and subsequently delivered into a nose-only inhalation exposure system. Results We found that more than 95% of the number of particles, equating to more than 83% of the mass generated by the 6-jet Collison nebulizer, were below 0.5 µm. To characterize the entire size range, the APS as single detector has only limited value, therefore the addition of supplementary instrumentation such as the SMPS or the ELPI is required. After real-time measurements in the size range of 30 nm to 10 µm, ex-situ chromatographic chemical analysis is essential for quantification of the delivered mass concentration. Conclusions In summary, the present work demonstrates the utility of the ELPI technology, in combination with off-line analysis, for characterizing aerosols with various size, shape, charge, and composition. This makes the aerosol generation and analysis suite described a promising tool for quantitative inhalation exposure studies.

Thermodynamical framework for effective mitigation of high aerosol loading in the Indo-Gangetic Plain during winter

The Indo-Gangetic Plain (IGP) experiences severe air pollution every winter, with ammonium chloride and ammonium nitrate as the major inorganic fractions of fine aerosols. Many past attempts to tackle air pollution in the IGP were inadequate, as they targeted a subset of the primary pollutants in an environment where the majority of the particulate matter burden is secondary in nature. Here, we provide new mechanistic insight into aerosol mitigation by integrating the ISORROPIA-II thermodynamical model with high-resolution simultaneous measurements of precursor gases and aerosols. A mathematical framework is explored to investigate the complex interaction between hydrochloric acid (HCl), nitrogen oxides (NOx), ammonia (NH3), and aerosol liquid water content (ALWC). Aerosol acidity (pH) and ALWC emerge as governing factors that modulate the gas-to-particle phase partitioning and mass loading of fine aerosols. Six "sensitivity regimes" were defined, where PM1 and PM2.5 fall in the "HCl and HNO3 sensitive regime", emphasizing that HCl and HNO3 reductions would be the most effective pathway for aerosol mitigation in the IGP, which is ammonia-rich during winter. This study provides evidence that precursor abatement for aerosol mitigation should not be based on their descending mass concentrations but instead on their sensitivity to high aerosol loading.

Airborne Bioaerosol Observations Imply a Strong Terrestrial Source in the Summertime Arctic

AbstractPrimary biological aerosol (PBA) is a component of coarse mode aerosol which may affect climate and health. The possible climate impacts arise from interactions between PBA and water vapor, especially since some PBA nucleate ice at warm temperatures. The health impacts span from seasonal allergies to transmission of pathogens. Despite their potential importance, the emissions, transport, and atmospheric distribution of PBA are poorly understood, especially at high latitudes where cloud effects could be pronounced. Here we report summertime measurements of fluorescent aerosol (a proxy for PBA) over the Bering and Chukchi Seas using a Wide‐Band Integrated Bioaerosol Sensor aboard a Twin Otter, alongside a lidar which detected water column productivity. Most observations occurred at 300 m over the ocean with periodic excursions to 60 and 900 m. Loadings were always low in the marine boundary layer, despite the presence of subsurface plankton layers and in contrast to other recent reports, likely indicating low oceanic emissions during our study. Large variability was observed in PBA aloft, with higher concentrations approaching those observed over the Continental US. Back trajectory analysis showed that high loadings were associated with recent transit through the continental boundary layer and we estimate PBA emissions from the Arctic tundra of up to 300 m−2 s−1 at the warmest observed temperatures. On days with strong transport from land (∼50% of our flights), PBA accounts for 12% of supermicron number and 64% of supermicron volume, indicating potentially significant effects on the albedo, glaciation and lifetime of Arctic clouds.

Suitability of Low-Cost Sensors for Submicron Aerosol Particle Measurement

The measurement and assessment of indoor air quality in terms of respirable particulate constituents is relevant, especially in light of the COVID-19 pandemic and associated infection events. To analyze indoor infectious potential and to develop customized hygiene concepts, the measurement monitoring of the anthropogenic aerosol spreading is necessary. For indoor aerosol measurements usually standard lab equipment is used. However, these devices are time-consuming, expensive and unwieldy. The idea is to replace this standard laboratory equipment with low-cost sensors widely used for monitoring fine dust (particulate matter—PM). Due to the low acquisition costs, many sensors can be used to determine the aerosol load, even in large rooms. Thus, the aim of this work is to verify the measurement capability of low-cost sensors. For this purpose, two different models of low-cost sensors are compared with established laboratory measuring instruments. The study was performed with artificially prepared NaCl aerosols with a well-defined size and morphology. In addition, the influence of the relative humidity, which can vary significantly indoors, on the measurement capability of the low-cost sensors is investigated. For this purpose, a heating stage was developed and tested. The results show a discrepancy in measurement capability between low-cost sensors and laboratory measuring instruments. This difference can be attributed to the partially different measuring method, as well as the different measuring particle size ranges. The determined measurement accuracy is nevertheless good, considering the compactness and the acquisition price of the low-cost sensors.

Aging of biomass burning emissions in the Indo-Gangetic Plain outflow: Implications for black carbon light-absorption enhancement

Recent studies worldwide have demonstrated that coating on atmospheric black carbon (BC) aerosol enhances its absorption potential. However, studies quantifying the light-absorption enhancement (Eabs) of BC are extremely limited over the Indian region. The northwestern Indo-Gangetic Plain (IGP) region witnesses annual episodes of substantial crop-residue burning during the post-monsoon season (PoMS), which has been attracting wide attention due to its impact on regional air quality and aerosol characteristics. Chemical aging of these biomass burning (BB) emissions occurs during its long-range transport across the IGP by the weak westerlies, and such atmospheric processing affects their chemical, optical, and radiative properties over downwind locations. This study examines the impact of atmospheric aging of biomass burning emissions on BC light-absorption enhancement (Eabs) using extensive, simultaneous measurements of single particle refractory BC and near-real-time mass spectrometry measurements of non-refractory submicron aerosols from an IGP outflow site. It was observed that organics were the dominant submicron aerosol species, and positive matrix factorization analysis of the organics mass spectra suggested that a large fraction of organics (64%) was secondary in nature. The BC particles in the IGP outflow (mass median diameter ∼ 0.18 ± 0.01 μm) were found to be thickly coated with volume-weighted bulk relative coating thickness in the range of 1.3–1.8. The evolution of biomass-burning organic aerosols (BBOA) indicated the presence of significant amounts of aged BBOA during the PoMS. Further, the oxidation products from the evolution of BB emissions contributed to enhanced coatings (∼ 30–70%) on BC. Mie core-shell theory calculations were then used to assess the changes in BC light absorption characteristics due to the coating of non-refractory mass on its cores. It was found that thick coatings on BC led to significant light-absorption enhancement (Eabs) (bulk Eabs in the range of 1.14–1.94 at 550 nm, depending on the extent of coating). Increased Eabs values of ≥1.8 were seen when the coating on BC exceeded 60% of its core size. The modeled bulk Eabs at 550 nm depicted a better association with highly oxidized secondary organic aerosols (SOA) than sulfate among the secondary aerosol species, suggesting an SOA-dominant regime. The present findings suggest that the critical impact of the aging of BC and co-emitted species from widespread BB emissions in the IGP outflow should be considered when evaluating the regional radiative implications.