Aerosol Measurements Research Articles

Horizontal distribution of tropospheric NO2 and aerosols derived by dual-scan multi-wavelength multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements in Uccle, Belgium

Abstract. Dual-scan ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of tropospheric nitrogen dioxide (NO2) and aerosols were carried out in Uccle (50.8∘ N, 4.35∘ E; Brussels region, Belgium) for 2 years from March 2018 to February 2020. The MAX-DOAS instrument operated in both UV and visible wavelength ranges in a dual-scan configuration consisting of two submodes: (1) an elevation scan in a fixed viewing azimuthal direction and (2) an azimuthal scan in a fixed low elevation angle (2∘). By analyzing the O4 and NO2 differential slant column density (dSCD) at six different wavelength intervals along every azimuthal direction and by applying a new optimal-estimation-based inversion approach (the so-called mapping MAX-DOAS technique), the horizontal distribution of the NO2 near-surface concentrations and vertical column densities (VCDs) as well as the aerosol near-surface extinction coefficients are retrieved along 10 azimuthal directions. The retrieved horizontal NO2 concentration profiles allow the identification of the main NO2 hotspots in the Brussels area. Correlative comparisons of the retrieved horizontal NO2 distribution were conducted with airborne, mobile, air quality model, and satellite datasets, and overall good agreement is found. The comparison with TROPOMI observations from operational and scientific data products reveals that the characterization of the horizontal distribution of tropospheric NO2 VCDs by ground-based measurements and an adequate a priori NO2 profile shape in TROPOMI retrievals lead to better consistency between satellite and ground-based datasets.

HazeL: A Low-Cost Learning Platform for Aerosol Measurements

HazeL: A Low-Cost Learning Platform for Aerosol Measurements

Vertical aerosol particle exchange in the marine boundary layer estimated from helicopter-borne measurements in the Azores region

Abstract. Aerosol particles are important for radiation effects, cloud formation, and therefore the climate system. A detailed understanding of the spatial distribution of aerosol particles within the atmospheric boundary layer, which depends on sources and sinks, as well as long-range transport and vertical exchange, is important. Especially in marine regions, where the climate effect of clouds is comparably high, long-range transport with subsequent vertical mixing dominates over local aerosol sources. In this study, three different methods were applied to estimate the vertical aerosol particle flux in the marine boundary layer (MBL) and the vertical exchange between the MBL and the free troposphere (FT): eddy covariance (EC), flux–gradient similarity (K theory), and the mixed-layer gradient method (MLG). For the first time, MBL aerosol fluxes derived from these three methods were compared in the framework of the “Azores Stratocumulus Measurements of Radiation, Turbulence and Aerosols” (ACORES) field campaign in the Azores region in the northeastern Atlantic Ocean in July 2017. Meteorological parameters and aerosol and cloud properties were measured in the marine troposphere using the helicopter-borne measurement platform ACTOS (Airborne Cloud Turbulence Observation System). All three methods were applied to estimate the net particle exchange between MBL and FT. In many cases, the entrainment fluxes of the MLG method agreed within the range of uncertainty with the EC and K-theory flux estimates close to the top of the MBL, while the surface flux estimates of the different methods diverged. It was not possible to measure directly above the surface with the helicopter-borne payload, which might be a source of uncertainty in the surface fluxes. The observed particle fluxes at the top of the MBL ranged from 0 to 10×106 m−2 s−1 both in the upward and the downward direction, and the associated uncertainties were on the same order of magnitude. Even though the uncertainties of all three methods are considerable, the results of this study contribute to an improved understanding of the transport of particles between the MBL and FT and their distribution in the MBL.

Retrieving ice-nucleating particle concentration and ice multiplication factors using active remote sensing validated by in situ observations

Abstract. Understanding the evolution of the ice phase within mixed-phase clouds (MPCs) is necessary to reduce uncertainties related to the cloud radiative feedback in climate projections and precipitation initiation. Both primary ice formation via ice-nucleating particles (INPs) and secondary ice production (SIP) within MPCs are unconstrained, not least because of the lack of atmospheric observations. In the past decades, advanced remote sensing methods have emerged which provide high-resolution data of aerosol and cloud properties and could be key in understanding microphysical processes on a global scale. In this study, we retrieved INP concentrations and ice multiplication factors (IMFs) in wintertime orographic clouds using active remote sensing and in situ observations obtained during the RACLETS campaign in the Swiss Alps. INP concentrations in air masses dominated by Saharan dust and continental aerosol were retrieved from a polarization Raman lidar and validated with aerosol and INP in situ observations on a mountaintop. A calibration factor of 0.0204 for the global INP parameterization by DeMott et al. (2010) is derived by comparing in situ aerosol and INP measurements, improving the INP concentration retrieval for continental aerosols. Based on combined lidar and radar measurements, the ice crystal number concentration and ice water content were retrieved and validated with balloon-borne in situ observations, which agreed with the balloon-borne in situ observations within an order of magnitude. For seven cloud cases the ice multiplication factors (IMFs), defined as the quotient of the ice crystal number concentration to the INP concentration, were calculated. The median IMF was around 80, and SIP was active (defined as IMFs > 1) nearly 85 % of the time. SIP was found to be active at all observed temperatures (−30 to −5 ∘C), with the highest IMFs between −20 and −5 ∘C. The introduced methodology could be extended to larger datasets to better understand the impact of SIP not only over the Alps but also at other locations and for other cloud types.

Seasonal Investigation of MAX-DOAS and In Situ Measurements of Aerosols and Trace Gases over Suburban Site of Megacity Shanghai, China

Shanghai has gained much attention in terms of air quality research owing to its importance to economic capital and its huge population. This study utilizes ground-based remote sensing instrument observations, namely by Multiple AXis Differential Optical Absorption Spectroscopy (MAX-DOAS), and in situ measurements from the national air quality monitoring platform for various atmospheric trace gases including Nitrogen dioxide (NO2), Sulfur dioxide (SO2), Ozone (O3), Formaldehyde (HCHO), and Particulate Matter (PM; PM10: diameter ≤ 10 µm, and PM2.5: diameter ≤ 2.5 µm) over Shanghai from June 2020 to May 2021. The results depict definite diurnal patterns and strong seasonality in HCHO, NO2, and SO2 concentrations with maximum concentrations during winter for NO2 and SO2 and in summer for HCHO. The impact of meteorology and biogenic emissions on pollutant concentrations was also studied. HCHO emissions are positively correlated with temperature, relative humidity, and the enhanced vegetation index (EVI), while both NO2 and SO2 depicted a negative correlation to all these parameters. The results from diurnal to seasonal cycles consistently suggest the mainly anthropogenic origin of NO2 and SO2, while the secondary formation from the photo-oxidation of volatile organic compounds (VOCs) and substantial contribution of biogenic emissions for HCHO. Further, the sensitivity of O3 formation to its precursor species (NOx and VOCs) was also determined by employing HCHO and NO2 as tracers. The sensitivity analysis depicted that O3 formation in Shanghai is predominantly VOC-limited except for summer, where a significant percentage of O3 formation lies in the transition regime. It is worth mentioning that seasonal variation of O3 is also categorized by maxima in summer. The interdependence of criteria pollutants (O3, SO2, NO2, and PM) was studied by employing the Pearson’s correlation coefficient, and the results suggested complex interdependence among the pollutant species in different seasons. Lastly, potential source contribution function (PSCF) analysis was performed to have an understanding of the contribution of different source areas towards atmospheric pollution. PSCF analysis indicated a strong contribution of local sources on Shanghai’s air quality compared to regional sources. This study will help policymakers and stakeholders understand the complex interactions among the atmospheric pollutants and provide a baseline for designing effective control strategies to combat air pollution in Shanghai.

Aerosol Generation During Otologic Surgery.

ObjectiveTo assess whether aerosol generation occurs during otologic surgery, to define which instruments are aerosol generating, and to identify factors that enhance safety in protection against airborne pathogens, such as severe acute respiratory syndrome coronavirus 2.Study DesignAn observational prospective study on aerosol measurements during otologic operations recorded between August and December 2020.SettingAerosol generation was measured with an Optical Particle Sizer as part of otologic operations with anesthesia. Particles with a size range of 0.3 to 10 μm were quantified. Aerosol generation was measured during otologic operations to analyze aerosols during drilling in transcanal and transmastoid operations and when using the following instruments: bipolar electrocautery, laser, suction, and cold instruments. Coughing is known to produce significant concentration of aerosols and is commonly used as a reference for high-risk aerosol generation. Thus, the operating room background concentration and coughing were chosen as reference values.PatientsThirteen otologic operations were included. The average drilling time per surgery was 27.00 minutes (range, 2.00–71.80 min).InterventionDifferent rotation speeds during drilling and other instruments were used.Main Outcome MeasuresAerosol concentrations during operations were recorded and compared with background and cough aerosol concentrations.ResultsTotal aerosol concentrations during drilling were significantly higher than background (p < 0.0001, d = 2.02) or coughing (p < 0.0001, d = 0.50). A higher drilling rotation speed was associated with higher particle concentration (p = 0.037, η2 = 0.01). Aerosol generation during bipolar electrocautery, drilling, and laser was significantly higher than with cold instruments or suction (p < 0.0001, η2 = 0.04).ConclusionHigh aerosol generation is observed during otologic surgery when drill, laser, or bipolar electrocautery is used. Aerosol generation can be reduced by using cold instruments instead of electric and keeping the suction on during aerosol-generating procedures. If drilling is required, lower rotation speeds are recommended. These measures may help reduce the spread of airborne pathogens during otologic surgery.

A quadcopter unmanned aerial system (UAS)-based methodology for measuring biomass burning emission factors

Abstract. Biomass burning (BB) emits large quantities of greenhouse gases (GHG) and aerosols that impact the climate and adversely affect human health. Although much research has focused on quantifying BB emissions on regional to global scales, field measurements of BB emission factors (EFs) are sparse, clustered and indicate high spatio-temporal variability. EFs are generally calculated from ground or aeroplane measurements with respective potential biases towards smouldering or flaming combustion products. Unmanned aerial systems (UAS) have the potential to measure BB EFs in fresh smoke, targeting different parts of the plume at relatively low cost. We propose a light-weight UAS-based method to measure EFs for carbon monoxide (CO), carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) as well as PM2.5 (TSI Sidepak AM520) and equivalent black carbon (eBC, microAeth AE51) using a combination of a sampling system with Tedlar bags which can be analysed on the ground and with airborne aerosol sensors. In this study, we address the main challenges associated with this approach: (1) the degree to which a limited number of samples is representative for the integral smoke plume and (2) the performance of the lightweight aerosol sensors. While aerosol measurements can be made continuously in a UAS set-up thanks to the lightweight analysers, the representativeness of our Tedlar bag filling approach was tested during prescribed burning experiments in the Kruger National Park, South Africa. We compared fire-averaged EFs from UAS-sampled bags for savanna fires with integrated EFs from co-located mast measurements. Both measurements matched reasonably well with linear R2 ranging from 0.81 to 0.94. Both aerosol sensors are not factory calibrated for BB particles and therefore require additional calibration. In a series of smoke chamber experiments, we compared the lightweight sensors with high-fidelity equipment to empirically determine specific calibration factors (CF) for measuring BB particles. For the PM mass concentration from a TSI Sidepak AM520, we found an optimal CF of 0.27, using a scanning mobility particle sizer and gravimetric reference methods, although the CF varied for different vegetation fuel types. Measurements of eBC from the Aethlabs AE51 aethalometer agreed well with the multi-wavelength aethalometer (AE33) (linear R2 of 0.95 at λ=880 nm) and the wavelength corrected multi-angle absorption photometer (MAAP, R2 of 0.83 measuring at λ=637 nm). However, the high variability in observed BB mass absorption cross-section (MAC) values (5.2±5.1 m2 g−1) suggested re-calibration may be required for individual fires. Overall, our results indicate that the proposed UAS set-up can obtain representative BB EFs for individual savanna fires if proper correction factors are applied and operating limitations are well understood.

Sea-air transfer of a tracer dye observed during the Tracer Release Experiment with implications for airborne contaminant exposure

Rhodamine water tracer (RWT) released during the 2021 Tracer Release Experiment in the St. Lawrence Estuary provides a proxy for the water-soluble fractions of contaminant spills. Measurements of total and size-resolved aerosols were taken onboard a research vessel throughout the experiment. Size-resolved aerosol measurements show airborne transmission of water-soluble RWT in a bimodal distribution peaking at 5.2 μm and 0.9 μm. Highest aerosol RWT (30.5 pg m−3) was observed in the 12-hour daytime period following the first dye release (Sept. 5), while the lowest (8.8 pg m−3) was observed in the subsequent nighttime sample. Available wind and RWT patch information were used to identify factors contributing to the factor-of-three variation in aerosol RWT concentrations. Negligible correlations were found between aerosol RWT and wind speed and sample time-of-day. Wind direction is isolated as the key variable for consideration in identifying the impact of contaminant spills on coastal and inland communities.

Experimental and numerical investigation on aerosols emission in musical practice and efficiency of reduction means

Early in the CoViD-19 pandemic, musical practices, especially singing and playing wind instruments, have been pointed out as having a high risk disease transmission due to aerosol production. However, characterization of these emission sources was not consolidated. This study focuses on the generation of aerosols and potential reduction in the context of playing wind instruments and singing. Aerosol concentration reduction means are evaluated using aerosol measurements in clean room and Computational Fluid Dynamics. Measurements at the bell of a clarinet and in front of singers are performed with or without a protection (bell cover for clarinet and surgical mask for singers). Numerical results on clarinet suggest that most of the supermicron (≥1μm) particles are trapped on the walls of the instruments, which act as a filter, depending on toneholes configurations (closed or opened) changing the frequency of sound produced. Experimental results are consistent since almost only submicron particles contribute to the measured number concentration during playing clarinet. First of all, the high inter and intra-individuals variability is highlighted, with high coefficients of variation. This study highlights the impact of fingerings on the generated particles and the efficiency of protections such as bell cover (from 3 to 100 times), depending on the played note and players. Results for singers show that surgical masks significantly reduce the aerosol concentration (from 8 to 170 times) in front of the mouth. The evolution of aerosol concentration is also correlated with sound intensity.

Visible, near-infrared dual-polarization lidar based on polarization cameras: system design, evaluation and atmospheric measurements.

A visible, near-infrared (VIS-NIR) dual-polarization lidar technique employing laser diodes and polarization cameras has been designed and implemented for all-day unattended field measurements of atmospheric aerosols. The linear volume depolarization ratios (LVDR) and the offset angles can be retrieved from four-directional polarized backscattering signals at wavelengths of 458 nm and 808 nm without additional optical components and sophisticated system adjustments. Evaluations on the polarization crosstalk of the polarization camera and the offset angle have been performed in detail. A rotating linear polarizer (RLP) method based on the Stokes-Mueller formalism has been proposed and demonstrated for measuring extinction ratios of the polarization camera, which can be used to eliminate the polarization crosstalk between different polarization signals. The offset angles can be online measured with a precision of 0.1°, leading to negligible measurement errors on the LVDR. One-month statistical analysis revealed a small temporal variation of the offset angles, namely -0.13°±0.07° at 458 nm and 0.33°±0.09° at 808 nm, indicating good system stability for long-term measurement. Atmospheric measurements have been carried out to verify the system performance and investigate aerosol optical properties. The spectral characteristics of the aerosol extinction coefficient, the color ratio, the linear particle polarization ratio (LPDR) and the ratio of LPDR were retrieved and evaluated based on one-month continuous atmospheric measurements, from which different types of aerosols can be classified. The promising results showed great potential of employing the VIS-NIR dual-polarization lidar in characterizing aerosol optical properties, discriminating aerosol types and analyzing long-range aerosol transportation.

Factors controlling atmospheric DMS and its oxidation products (MSA and nssSO42−) in the aerosol at Terra Nova Bay, Antarctica

Abstract. This paper presents the results of simultaneous high time-resolution measurements of biogenic aerosol (methane sulfonic acid (MSA), non-sea salt sulfate nssSO42-) with its gaseous precursor dimethylsulfide (DMS), performed at the Italian coastal base Mario Zucchelli Station (MZS) in Terra Nova Bay (MZS) during two summer campaigns (2018–2019 and 2019–2020). Data on atmospheric DMS concentration are scarce, especially in Antarctica. The DMS maximum at MZS occurs in December, one month earlier than at other Antarctic stations. The maximum of DMS concentration is connected with the phytoplanktonic senescent phase following the bloom of Phaeocystis antarctica that occurs in the polynya when sea ice opens up. The second plankton bloom occurs in January and, despite the high dimethylsufoniopropionate (DMSP) concentration in seawater, atmospheric DMS remains low, probably due to its fast biological turnover in seawater in this period. The intensity and timing of the DMS evolution during the two years suggest that only the portion of the polynya close to the sampling site produces a discernible effect on the measured DMS. The closeness to the DMS source area and the occurrence of air masses containing DMS and freshly formed oxidation products allow us to study the kinetic of biogenic aerosol formation and the reliable derivation of the branch ratio between MSA and nssSO42- from DMS oxidation that is estimated to be 0.84±0.06. Conversely, for aged air masses with low DMS content, an enrichment of nssSO42- with respect to MSA, is observed. We estimate that the mean contribution of freshly formed biogenic aerosol to PM10 is 17 % with a maximum of 56 %. The high contribution of biogenic aerosol to the total PM10 mass in summer in this area highlights the dominant role of the polynya on biogenic aerosol formation. Finally, due to the regional and year-to-year variability of DMS and related biogenic aerosol formation, we stress the need for long-term measurements of seawater and atmospheric DMS and biogenic aerosol along the Antarctic coast and in the Southern Ocean.

Practical approach for an easy determination of the limit of detection and uncertainty budget associated with on-line measurements of gas and aerosols by ion chromatography

The Monitor for Aerosols and Gases in Ambient air (MARGA) is an on-line gas and aerosol sampling and analysis system based on ion chromatography (IC) that allows the monitoring at 1-h time resolution of major water-soluble atmospheric species in the gas phase (NH3, HCl, HONO, HNO3, SO2) and the particle phase (NH4+, Na+, K+, Ca2+, Mg2+, Cl−, NO3−, SO42−). The lack of a common procedure among users to determine the LOD and the uncertainty of measurements for each species led to the comparison of four different operational approaches for the LOD determination, one manual and three automatic. This comparison highlighted the high NO3− blank values around 0.6 μg m−3 when using a HNO3-based cation eluent, so the p-TSA-based eluent was proposed instead. A model for an easy estimation of measurement uncertainties is suggested based on main sources of uncertainty (liquid sample volume, air volume, representativeness of the sample, accuracy of the internal standard preparation, chemical background, repeatability), applied to a real dataset acquired in a rural site in the North of France. It gives relative average uncertainties between 5 and 30% for NH3, HONO, HNO3, SO2, NH4+ NO3− and SO42−, while Na+, K+, Ca2+, Mg2+ and Cl− range between 45% and >100%. A comparison between our dataset and other studies confirmed that the variation of the uncertainty budget depends on environmental concentrations of the species and site typology. The practical recommendations drawn in this paper may be helpful to the user community of gas and aerosol online samplers coupled to IC analysis.

Simulating indoor inorganic aerosols of outdoor origin with the inorganic aerosol thermodynamic equilibrium model ISORROPIA.

Outdoor aerosols can transform and have their composition altered upon transport indoors. Herein, IMAGES, a platform that simulates indoor organic aerosol with the 2-dimensional volatility basis set (2D-VBS), was extended to incorporate the inorganic aerosol thermodynamic equilibrium model, ISORROPIA. The model performance was evaluated by comparing aerosol component predictions to indoor measurements from an aerosol mass spectrometer taken during the summer and winter seasons. Since ammonia was not measured in the validation dataset, outdoor ammonia was estimated from aerosol measurements using a novel pH-based algorithm, while nitric acid was held constant. Modeled indoor ammonia sources included temperature-based occupant and surface emissions. Sensitivity to the nitric acid indoor surface deposition rate was explored by varying it in model runs, which did not affect modeled sulfate due to its non-volatile nature, though the fitting of a filter efficiency was required for good correlations of modeled sulfate with measurements in both seasons. Modeled summertime nitrate well-matched measured observations when , but wintertime comparisons were poor, possibly due to missing thermodynamic processes within the heating, ventilating, and air-conditioning (HVAC) system. Ammonium was consistently overpredicted, potentially due to neglecting thirdhand smoke impacts observed in the field campaign, as well as HVAC impacts.

Interdisciplinary Perspectives on the Role of Aerosol Transmission in SARS-CoV-2 Infections

The relevance of aerosols for the transmission of the Severe Acute Respiratory Syndrome Coronavirus Type 2 (SARS-CoV-2) is still debated. However, over time, in addition to distancing and hygiene rules, aerosol physics-based measures such as wearing face masks and ventilating indoor spaces were found to be efficient in reducing infections. In an interdisciplinary workshop "Aerosol & SARS-CoV-2" of the Association for Aerosol Research (GAeF) in cooperation with the German Society for Pneumology and Respiratory Medicine (DGP), the Professional Association of General Air Technology of the VDMA, the German Society for Virology (GfV), the Health Technology Society (GG) and the International Society for Aerosols in Medicine (ISAM) under the auspices of the Robert Koch Institute (RKI) in March 2021, the need for research and coordination on this topic was addressed. Fundamental findings from the various disciplines as well as interdisciplinary perspectives on aerosol transmission of SARS-CoV-2 and infection mitigation measures are summarized here. Finally, open research questions and needs are presented.

Characterization of in-stack particulate emissions from residential wood hydronic heater appliances under different combustion conditions

ABSTRACT In the current work, we provide measurements of size-resolved particle number concentration (PNC), particle mass concentration (PMC), lung-deposited surface area (LDSA), and black carbon (BC) concentration for three biomass fired hydronic heaters during operation in four different combustion conditions. The appliances include one woodchip-fueled hydronic heater and two outdoor cordwood-fueled hydronic heaters. The operating conditions included startup, low output, high output, and burnout. Measurements were made using a custom dilution sampling system and a suite of commercially available, time-resolved, ambient aerosol measurement instrumentation. The PNC, as measured using an Dekati Electrical Low Pressure Impactor+ (ELPI), had operating condition mean values ranging between 4.1 and 52 million particles per cubic centimeter (#/cm3). The highest reported PNC occurred during the startup condition in all cases. Calculating the particle size distribution measured across each operating phase for the same instrument gave geometric mean diameters (dg ) in the range of 0.080–0.256 µm. The largest dg per appliance was nearly always attributable to the startup condition (for hydronic heater 1, startup dg ranked second). We did not observe the same trends when we transformed the ELPI PNC to PMC and particle surface area concentration estimates across operating conditions, suggesting PNC and dg are highly variable. Furthermore, simultaneous measurements of PNC, PMC, and PSAC using instrumentation with different working principles gave varying results, potentially suggesting that particles of different composition and morphology are produced under different combustion conditions.Implications: In this work we compare the results from testing of 3 biomass fired hydronic heaters including one chip-fired appliance and two cordwood-fired appliances. The emissions from these appliances were made across four operating conditions and using three different non-regulatory emissions metrics. This work: describes the difference between chip and cordwood fired units and the effect of operating condition on emissions across the three emissions metrics.

Air quality observations onboard commercial and targeted Zeppelin flights in Germany – a platform for high-resolution trace-gas and aerosol measurements within the planetary boundary layer

Abstract. A Zeppelin airship was used as a platform for in situ measurements of greenhouse gases and short-lived air pollutants within the planetary boundary layer (PBL) in Germany. A novel quantum cascade laser-based multi-compound gas analyzer (MIRO Analytical AG) was deployed to simultaneously measure in situ concentrations of greenhouse gases (CO2, N2O, H2O, and CH4) and air pollutants (CO, NO, NO2, O3, SO2, and NH3) with high precision at a measurement rate of 1 Hz. These measurements were complemented by electrochemical sensors for NO, NO2, Ox (NO2 + O3), and CO, an optical particle counter, temperature, humidity, altitude, and position monitoring. Instruments were operated remotely without the need for on-site interactions. Three 2-week campaigns were conducted in 2020 comprising commercial passenger as well as targeted flights over multiple German cities including Cologne, Mönchengladbach, Düsseldorf, Aachen, Frankfurt, but also over industrial areas and highways. Vertical profiles of trace gases were obtained during the airship landing and take-off. Diurnal variability of the Zeppelin vertical profiles was compared to measurements from ground-based monitoring stations with a focus on nitrogen oxides and ozone. We find that their variability can be explained by the increasing nocturnal boundary layer height from early morning towards midday, an increase in emissions during rush hour traffic, and the rapid photochemical activity midday. Higher altitude (250–450 m) NOx to CO ratios are further compared to the 2015 EDGAR emission inventory to find that pollutant concentrations are influenced by transportation and residential emissions as well as manufacturing industries and construction activity. Finally, we report NOx and CO concentrations from one plume transect originating from a coal power plant and compare it to the EURopean Air pollution Dispersion-Inverse Modell (EURAD-IM) model to find agreement within 15 %. However, due to the increased contribution of solar and wind energy and the impact of lockdown measures the power plant was operating at max. 50 % capacity; therefore, possible overestimation of emissions by the model cannot be excluded.

Cloud phase and macrophysical properties over the Southern Ocean during the MARCUS field campaign

Abstract. To investigate the cloud phase and macrophysical properties over the Southern Ocean (SO), the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF2) was installed on the Australian icebreaker research vessel (R/V) Aurora Australis during the Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS) field campaign (41 to 69∘ S, 60 to 160∘ E) from October 2017 to March 2018. To examine cloud properties over the midlatitude and polar regions, the study domain is separated into the northern (NSO) and southern (SSO) parts of the SO, with a demarcation line of 60∘ S. The total cloud fractions (CFs) were 77.9 %, 67.6 %, and 90.3 % for the entire domain, NSO and SSO, respectively, indicating that higher CFs were observed in the polar region. Low-level clouds and deep convective clouds are the two most common cloud types over the SO. A new method was developed to classify liquid, mixed-phase, and ice clouds in single-layered, low-level clouds (LOW), where mixed-phase clouds dominate with an occurrence frequency (Freq) of 54.5 %, while the Freqs of the liquid and ice clouds were 10.1 % (most drizzling) and 17.4 % (least drizzling). The meridional distributions of low-level cloud boundaries are nearly independent of latitude, whereas the cloud temperatures increased by ∼8 K, and atmospheric precipitable water vapor increased from ∼5 mm at 69∘ S to ∼18 mm at 43∘ S. The mean cloud liquid water paths over NSO were much larger than those over SSO. Most liquid clouds occurred over NSO, with very few over SSO, whereas more mixed-phase clouds occurred over SSO than over NSO. There were no significant differences for the ice cloud Freq between NSO and SSO. The ice particle sizes are comparable to cloud droplets and drizzle drops and well mixed in the cloud layer. These results will be valuable for advancing our understanding of the meridional and vertical distributions of clouds and can be used to improve model simulations over the SO.

Hybrid measurement of respiratory aerosol reveals a dominant coarse fraction resulting from speech that remains airborne for minutes

Accurate measurements of the size and quantity of aerosols generated by various human activities in different environments are required for efficacious mitigation strategies and accurate modeling of respiratory disease transmission. Previous studies of speech droplets, using standard aerosol instrumentation, reported very few particles larger than 5 μm. This starkly contrasts with the abundance of such particles seen in both historical slide deposition measurements and more recent light scattering observations. We have reconciled this discrepancy by developing an alternative experimental approach that addresses complications arising from nucleated condensation. Measurements reveal that a large volume fraction of speech-generated aerosol has diameters in the 5- to 20-μm range, making them sufficiently small to remain airborne for minutes, not hours. This coarse aerosol is too large to penetrate the lower respiratory tract directly, and its relevance to disease transmission is consistent with the vast majority of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) infections initiating in the upper respiratory tract. Our measurements suggest that in the absence of symptoms such as coughing or sneezing, the importance of speech-generated aerosol in the transmission of respiratory diseases is far greater than generally recognized.

The MONARCH high-resolution reanalysis of desert dust aerosol over Northern Africa, the Middle East and Europe (2007–2016)

Abstract. One of the challenges in studying desert dust aerosol along with its numerous interactions and impacts is the paucity of direct in situ measurements, particularly in the areas most affected by dust storms. Satellites typically provide column-integrated aerosol measurements, but observationally constrained continuous 3D dust fields are needed to assess dust variability, climate effects and impacts upon a variety of socio-economic sectors. Here, we present a high-resolution regional reanalysis data set of desert dust aerosols that covers Northern Africa, the Middle East and Europe along with the Mediterranean Sea and parts of central Asia and the Atlantic and Indian oceans between 2007 and 2016. The horizontal resolution is 0.1∘ latitude × 0.1∘ longitude in a rotated grid, and the temporal resolution is 3 h. The reanalysis was produced using local ensemble transform Kalman filter (LETKF) data assimilation in the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (MONARCH) developed at the Barcelona Supercomputing Center (BSC). The assimilated data are coarse-mode dust optical depth retrieved from the Moderate Resolution Imaging Spectroradiometer (MODIS) Deep Blue Level 2 products. The reanalysis data set consists of upper-air variables (dust mass concentrations and the extinction coefficient), surface variables (dust deposition and solar irradiance fields among them) and total column variables (e.g. dust optical depth and load). Some dust variables, such as concentrations and wet and dry deposition, are expressed for a binned size distribution that ranges from 0.2 to 20 µm in particle diameter. Both analysis and first-guess (analysis-initialized simulation) fields are available for the variables that are diagnosed from the state vector. A set of ensemble statistics is archived for each output variable, namely the ensemble mean, standard deviation, maximum and median. The spatial and temporal distribution of the dust fields follows well-known dust cycle features controlled by seasonal changes in meteorology and vegetation cover. The analysis is statistically closer to the assimilated retrievals than the first guess, which proves the consistency of the data assimilation method. Independent evaluation using Aerosol Robotic Network (AERONET) dust-filtered optical depth retrievals indicates that the reanalysis data set is highly accurate (mean bias = −0.05, RMSE = 0.12 and r = 0.81 when compared to retrievals from the spectral de-convolution algorithm on a 3-hourly basis). Verification statistics are broadly homogeneous in space and time with regional differences that can be partly attributed to model limitations (e.g. poor representation of small-scale emission processes), the presence of aerosols other than dust in the observations used in the evaluation and differences in the number of observations among seasons. Such a reliable high-resolution historical record of atmospheric desert dust will allow a better quantification of dust impacts upon key sectors of society and economy, including health, solar energy production and transportation. The reanalysis data set (Di Tomaso et al., 2021) is distributed via Thematic Real-time Environmental Distributed Data Services (THREDDS) at BSC and is freely available at http://hdl.handle.net/21.12146/c6d4a608-5de3-47f6-a004-67cb1d498d98 (last access: 10 June 2022).

Physical and Chemical Properties of Cloud Droplet Residuals and Aerosol Particles During the Arctic Ocean 2018 Expedition.

Detailed knowledge of the physical and chemical properties and sources of particles that form clouds is especially important in pristine areas like the Arctic, where particle concentrations are often low and observations are sparse. Here, we present in situ cloud and aerosol measurements from the central Arctic Ocean in August–September 2018 combined with air parcel source analysis. We provide direct experimental evidence that Aitken mode particles (particles with diameters ≲70 nm) significantly contribute to cloud condensation nuclei (CCN) or cloud droplet residuals, especially after the freeze‐up of the sea ice in the transition toward fall. These Aitken mode particles were associated with air that spent more time over the pack ice, while size distributions dominated by accumulation mode particles (particles with diameters ≳70 nm) showed a stronger contribution of oceanic air and slightly different source regions. This was accompanied by changes in the average chemical composition of the accumulation mode aerosol with an increased relative contribution of organic material toward fall. Addition of aerosol mass due to aqueous‐phase chemistry during in‐cloud processing was probably small over the pack ice given the fact that we observed very similar particle size distributions in both the whole‐air and cloud droplet residual data. These aerosol–cloud interaction observations provide valuable insight into the origin and physical and chemical properties of CCN over the pristine central Arctic Ocean.