Aerosol Measurements Research Articles

Grid-independent high-resolution dust emissions (v1.0) for chemical transport models: application to GEOS-Chem (12.5.0)

Abstract. The nonlinear dependence of the dust saltation process on wind speed poses a challenge for models of varying resolutions. This challenge is of particular relevance for the next generation of chemical transport models with nimble capability for multiple resolutions. We develop and apply a method to harmonize dust emissions across simulations of different resolutions by generating offline grid-independent dust emissions driven by native high-resolution meteorological fields. We implement into the GEOS-Chem chemical transport model a high-resolution dust source function to generate updated offline dust emissions. These updated offline dust emissions based on high-resolution meteorological fields strengthen dust emissions over relatively weak dust source regions, such as in southern South America, southern Africa and the southwestern United States. Identification of an appropriate dust emission strength is facilitated by the resolution independence of offline emissions. We find that the performance of simulated aerosol optical depth (AOD) versus measurements from the AERONET network and satellite remote sensing improves significantly when using the updated offline dust emissions with the total global annual dust emission strength of 2000 Tg yr−1 rather than the standard online emissions in GEOS-Chem. The updated simulation also better represents in situ measurements from a global climatology. The offline high-resolution dust emissions are easily implemented in chemical transport models. The source code and global offline high-resolution dust emission inventory are publicly available.

Atmospheric Carbon and Transport - America (ACT-America) Data Sets: Description, Management, and Delivery.

The ACT‐America project is a NASA Earth Venture Suborbital‐2 mission designed to study the transport and fluxes of greenhouse gases. The open and freely available ACT‐America data sets provide airborne in situ measurements of atmospheric carbon dioxide, methane, trace gases, aerosols, clouds, and meteorological properties, airborne remote sensing measurements of aerosol backscatter, atmospheric boundary layer height and columnar content of atmospheric carbon dioxide, tower‐based measurements, and modeled atmospheric mole fractions and regional carbon fluxes of greenhouse gases over the Central and Eastern United States. We conducted 121 research flights during five campaigns in four seasons during 2016–2019 over three regions of the US (Mid‐Atlantic, Midwest and South) using two NASA research aircraft (B‐200 and C‐130). We performed three flight patterns (fair weather, frontal crossings, and OCO‐2 underflights) and collected more than 1,140 h of airborne measurements via level‐leg flights in the atmospheric boundary layer, lower, and upper free troposphere and vertical profiles spanning these altitudes. We also merged various airborne in situ measurements onto a common standard sampling interval, which brings coherence to the data, creates geolocated data products, and makes it much easier for the users to perform holistic analysis of the ACT‐America data products. Here, we report on detailed information of data sets collected, the workflow for data sets including storage and processing of the quality controlled and quality assured harmonized observations, and their archival and formatting for users. Finally, we provide some important information on the dissemination of data products including metadata and highlights of applications of ACT‐America data sets.

Aerosol Generation in Ear Canal and Air‐Fluid Interface Suction

ObjectiveThe identification of aerosol-generating procedures (AGPs) is important during the current SARS-CoV-2 pandemic due to aerosol-mediated virus transmission. Aerosol measurement during clinical procedures using particle counting may be confounded by variable natural background aerosol levels or limited by partial volume sampling. The study objective was to quantify any significant aerosol generated from simulated suction clearance procedures.Study DesignProspective quantification of aerosol generation during clinical suction simulation.SettingClean chamber.MethodsWe created a clean environment for particle counting in a transparent neutralized polypropylene chamber. Air was passed through a HEPA 14 class filter to maintain a constant chamber inlet pressure. An optical particle counter was connected in line to the chamber exhaust vent to measure all of the vented particles. The chamber background count was 1 particle ≥0.3 µm per 15 minutes at a flow rate of 1 chamber air change per minute. We used this system to quantify very low aerosol counts generated from suction clearance of a silicone ear canal and at an open air-fluid interface.ResultsNo clinically significant aerosol generation was found by particle counting of the whole chamber air volume during simulated suction procedures.ConclusionSimulated ear suction clearance and air-fluid interface suction does not generate any significant aerosol. It appears likely that any aerosol potentially generated at the suction tube tip is entrained by incoming air flow. This is the first study to quantify aerosols generated by suction in a controlled environment; further research is required to determine its clinical implications.

The aftermath of COVID-19 pandemic: Rhino-orbital mucormycosis.

The aftermath of COVID-19 pandemic: Rhino-orbital mucormycosis.

Large seasonal and interannual variations of biogenic sulfur compounds in the Arctic atmosphere (Svalbard; 78.9° N, 11.9° E)

Abstract. Seasonal to interannual variations in the concentrations of sulfur aerosols (< 2.5 µm in diameter; non sea-salt sulfate: NSS-SO42-; anthropogenic sulfate: Anth-SO42-; biogenic sulfate: Bio-SO42-; methanesulfonic acid: MSA) in the Arctic atmosphere were investigated using measurements of the chemical composition of aerosols collected at Ny-Ålesund, Svalbard (78.9∘ N, 11.9∘ E) from 2015 to 2019. In all measurement years the concentration of NSS-SO42- was highest during the pre-bloom period and rapidly decreased towards summer. During the pre-bloom period we found a strong correlation between NSS-SO42- (sum of Anth-SO42- and Bio-SO42-) and Anth-SO42-. This was because more than 50 % of the NSS-SO42- measured during this period was Anth-SO42-, which originated in northern Europe and was subsequently transported to the Arctic in Arctic haze. Unexpected increases in the concentration of Bio-SO42- aerosols (an oxidation product of dimethylsulfide: DMS) were occasionally found during the pre-bloom period. These probably originated in regions to the south (the North Atlantic Ocean and the Norwegian Sea) rather than in ocean areas in the proximity of Ny-Ålesund. Another oxidation product of DMS is MSA, and the ratio of MSA to Bio-SO42- is extensively used to estimate the total amount of DMS-derived aerosol particles in remote marine environments. The concentration of MSA during the pre-bloom period remained low, primarily because of the greater loss of MSA relative to Bio-SO42- and the suppression of condensation of gaseous MSA onto particles already present in air masses being transported northwards from distant ocean source regions (existing particles). In addition, the low light intensity during the pre-bloom period resulted in a low concentration of photochemically activated oxidant species including OH radicals and BrO; these conditions favored the oxidation pathway of DMS to Bio-SO42- rather than to MSA, which acted to lower the MSA concentration at Ny-Ålesund. The concentration of MSA peaked in May or June and was positively correlated with phytoplankton biomass in the Greenland and Barents seas around Svalbard. As a result, the mean ratio of MSA to the DMS-derived aerosols was low (0.09 ± 0.07) in the pre-bloom period but high (0.32 ± 0.15) in the bloom and post-bloom periods. There was large interannual variability in the ratio of MSA to Bio-SO42- (i.e., 0.24 ± 0.11 in 2017, 0.40 ± 0.14 in 2018, and 0.36 ± 0.14 in 2019) during the bloom and post-bloom periods. This was probably associated with changes in the chemical properties of existing particles, biological activities surrounding the observation site, and air mass transport patterns. Our results indicate that MSA is not a conservative tracer for predicting DMS-derived particles, and the contribution of MSA to the growth of newly formed particles may be much larger during the bloom and post-bloom periods than during the pre-bloom period.

Aerosol Layering in the Free Troposphere over the Industrial City of Raciborz in Southwest Poland and Its Influence on Surface UV Radiation

Atmospheric aerosol and ultraviolet index (UVI) measurements performed in Racibórz (50.08° N, 18.19° E) were analyzed for the period June–September 2019. Results of the following observations were taken into account: columnar characteristics of the aerosols (aerosol thickness, Angstrom exponent, single scattering albedo, asymmetry factor) obtained from standard CIMEL sun-photometer observations and parameters of aerosol layers (ALs) in the free troposphere (the number of layers and altitudes of the base and top) derived from continuous monitoring by a CHM-15k ceilometer. Three categories of ALs were defined: residues from the daily evolution of the planetary boundary layer (PBL) aerosols, from the PBL-adjacent layer, and from the elevated layer above the PBL. Total column ozone measurements taken by the Ozone-Monitoring Instrument on board NASA’s Aura satellite completed the list of variables used to model UVI variability under clear-sky conditions. The aim was to present a hybrid model (radiative transfer model combined with a regression model) for determining ALs’ impact on the observed UVI series. First, a radiative transfer model, the Tropospheric Ultraviolet–Visible (TUV) model, which uses typical columnar characteristics to describe UV attenuation in the atmosphere, was applied to calculate hypothetical surface UVI values under clear-sky conditions. These modeled values were used to normalize the measured UVI data obtained during cloudless conditions. Next, a regression of the normalized UVI values was made using the AL characteristics. Random forest (RF) regression was chosen to search for an AL signal in the measured data. This explained about 55% of the variance in the normalized UVI series under clear-sky conditions. Finally, the UVI values were calculated as the product of the RF regression and the relevant UVIs by the columnar TUV model. The root mean square error and mean absolute error of the hybrid model were 1.86% and 1.25%, respectively, about 1 percentage point lower than corresponding values derived from the columnar TUV model. The 5th–95th percentile ranges of the observation/model differences were [−2.5%, 2.8%] and [−3.0%, 5.3%] for the hybrid model and columnar TUV model, respectively. Therefore, the impact of ALs on measured surface UV radiation could be demonstrated using the proposed AL characteristics. The statistical analysis of the UVI differences between the models allowed us to identify specific AL configuration responsible for these differences.

Strategies to minimize SARS-CoV-2 transmission in classroom settings: combined impacts of ventilation and mask effective filtration efficiency

Strong evidence exists indicating that aerosol transmission of the novel coronavirus SARS-CoV-2 is a significant transmission modality. We experimentally evaluated the impact of ventilation on aerosol dynamics and distribution along with the effective filtration efficiency (EFE) of four different mask types, with and without mask fitters, in a classroom setting. These were used to estimate aerosol conditional infection probability using the Wells–Riley model for three scenarios with different ventilation and mask interventions. Aerosol measurements confirmed that aerosol in the room was uniform within a factor of 2 for distances >2 m from the source. Mask EFE results demonstrate that most masks fit poorly with estimated leakage rates typically >50%. However, EFEs approaching the mask material FE were achievable using mask fitters. Infection probability estimates indicate that ventilation alone is not able to achieve probabilities <0.01 (1%). The use of moderate to high EFE masks reduces infection probability, >5× in some cases. Reductions provided by ventilation and masks are synergistic and multiplicative. The results reinforce the use of properly donned masks to achieve reduced aerosol transmission of SARS-CoV-2 and other infectious diseases and motivate improvements in the EFE of masks through improved design or use of mask fitters.

Summer aerosol measurements over the East Antarctic seasonal ice zone

Abstract. Aerosol measurements over the Southern Ocean have been identified as critical to an improved understanding of aerosol–radiation and aerosol–cloud interactions, as there currently exists significant discrepancies between model results and measurements in this region. The atmosphere above the Southern Ocean provides crucial insight into an aerosol regime relatively free from anthropogenic influence, yet its remoteness ensures atmospheric measurements are relatively rare. Here we present observations from the Polar Cell Aerosol Nucleation (PCAN) campaign, hosted aboard the RV Investigator during a summer (January–March) 2017 voyage from Hobart, Australia, to the East Antarctic seasonal sea ice zone. A median particle number concentration (condensation nuclei &gt; 3 nm; CN3) of 354 (95 % CI 345–363) cm−3 was observed from the voyage. Median cloud condensation nuclei (CCN) concentrations were 167 (95 % CI 158–176) cm−3. Measured particle size distributions suggested that aerosol populations had undergone significant cloud processing. To understand the variability in aerosol observations, measurements were classified by meteorological variables. Wind direction and absolute humidity were used to identify different air masses, and aerosol measurements were compared based on these identifications. CN3 concentrations measured during SE wind directions (median 594 cm−3) were higher than those measured during wind directions from the NW (median 265 cm−3). Increased frequency of measurements from these wind directions suggests the influence of large-scale atmospheric transport mechanisms on the local aerosol population in the boundary layer of the East Antarctic seasonal ice zone. Modelled back trajectories imply different air mass histories for each measurement group, supporting this suggestion. CN3 and CCN concentrations were higher during periods where the absolute humidity was less than 4.3 gH2O/m3, indicative of free tropospheric or Antarctic continental air masses, compared to other periods of the voyage. Increased aerosol concentration in air masses originating close to the Antarctic coastline have been observed in numerous other studies. However, the smaller changes observed in the present analyses suggest seasonal differences in atmospheric circulation, including lesser impact of synoptic low-pressure systems in summer. Further measurements in the region are required before a more comprehensive picture of atmospheric circulation in this region can be captured and its influence on local aerosol populations understood.

Radiocarbon in the atmospheric gases and PM10 aerosol around the Paks Nuclear Power Plant, Hungary

Our study shows a one-year-long, monthly integrated continuous monitoring campaign of gaseous radiocarbon emission and ambient air compared with 4 event-like, weekly (168 h) atmospheric aerosol radiocarbon data in every season of 2019, at 4 locations (n = 16 aerosol sample) around the Paks Nuclear Power Plant, Hungary. The study shows the first aerosol radiocarbon results around a nuclear power plant measured by accelerator mass spectrometry in Hungary. There was no dominant contribution detected in the atmospheric CO2 gas fraction, but we could detect excess radiocarbon in the total gaseous carbon fraction at almost every sampling point around the Paks Nuclear Power Plant. The highest Δ14C value in the total gaseous carbon form was 157.9 ± 4.6‰ in November and the highest Δ 14C value in the CO2 fraction was 86.1 ± 4.0‰ in December during 2019. Observed 14C activity excess is not higher than previously published values around the Paks Nuclear Power plant at the same sampling points (Molnár et al., 2007; Varga et al., 2020). Our aerosol radiocarbon measurements show that there is no significant contribution from the nuclear power plant to the atmospheric PM10 fraction. We could not detect a Δ 14C value higher than 0‰ in any season. The results show that the simple aerosol sampling, without pre-treatment of the filters, is appropriate for the measurement of excess radiocarbon at the vicinity of nuclear power plants. The applied preparation and measurement method can be applicable for detection of hot (14C) particles and early identification of radiocarbon emission from nuclear power plants in the PM10 fraction.

A long-term study of cloud residuals from low-level Arctic clouds

Abstract. To constrain uncertainties in radiative forcings associated with aerosol–cloud interactions, improved understanding of Arctic cloud formation is required, yet long-term measurements of the relevant cloud and aerosol properties remain sparse. We present the first long-term study of cloud residuals, i.e. particles that were involved in cloud formation and cloud processes, in Arctic low-level clouds measured at Zeppelin Observatory, Svalbard. To continuously sample cloud droplets and ice crystals and separate them from non-activated aerosol, a ground-based counter-flow virtual impactor inlet system (GCVI) was used. A detailed evaluation of the GCVI measurements, using concurrent cloud particle size distributions, meteorological parameters, and aerosol measurements, is presented for both warm and cold clouds, and the potential contribution of sampling artefacts is discussed in detail. We find an excellent agreement of the GCVI sampling efficiency of liquid clouds using two independent approaches. The 2-year data set of cloud residual size distributions and number concentrations reveals that the cloud residuals follow the typical seasonal cycle of Arctic aerosol, with a maximum concentration in spring and summer and a minimum concentration in the late autumn and winter months. We observed average activation diameters in the range of 58–78 nm for updraught velocities below 1 m s−1. A cluster analysis also revealed cloud residual size distributions that were dominated by Aitken mode particles down to around 20–30 nm. During the winter months, some of these small particles may be the result of ice, snow, or ice crystal shattering artefacts in the GCVI inlet; however, cloud residuals down to 20 nm in size were also observed during conditions when artefacts are less likely.

Urban aerosol size distributions: a global perspective

Abstract. Urban aerosol measurements are necessary to establish associations between air pollution and human health outcomes and to evaluate the efficacy of air quality legislation and emissions standards. The measurement of urban aerosol particle size distributions (PSDs) is of particular importance as they enable characterization of size-dependent processes that govern a particle's transport, transformation, and fate in the urban atmosphere. PSDs also improve our ability to link air pollution to health effects through evaluation of particle deposition in the respiratory system and inhalation toxicity. To inform future measurements of urban aerosol observations, this paper reviews and critically analyzes the current state of knowledge on urban aerosol PSD measurements by synthesizing 737 PSD observations made between 1998 to 2017 in 114 cities in 43 countries around the globe. Significant variations in the shape and magnitude of urban aerosol number and mass PSDs were identified among different geographical regions. In general, number PSDs in Europe (EU) and North America, Australia, and New Zealand (NAAN) are dominated by nucleation- and Aitken-mode particles. PSDs in Central, South, and Southeast Asia (CSSA) and East Asia (EA) are shifted to larger sizes, with a meaningful contribution from the accumulation mode. Urban mass PSDs are typically bimodal, presenting a dominant mode in the accumulation mode and a secondary mode in the coarse mode. Most PSD observations published in the literature are short-term, with only 14 % providing data for longer than 6 months. There is a paucity of PSDs measured in Africa (AF), CSSA, Latin America (LA), and West Asia (WA), demonstrating the need for long-term aerosol measurements across wide size ranges in many cities around the globe. Geographical variations in urban aerosol effective densities were also reviewed. Size-resolved urban aerosol effective density functions from 3 to 10 000 nm were established for different geographical regions and intra-city sampling locations in order to accurately translate number PSDs to mass PSDs, with significant variations observed between near-road and urban background sites. The results of this study demonstrate that global initiatives are urgently needed to develop infrastructure for routine and long-term monitoring of urban aerosol PSDs spanning the nucleation to coarse mode. Doing so will advance our understanding of spatiotemporal trends in urban PSDs throughout the world and provide a foundation to more reliably elucidate the impact of urban aerosols on atmospheric processes, human health, and climate.

Novel measurement system for respiratory aerosols and droplets in indoor environments.

The SARS‐CoV‐2 pandemic has created a great demand for a better understanding of the spread of viruses in indoor environments. A novel measurement system consisting of one portable aerosol‐emitting mannequin (emitter) and a number of portable aerosol‐absorbing mannequins (recipients) was developed that can measure the spread of aerosols and droplets that potentially contain infectious viruses. The emission of the virus from a human is simulated by using tracer particles solved in water. The recipients inhale the aerosols and droplets and quantify the level of solved tracer particles in their artificial lungs simultaneously over time. The mobile system can be arranged in a large variety of spreading scenarios in indoor environments and allows for quantification of the infection probability due to airborne virus spreading. This study shows the accuracy of the new measurement system and its ability to compare aerosol reduction measures such as regular ventilation or the use of a room air purifier.

Persistence of Primary and Secondary Pollutants in Delhi: Concentrations and Composition from 2017 through the COVID Pandemic

We assess impacts of the 2020 COVID-19 lockdown on ambient air quality in Delhi, building on over three years of real-time measurements of black carbon (BC) and nonrefractory submicrometer aerosol (NR-PM1) composition from the Delhi Aerosol Supersite and public data from the regulatory monitoring network. We performed source apportionment of organic aerosol (OA) and robust statistical analyses to differentiate lockdown-related impacts from baseline seasonal and interannual variability. The primary pollutants NOx, CO, and BC were most reduced, primarily due to lower transportation emissions. Local and regional emissions such as agricultural burning decreased during the lockdown. PM2.5 declined but remained well above WHO guidelines. Despite the lockdown, NR-PM1 changed only moderately compared to prior years. Differences in the trends of hydrocarbon-like OA and BC suggest that some sources of primary aerosol may have increased. Despite notable reductions in some primary pollutants, the lockdown restrictions led to rather small perturbations in the primary fraction of NR-PM1, with secondary aerosol continuing to dominate. Overall, our results demonstrate the impact of secondary and primary pollution on Delhi's air quality and show that large changes in emissions within Delhi alone are insufficient to bring about needed improvements in air quality. © 2021 American Chemical Society.

COVID-19: measurement of viral aerosols during use of supraglottic airway device.

COVID-19: measurement of viral aerosols during use of supraglottic airway device.

Aerosol above-cloud direct radiative effect and properties in the Namibian region during the AErosol, RadiatiOn, and CLOuds in southern Africa (AEROCLO-sA) field campaign – Multi-Viewing, Multi-Channel, Multi-Polarization (3MI) airborne simulator and sun photometer measurements

Abstract. We analyse the airborne measurements of above-cloud aerosols from the AErosol, RadiatiOn, and CLOuds in southern Africa (AEROCLO-sA) field campaign performed in Namibia during August and September 2017. The study aims to retrieve the aerosol above-cloud direct radiative effect (DRE) with well-defined uncertainties. To improve the retrieval of the aerosol and cloud properties, the airborne demonstrator of the Multi-Viewing, Multi-Channel, Multi-Polarization (3MI) satellite instrument, called the Observing System Including PolaRisation in the Solar Infrared Spectrum (OSIRIS), was deployed on-board the SAFIRE (Service des Avions Français Instrumentés pour la Rechercheen Environnement) Falcon 20 aircraft during 10 flights performed over land, over the ocean, and along the Namibian coast. The airborne instrument OSIRIS provides observations at high temporal and spatial resolutions for aerosol above clouds (AACs) and cloud properties. OSIRIS was supplemented with the Photomètre Léger Aéroporté pour la surveillance des Masses d'Air version 2 (PLASMA2). The combined airborne measurements allow, for the first time, the validation of AAC algorithms previously developed for satellite measurements. The variations in the aerosol properties are consistent with the different atmospheric circulation regimes observed during the deployment. Airborne observations typically show strong aerosol optical depth (AOD; up to 1.2 at 550 nm) of fine-mode particles from biomass burning (extinction Ångström exponent varying between 1.6 and 2.2), transported above bright stratocumulus decks (mean cloud top around 1 km above mean sea level), with cloud optical thickness (COT) up to 35 at 550 nm. The above-cloud visible AOD retrieved with OSIRIS agrees within 10 % of the PLASMA2 sun photometer measurements in the same environment. The single scattering albedo (SSA) is one of the most influential parameters on the AAC DRE calculation that remains largely uncertain in models. During the AEROCLO-sA campaign, the average SSA obtained by OSIRIS at 550 nm is 0.87, which is in agreement within 3 %, on average, with previous polarimetric-based satellite and airborne retrievals. The strong absorption of the biomass burning plumes in the visible range is generally consistent with the observations from the Aerosol Robotic Network (AERONET) ground-based sun photometers. This, however, shows a significant increase in the particles' absorption at 440 nm in northern Namibia and Angola, which indicates more absorbing organic species within the observed smoke plumes. Biomass burning aerosols are also vertically collocated, with significant amounts of water content up to the top of the plume at around 6 km height in our measurements. The detailed characterization of aerosol and cloud properties, water vapour, and their uncertainties obtained from OSIRIS and PLASMA2 measurements allows us to study their impacts on the AAC DRE. The high-absorbing load of AAC, combined with high cloud albedo, leads to unprecedented DRE estimates, which are higher than previous satellite-based estimates. The average AAC DRE calculated from the airborne measurements in the visible range is +85 W m−2 (standard deviation of 26 W m−2), with instantaneous values up to +190 W m−2 during intense events. These high DRE values, associated with their uncertainties, have to be considered as new upper cases in order to evaluate the ability of models to reproduce the radiative impact of the aerosols over the southeastern Atlantic region.

Characterization and source identification of submicron aerosol during serious haze pollution periods in Beijing

Submicron aerosol is of extensive concern not only due to its significant impact on air quality but also because it is detrimental to human health. In this study, we investigated the characteristics, sources and chemical processes of submicron aerosol based on real-time online measurements of submicron aerosols (NR-PM1) during December 2015 at an urban site in Beijing. The average mass concentration of NR-PM1 was 92.5±84.9 µg/m3, the hourly maximum was 459.1 µg/m3 during the entire observation. The organic aerosol (OA) (55%) was the largest contributor to NR-PM1. The average mass concentration of PAHs was 0.217±0.247 µg/m3, exhibiting the highest concentration at night and the lowest levels in the daytime. The average mass concentration of organic nitrate was 2.52±2.36 µg/m3 and that of inorganic nitrate was 7.62±8.22 µg/m3, accounting for 36% and 64%, respectively, of the total nitrate mass. Positive matrix factorization (PMF) differentiated the OA into five chemical components including LV-OOA, SV-OOA, COA, HOA and CCOA, accounting for 22%, 16%, 13%, 25% and 24% respectively, of the total OA. The average NR-PM1 mass concentration on the heavy polluted days (HPD) was 182.8±70.2 µg/m3, which was approximately 9 times that on clean days (CD). The enhanced secondary formation of SNA was evident on HPD, especially the rapid increase of sulfate (23%) and nitrate (19%).

VAHCOLI, a new concept for lidars: technical setup, science applications, and first measurements

Abstract. A new concept for a cluster of compact lidar systems named VAHCOLI (Vertical And Horizontal COverage by LIdars) is presented, which allows for the measurement of temperatures, winds, and aerosols in the middle atmosphere (∼ 10–110 km) with high temporal and vertical resolution of minutes and some tens of meters, respectively, simultaneously covering horizontal scales from a few hundred meters to several hundred kilometers (“four-dimensional coverage”). The individual lidars (“units”) being used in VAHCOLI are based on a diode-pumped alexandrite laser, which is currently designed to detect potassium (λ=770 nm), and on sophisticated laser spectroscopy measuring all relevant frequencies (seeder laser, power laser, backscattered light) with high temporal resolution (2 ms) and high spectral resolution applying Doppler-free spectroscopy. The frequency of the lasers and the narrowband filter in the receiving system are stabilized to typically 10–100 kHz, which is a factor of roughly 10−5 smaller than the Doppler-broadened Rayleigh signal. Narrowband filtering allows for the measurement of Rayleigh and/or resonance scattering separately from the aerosol (Mie) signal during both night and day. Lidars used for VAHCOLI are compact (volume: ∼ 1 m3) and multi-purpose systems which employ contemporary electronic, optical, and mechanical components. The units are designed to autonomously operate under harsh field conditions in remote locations. An error analysis with parameters of the anticipated system demonstrates that temperatures and line-of-sight winds can be measured from the lower stratosphere to the upper mesosphere with an accuracy of ±(0.1–5) K and ±(0.1–10) m s−1, respectively, increasing with altitude. We demonstrate that some crucial dynamical processes in the middle atmosphere, such as gravity waves and stratified turbulence, can be covered by VAHCOLI with sufficient temporal, vertical, and horizontal sampling and resolution. The four-dimensional capabilities of VAHCOLI allow for the performance of time-dependent analysis of the flow field, for example by employing Helmholtz decomposition, and for carrying out statistical tests regarding, for example, intermittency and helicity. The first test measurements under field conditions with a prototype lidar were performed in January 2020. The lidar operated successfully during a 6-week period (night and day) without any adjustment. The observations covered a height range of ∼ 5–100 km and demonstrated the capability and applicability of this unit for the VAHCOLI concept.

Aircraft measurements of aerosol and trace gas chemistry in the eastern North Atlantic

Abstract. The Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA) investigated properties of aerosols and subtropical marine boundary layer (MBL) clouds. Low subtropical marine clouds can have a large effect on Earth's radiative budget, but they are poorly represented in global climate models. In order to understand their radiative effects, it is imperative to understand the composition and sources of the MBL cloud condensation nuclei (CCN). The campaign consisted of two intensive operation periods (IOPs) (June–July 2017 and January–February 2018) during which an instrumented G-1 aircraft was deployed from Lajes Field on Terceira Island in the Azores, Portugal. The G-1 conducted research flights in the vicinity of the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) atmospheric observatory on Graciosa Island. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and Ionicon proton-transfer-reaction mass spectrometer (PTR-MS) were deployed aboard the aircraft, characterizing chemistry of non-refractory aerosol and trace gases, respectively. The eastern North Atlantic region was found to be very clean, with an average non-refractory submicrometer aerosol mass loading of 0.6 µg m−3 in the summer and 0.1 µg m−3 in the winter, measured by the AMS. Average concentrations of the trace reactive gases methanol and acetone were 1–2 ppb; benzene, toluene and isoprene were even lower, &lt;1 ppb. Mass fractions of sulfate, organics, ammonium and nitrate in the boundary layer were 69 %, 23 %, 7 % and 1 % and remained largely similar between seasons. The aerosol chemical composition was dominated by sulfate and highly processed organics. Particulate methanesulfonic acid (MSA), a well-known secondary biogenic marine species, was detected, with an average boundary layer concentration of 0.021 µg m−3, along with its gas-phase precursor, dimethyl sulfide (DMS). MSA accounted for no more than 3 % of the submicron, non-refractory aerosol in the boundary layer. Examination of vertical profiles of aerosol and gas chemistry during ACE-ENA reveals an interplay of local marine emissions and long-range-transported aged aerosol. A case of transport of biomass burning emissions from North American fires has been identified using back-trajectory analysis. In the summer, the non-refractory portion of the background CCN budget was heavily influenced by aerosol associated with ocean productivity, in particular sulfate formed from DMS oxidation. Episodic transport from the continents, particularly of biomass burning aerosol, periodically increased CCN concentrations in the free troposphere. In the winter, with ocean productivity lower, CCN concentrations were overall much lower and dominated by remote transport. These results show that anthropogenic emissions perturb CCN concentrations in remote regions that are sensitive to changes in CCN number and illustrate that accurate predictions of both transport and regional aerosol formation from the oceans are critical to accurately modeling clouds in these regions.

Historical Changes in Seasonal Aerosol Acidity in the Po Valley (Italy) as Inferred from Fog Water and Aerosol Measurements.

Acidity profoundly affects almost every aspect that shapes the composition of ambient particles and their environmental impact. Thermodynamic analysis of gas-particle composition datasets offers robust estimates of acidity, but they are not available for long periods of time. Fog composition datasets, however, are available for many decades; we develop a thermodynamic analysis to estimate the ammonia in equilibrium with fog water and to infer the pre-fog aerosol pH starting from fog chemical composition and pH. The acidity values from the new method agree with the results of thermodynamic analysis of the available gas-particle composition data. Applying the new method to historical (25 years) fog water composition at the rural station of San Pietro Capofiume (SPC) in the Po Valley (Italy) suggests that the aerosol has been mildly acidic, with its pH decreasing by 0.5–1.5 pH units over the last decades. The observed pH of the fog water also increased 1 unit over the same period. Analysis of the simulated aerosol pH reveals that the aerosol acidity trend is driven by a decrease in aerosol precursor concentrations, and changes in temperature and relative humidity. Currently, NOx controls would be most effective for PM2.5 reduction in the Po valley both during summer and winter. In the future, however, seasonal transitions to the NH3-sensitive region may occur, meaning that the NH3 reduction policy may become increasingly necessary.

Trends, composition, and sources of carbonaceous aerosol at the Birkenes Observatory, northern Europe, 2001–2018

Abstract. We present 18 years (2001–2018) of aerosol measurements, including organic and elemental carbon (OC and EC), organic tracers (levoglucosan, arabitol, mannitol, trehalose, glucose, and 2-methyltetrols), trace elements, and ions, at the Birkenes Observatory (southern Norway) – a site representative of the northern European region. The OC/EC (2001–2018) and the levoglucosan (2008–2018) time series are the longest in Europe, with OC/EC available for the PM10, PM2.5 (fine), and PM10–2.5 (coarse) size fractions, providing the opportunity for a nearly 2-decade-long assessment. Using positive matrix factorization (PMF), we identify seven carbonaceous aerosol sources at Birkenes: mineral-dust-dominated aerosol (MIN), traffic/industry-like aerosol (TRA/IND), short-range-transported biogenic secondary organic aerosol (BSOASRT), primary biological aerosol particles (PBAP), biomass burning aerosol (BB), ammonium-nitrate-dominated aerosol (NH4NO3), and (one low carbon fraction) sea salt aerosol (SS). We observed significant (p&lt;0.05), large decreases in EC in PM10 (−3.9 % yr−1) and PM2.5 (−4.2 % yr−1) and a smaller decline in levoglucosan (−2.8 % yr−1), suggesting that OC/EC from traffic and industry is decreasing, whereas the abatement of OC/EC from biomass burning has been slightly less successful. EC abatement with respect to anthropogenic sources is further supported by decreasing EC fractions in PM2.5 (−3.9 % yr−1) and PM10 (−4.5 % yr−1). PMF apportioned 72 % of EC to fossil fuel sources; this was further supported by PMF applied to absorption photometer data, which yielded a two-factor solution with a low aerosol Ångstrøm exponent (AAE = 0.93) fraction, assumed to be equivalent black carbon from fossil fuel combustion (eBCFF), contributing 78 % to eBC mass. The higher AAE fraction (AAE = 2.04) is likely eBC from BB (eBCBB). Source–receptor model calculations (FLEXPART) showed that continental Europe and western Russia were the main source regions of both elevated eBCBB and eBCFF. Dominating biogenic sources explain why there was no downward trend for OC. A relative increase in the OC fraction in PM2.5 (+3.2 % yr−1) and PM10 (+2.4 % yr−1) underscores the importance of biogenic sources at Birkenes (BSOA and PBAP), which were higher in the vegetative season and dominated both fine (53 %) and coarse (78 %) OC. Furthermore, 77 %–91 % of OC in PM2.5, PM10–2.5, and PM10 was attributed to biogenic sources in summer vs. 22 %–37 % in winter. The coarse fraction had the highest share of biogenic sources regardless of season and was dominated by PBAP, except in winter. Our results show a shift in the aerosol composition at Birkenes and, thus, also in the relative source contributions. The need for diverse offline and online carbonaceous aerosol speciation to understand carbonaceous aerosol sources, including their seasonal, annual, and long-term variability, has been demonstrated.