Aerosol Size Distribution Research Articles

An improved representation of aerosol in the ECMWF IFS-COMPO 49R1 through the integration of EQSAM4Climv12 – a first attempt at simulating aerosol acidity

Abstract. The atmospheric composition forecasting system used to produce the Copernicus Atmosphere Monitoring Service (CAMS) forecasts of global aerosol and trace gas distributions, the Integrated Forecasting System (IFS-COMPO), undergoes periodic upgrades. In this study we describe the development of the future operational cycle 49R1 and focus on the implementation of the thermodynamical model EQSAM4Clim version 12, which represents gas–aerosol partitioning processes for the nitric acid–nitrate and ammonia–ammonium couples and computes diagnostic aerosol, cloud, and precipitation pH values at the global scale. This information on aerosol acidity influences the simulated tropospheric chemistry processes associated with aqueous-phase chemistry and wet deposition. The other updates of cycle 49R1 concern wet deposition, sea-salt aerosol emissions, dust optics, and size distribution used for the calculation of sulfate aerosol optics. The implementation of EQSAM4Clim significantly improves the partitioning of reactive nitrogen compounds, decreasing surface concentrations of both nitrate and ammonium in the particulate phase, which reduces PM2.5 biases for Europe, the US, and China, especially during summertime. For aerosol optical depth there is generally a decrease in the simulated wintertime biases and for some regions an increase in the summertime bias. Improvements in the simulated Ångström exponent are noted for almost all regions, resulting in generally good agreement with observations. The diagnostic aerosol and precipitation pH calculated by EQSAM4Clim have been compared to ground observations and published simulation results. For precipitation pH, the annual mean values show relatively good agreement with the regional observational datasets, while for aerosol pH the simulated values over continents are quite close to those simulated by ISORROPIA II. The use of aerosol acidity has a relatively smaller impact on the aqueous-phase production of sulfate compared to the changes in gas-to-particle partitioning induced by the use of EQSAM4Clim.

Aerosol size distribution properties associated with cold-air outbreaks in the Norwegian Arctic

Abstract. The aerosol particles serving as cloud condensation and ice nuclei contribute to key cloud processes associated with cold-air outbreak (CAO) events but are poorly constrained in climate models due to sparse observations. Here we retrieve aerosol number size distribution modes from measurements at Andenes, Norway, during the Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) and at Zeppelin Observatory, approximately 1000 km upwind from Andenes at Svalbard. During CAO events at Andenes, the sea-spray-mode number concentration is correlated with strong over-ocean winds with a mean of 8±4 cm−3 that is 71 % higher than during non-CAO conditions. Additionally, during CAO events at Andenes, the mean Hoppel minimum diameter is 6 nm smaller than during non-CAO conditions, though the estimated supersaturation is lower, and the mean number concentration of particles that likely activated in-cloud is 109±61 cm−3 with no statistically significant difference from the non-CAO mean of 99±66 cm−3. For CAO trajectories between Zeppelin Observatory and Andenes, the upwind-to-downwind change in number concentration is the largest for the accumulation mode with a mean decrease of 93±95 cm−3, likely attributable primarily to precipitation scavenging. These characteristic properties of aerosol number size distributions during CAO events provide guidance for evaluating CAO aerosol–cloud interaction processes in models.

Size distribution of protein aerosols in a megacity in Northwest China and their in silico deposition characteristics in the human respiratory tract

Size distribution of protein aerosols in a megacity in Northwest China and their in silico deposition characteristics in the human respiratory tract

The Transition from Aerosol- to Updraft-Limited Susceptibility Regime in Large-Eddy Simulations with Bulk Microphysics

Large-eddy simulation (LES) is often used as a benchmark simulation in climate science and is suggested as a fundamental tool to examine, e.g., marine cloud brightening. Therefore, it is necessary to critically evaluate if these high-resolution models can skillfully simulate expected physical phenomena. This study focuses on the first indirect aerosol effect in warm stratocumulus clouds. We investigate if an LES code with explicit aerosol-cloud interactions and a widely used two-moment bulk microphysical scheme can reproduce well-known cloud droplet number susceptibility regimes previously identified by observations and supported by detailed parcel model simulations—the updraft-limited regime (typically occurring at high aerosol number concentrations and low updraft speeds) and the aerosol-limited regime (typically occurring at low aerosol number concentrations and high updraft speeds). Our simulations show that the LES in its default configuration cannot reproduce the two regimes if the initial droplet radius of newly activated droplets (rid) is estimated by integrating the wet aerosol size distribution. The main reason is related to the relatively coarse (but commonly used) time step in the model (Δt ≈ 1s), which is too long to resolve relevant microphysical processes adequately at high aerosol concentrations. A regime transition does occur if the timestep is decreased to Δt ≈ 0.1s and if a renormalization procedure is applied, which limits the number of activated droplets so that the water mass of the newly activated droplets cannot exceed the available amount of supersaturated water vapor. Another way to obtain a regime transition is to increase rid to values >1 µm. However, a clear recommendation for the choice of rid cannot be made upon physical arguments. An alternative solution could be to introduce a sub-time-stepping or adaptive time-stepping algorithm to calculate droplet formation and growth, particularly for updraft-limited conditions. Our study highlights the importance of critically evaluating LES results to guarantee that relevant physical processes are properly represented.

Quantifying multi-virion aerosols in respiratory infection transmission

Infectious aerosols are expired in various sizes, and the number of contained virions is expected to significantly vary among expired aerosols. To evaluate the effect of the number of contained virions on infection risk, multi-virion aerosols in expired air should be first quantified. In this study, we categorised expired aerosols into traditional aerosol size bins and aerosols containing different number of virions. We quantified the number of virions in aerosols of each size bin and estimated the size distribution of aerosols which contain a certain number of virions when the viral load is known. This analysis helped us to determine the relationship between multi-size aerosols and multi-virion aerosols. Our findings indicate that for long-range airborne transmission, the airborne transmission droplets derived from four COVID-19 outbreak venues contain at most one infectious virion, supporting the one-virion assumption for the considered viral load ranges. However, for short-range airborne transmission, the impact of multi-virion aerosols on infection risk must be considered. Our quantification of multi-virion aerosols for the first time lays the groundwork for incorporating the multi-virion assumption into infection risk assessments.

Comparison of aerosol number size distribution and new particle formation in summer at alpine and urban regions in the Guanzhong Plain, Northwest China

Ultrafine particles play a crucial role in understanding climate change, mitigating adverse health effects, and developing strategies for air pollution control. However, the factors influencing the occurrence and development of new particle formation (NPF) events, as well as the underlying chemical mechanisms, remain inadequately explained. This study compared number concentrations and size distributions of atmospheric ultrafine particles at Xi'an (urban area) and the summit of Mt. Hua (alpine region) in summer to investigate the NPF mechanism and particle growth in both clean and polluted areas of the Guanzhong Plain. The average particle number concentration in Xi'an was significantly higher than that at Mt. Hua. The diurnal variation of total particle number concentration differed between Xi'an and Mt. Hua indicating a divergence in influencing factors. The size distributions in Xi'an varied across different timescales and weather conditions, whereas Mt. Hua exhibited little variation. This stability at Mt. Hua is attributed to its cleaner background atmosphere and the steady influx of aging particles with larger diameters transported from the free atmosphere. In both areas, geometric mean diameters (GMDs) were inversely proportional to particle number concentrations suggesting that increase in particle numbers were primarily due to the generation of smaller particles. The potential governing factors for NPF events differed somewhat between the urban and mountainous stations. In the urban area, intense local stationary and mobile emission sources promoted the growth of newly formed nanoparticles, with ozone-oxidized condensable vapors serving as key precursors. In contrast, at the mountainous station, NPF process were significantly influenced by anthropogenic precursors from long-range transport and locally emitted biogenic organics. The rapid increase in ultrafine particle concentrations primarily poses serious health risks and degrades air quality in urban areas, while also contributing to climate-related effects in alpine regions.

Lognormal mode dissociation method based on intrinsic characteristics of aerosol size distribution

Aerosols significantly affect the transmission of optical signals in the atmosphere, necessitating accurate atmospheric models for the performance evaluation of electro-optic devices. Aerosol size distribution is a critical parameter in these models, and the lognormal function is commonly used to mathematically represent it. This study aims to handle the lack of a solid criterion for determining the number of lognormal modes and introduces an improved scheme that leverages the characteristics of the second derivative (SD) of the Gaussian curve to identify the mode amount and to initialize mode parameters for fitting. The optimization problem is solved using a genetic algorithm, incorporating a goodness-of-fit index to determine the presence of spurious modes. For aerosol size distributions characterized by a single Gaussian peak, mode parameters such as mode radius and width can be straightforwardly identified through the positions of peaks and roots on the SD curve. However, the original mode dissociation method may overlook potential modes in distributions composed of superimposed Gaussian peaks. Numerical tests indicate that such oversights can result in substantial errors in calculating the aerosol extinction coefficient, with relative errors exceeding 100%. The proposed scheme significantly enhances the accuracy of mode dissociation in aerosol size distribution, reducing errors in aerosol extinction coefficient calculations by approximately 40% when applied to data from the Aerosol Robotic Network (AERONET). An additional benefit of this method is its ability to constrain the number of lognormal modes in an aerosol size distribution. Results from applying this scheme to data from selected AERONET sites reveal that over half of the size distributions consist of more than two lognormal modes, highlighting the effectiveness of the proposed approach in capturing complex aerosol behaviors.

Rapid Nucleation and Growth of Indoor Atmospheric Nanocluster Aerosol during the Use of Scented Volatile Chemical Products in Residential Buildings.

Scented volatile chemical products (sVCPs) are frequently used indoors. We conducted field measurements in a residential building to investigate new particle formation (NPF) from sVCP emissions. State-of-the-art instrumentation was used for real-time monitoring of indoor atmospheric nanocluster aerosol (NCA; 1-3 nm particles) size distributions and terpene mixing ratios. We integrated our NCA measurements with a comprehensive material balance model to analyze sVCP-nucleated indoor NCA dynamics. Our results reveal that sVCPs significantly increase indoor terpene mixing ratios (10-1,000 ppb), exceeding those in outdoor forested environments. The emitted terpenes react with indoor atmospheric O3 and initiate indoor NPF, resulting in nucleation rates as high as ∼105 cm-3 s-1 and condensational growth rates up to 300 nm h-1; these are orders of magnitude higher than those reported during outdoor NPF events. Notably, high particle nucleation rates significantly increase indoor atmospheric NCA concentrations (105-108 cm-3), and high growth rates drive their survival and growth to sizes that efficiently reach the deepest regions of the human respiratory system. We found sVCP-nucleated NCA to cause respiratory exposures and dose rates comparable to or exceeding those from primary aerosol sources such as gas stoves and diesel engines, highlighting their significant impact on indoor atmospheric environments.

Modelling the ejection of primary aerosols during the fast pyrolysis of biomass anisotropic particles

A model for the fast pyrolysis of anisotropic biomass particles is presented which considers bubbling dynamics within the liquid intermediate phase (metaplast) and aerosol ejection from this phase. The model employs the population balance equation and the method of moments to estimate the production rate and resultant size distribution of aerosol ejections, incorporating a detailed CRECK reaction mechanism, and considers the effect of anisotropic biomass microstructure on the intraparticle transport of mass and energy. This study investigates the impact of particle size, heating rate (heat transfer coefficient), and lignocellulosic composition on aerosol ejection. The model predicts that, at high heating rates (convective heat transfer coefficient of 359 W/m2.K), aerosols can contribute over 20% to the heavy fraction yield in bio-oil for small particles (1 mm diameter, 4 mm length). The model can predict aerosol size distribution and surface area, indicating an average size of 20 μm for bubbles and 5 μm for aerosols during increased bubble production and aerosol ejection rates. These findings are consistent with prior experimental results and provide essential information for future modeling of extra-particle reactions of the aerosols as they progress through the reactor.

Optimizing indoor air models through k-means clustering of nanoparticle size distribution data

Sectional physics-based aerosol models imply a computational effort that hinders their use in building digital twins, real-time predictive control, and computer-based iterative optimization versus black-box approaches. The innovation of this paper lies in the proposal of a novel systematic methodology to optimize the number of size bins in sectional reduced-order models for particle concentration simulations. This allows its application in indoor air quality management and overcomes generalizability and data-dependency issues of black-box models. This method, based on k-means clustering, aims to ensure precision when tackling relatively fast fine and ultrafine particle simulations targeting the reduction of time and resource consumption from experimentally-determined aerosol size distribution time series. Consequently, three tests were carried out using combustion aerosols inside a custom-designed emission chamber to simulate emission hotspots in non-commercial and occupational settings. 2-, 3-, 4-, and 5-cluster classifications were evaluated for data coming from 13 particle size bins through silhouette analysis and the study of their temporal profiles. Results show that the 4-cluster classification summarizes the behavior of data in the 10–420 nm range, ensuing up to a 77 % improvement in the model's computational demand. Moreover, this method allows an accurate definition of the necessary size ranges to calculate nanoparticle concentrations inside the chamber and facilitates the interpretation of aerosol behavior and processes through the resulting clusters' temporal profiles.

MAP-IO: an atmospheric and marine observatory program on board Marion Dufresne over the Southern Ocean

Abstract. This article is devoted to the presentation of the MAP-IO observation program. This program, launched in early 2021, has enabled the observation of nearly 700 d of measurements over the Indian and Southern Ocean with the equipment of 17 meteorological and oceanographic scientific instruments on board the ship Marion Dufresne. Several observational techniques have been developed to respond to the difficulties of observations on board the ship, in particular for passive remote sensing data, as well as for quasi-autonomous data acquisition and transfer. The first measurements made it possible to draw up unprecedented climatological data of the Southern Ocean regarding the size distribution and optical thickness of aerosols, the concentration of trace gases and greenhouse gases, UV, and integrated water vapor. High-resolution observations of phytoplankton in surface waters have also shown a great variability in latitude in terms of abundance and community structure (diversity). The operational success of this program and these unique scientific results together establish a proof of concept and underline the need to transform this program into a permanent observatory. The multi-year rotations over the Indian Ocean will enable us to assess the trends and seasonal variability of phytoplankton, greenhouse gases, ozone, and marine aerosols in a sensitive and poorly documented climatic region. Without being exhaustive, MAP-IO should make it possible to better understand and assess the biological carbon pump, to study the variability of gases and aerosols in a region that is remote in relation to the main anthropogenic sources, and to monitor the transport of stratospheric ozone by the Brewer–Dobson circulation. The meteorological MAP-IO data set is publicly available at https://www.aeris-data.fr/catalogue-map-io/ (last access: 26 August 2024) (atmospheric data) and at https://doi.org/10.17882/89505 (Thyssen et al., 2022a) (phytoplankton data).

Physicochemical Characterization of Religious Burning Aerosols in Lhasa on the Qinghai‐Tibet Plateau

AbstractReligious burning (RB) has been identified as a major source of atmospheric aerosols on the Qinghai‐Tibet Plateau. However, there is limited understanding of the detailed chemical composition, size distribution, and optical properties of RB aerosols in this region. To characterize these important aerosol properties, ambient PM2.5 and size resolved aerosols from RB emissions in Lhasa were collected during summer 2019. Organic functional group (OFG) and inorganic ion composition was measured using Fourier transform infrared spectroscopy and ion chromatography, respectively. The ambient PM2.5 was dominated by organic components, with the OFG concentrations significantly higher during religious events, reflecting the substantial impact of RB emissions on local air quality. The RB aerosols were characterized by high fractions of alkane (34%), hydroxyl (29%), and carboxylic acid (13%) groups, with peak mass in the accumulation mode (0.56–1.00 μm). The high abundance of hydroxyl group and the size distribution pattern suggested that the RB aerosols were formed from volatilization of fuel materials followed by unaltered condensation, a process that may be unique to the low‐temperature, low‐oxygen burning in the scattered burners at the temples. The absorption coefficient of RB aerosols showed similar size distribution to the mass size distribution, but the absorption Ångström exponent displayed the lowest value in the 0.56–1.00 μm size mode. This specific size distribution aligned with the mass fraction of carboxylic acids and mirrored the mass proportion of alkanes, suggesting that smaller and larger particles were enriched with substances that have higher light‐absorbing capabilities.

Evolution of Light Absorption Enhancement of Black Carbon Aerosols From Biomass Burning in Atmospheric Photochemical Aging

AbstractThe light absorption enhancement (Eabs) of black carbon (BC) coated with non‐BC materials is crucial in the assessment of radiative forcing, yet its evolution during photochemical aging of plumes from biomass burning, the globe's largest source of BC, remains poorly understood. In this study, plumes from open burning of corn straw were introduced into a smog chamber to explore the evolution of Eabs during photochemical aging. The light absorption of BC was measured with and without coating materials by using a thermodenuder, while the size distributions of aerosols and composition of BC coating materials were also monitored. Eabs was found to increase initially, and then decrease with an overall downward trend. The lensing effect dominated in Eabs at 520 nm, with an estimated contribution percentages of 47.5%–94.5%, which is far greater than light absorption of coated brown carbon (BrC). The effects of thickening and chemical composition changes of the coating materials on Eabs were evaluated through comparing measured Eabs with that calculated by the Mie theory. After OH exposure of 1 × 1010 molecules cm−3 s, the thickening of coating materials led to an Eabs increase by 3.2% ± 1.6%, while the chemical composition changes or photobleaching induced an Eabs decrease by 4.7% ± 0.6%. Simple forcing estimates indicate that coated BC aerosols exhibit warming effects that were reduced after aging. The oxidation of light‐absorbing CxHy compounds, such as polycyclic aromatic hydrocarbons (PAHs), to CxHyO and CxHyO>1 compounds in coating materials may be responsible for the photobleaching of coated BrC.

Aerosol mixing state, new particle formation, and cloud droplet number concentration in an urban environment

Anthropogenically derived aerosols have been hypothesized to influence convective precipitation by increasing the available pool of cloud condensation nuclei. Here, we present a synthesis of aerosol size distribution and subsaturated hygroscopicity measurements between 15 and 250 nm diameter particles during the TRacking Aerosol Convection interactions ExpeRiment (TRACER). We found that the aerosol is externally mixed and can be described by a quasi-two-component description comprising a more and less hygroscopic mode. The mean hygroscopicity parameters for these modes across all sizes were 0.03 ± 0.04 and 0.22 ± 0.08 with no significant dependence on particle size. The number fraction of the more hygroscopic mode is 40 % for particles between 15 and 40 nm and gradually increases to ~70 % for particles >100 nm. Winds from the southerly direction feature particles with larger hygroscopicity parameters and have a larger fraction of particles in the more hygroscopic mode. The hygroscopicity parameter exhibits diurnal cycles that are consistent with condensation of a species with a hygroscopicity parameter ~0.1 which corresponds to values expected for secondary organic aerosol. We also identified nine small particle events that were attributed to particle formation by nucleation. The data are consistent with new particle formation having occurred aloft, followed by downward mixing with daytime turbulence. The species that are responsible for modal growth had hygroscopicity parameters varying between 0.05 and 0.34. These values systematically depended on the wind sector, suggesting that the chemical composition of the precursors differed. Hourly cloud condensation nuclei (CCN) and cloud droplet number concentration (CDNC) values derived from the aerosol size distribution, subsaturated hygroscopicity measurements, and adiabatic parcel model simulations showed a dynamic range of a factor of 2–3 in CDNC depending on the wind sector, with lower values associated with southerly onshore flow.

Seasonal dynamics of airborne biomolecules influence the size distribution of Arctic aerosols

Organic matter is crucial in aerosol–climate interactions, yet the physicochemical properties and origins of organic aerosols remain poorly understood. Here we show the seasonal characteristics of submicron organic aerosols in Arctic Svalbard during spring and summer, emphasizing their connection to transport patterns and particle size distribution. Microbial-derived organic matter (MOM) and terrestrial-derived organic matter (TOM) accounted for over 90% of the total organic mass in Arctic aerosols during these seasons, comprising carbohydrate/protein-like and lignin/tannin-like compounds, respectively. In spring, aerosols showed high TOM and low MOM intensities due to biomass-burning influx in the central Arctic. In contrast, summer exhibited elevated MOM intensity, attributed to the shift in predominant atmospheric transport from the central Arctic to the biologically active Greenland Sea. MOM and TOM were associated with Aitken mode particles (<100 nm diameter) and accumulation mode particles (>100 nm diameter), respectively. This association is linked to the molecular size of biomolecules, impacting the number concentrations of corresponding aerosol classes. These findings highlight the importance of considering seasonal atmospheric transport patterns and organic source-dependent particle size distributions in assessing aerosol properties in the changing Arctic.

The algorithm of microphysical-parameter profiles of aerosol and small cloud droplets based on the dual-wavelength lidar data

Abstract. This study proposed an inversion method for atmospheric-aerosol or cloud microphysical parameters based on dual-wavelength lidar data. The matching characteristics between aerosol and cloud particle size distributions and gamma distributions were studied using aircraft observation data. The feasibility of the retrieval of the particle effective radius from lidar ratios and backscatter ratios was simulated and studied. A method for inverting the effective radius and number concentration of atmospheric aerosols or small cloud droplets using the backscatter ratio was proposed, and the error sources and applicability of the algorithm were analyzed. This algorithm was suitable for the inversion of uniformly mixed and single-property aerosol layers or small cloud droplets. Compared with the previous study, this algorithm could quickly obtain the microphysical parameters of atmospheric particles and has good robustness. For aerosol particles, the inversion range that this algorithm can achieve is 0.3–1.7 µm. For cloud droplets, it is 1.0–10 µm. An atmospheric-observation experiment was conducted using the multi-wavelength lidar developed by Xi'an University of Technology, and a thin cloud layer was captured. The microphysical parameters of aerosol and clouds during this process were retrieved. The results clearly demonstrate the growth of the effective radius and number concentration.

Validating a microphysical prognostic stratospheric aerosol implementation in E3SMv2 using observations after the Mount Pinatubo eruption

Abstract. This paper describes the addition of a stratospheric prognostic aerosol (SPA) capability – developed with the goal of accurately simulating sulfate aerosol formation and evolution in the stratosphere – in the Department of Energy (DOE) Energy Exascale Earth System Model, version 2 (E3SMv2). The implementation includes changes to the four-mode Modal Aerosol Module microphysics in the stratosphere to allow for larger particle growth and more accurate stratospheric aerosol lifetime following the Pinatubo eruption. E3SMv2-SPA reasonably reproduces stratospheric aerosol lifetime, burden, aerosol optical depth, and top-of-atmosphere flux when compared to remote sensing observations. E3SMv2-SPA also has close agreement with the interactive chemistry–climate model CESM2-WACCM (Community Earth System Model version 2–Whole Atmosphere Community Climate Model) – which has a more complete chemical treatment – and the observationally constrained, prescribed volcanic aerosol treatment in E3SMv2. Global stratospheric aerosol size distributions identify the nucleation and growth of sulfate aerosol from volcanically injected SO2 from both major and minor volcanic eruptions from 1991 to 1993. The modeled aerosol effective radius is consistently lower than satellite and in situ measurements (max differences of ∼ 30 %). Comparisons with in situ size distribution samples indicate that this simulated underestimation in both E3SMv2-SPA and CESM2-WACCM is due to overly small accumulation and coarse-mode aerosols 6–18 months post-eruption, with E3SMv2-SPA simulating ∼ 50 % of the coarse-mode geometric mean diameters of observations 11 months post-eruption. Effective radii from the models and observations are used to calculate offline scattering and absorption efficiencies to explore the implications of smaller simulated aerosol size for the Pinatubo climate impacts. Scattering efficiencies at wavelengths of peak solar irradiance (∼ 0.5 µm) are 10 %–80 % higher for daily samples in models relative to observations through 1993, suggesting higher diffuse radiation at the surface and a larger cooling effect in the models due to the smaller simulated aerosol; absorption efficiencies at the peak wavelengths of outgoing terrestrial radiation (∼ 10 µm) are 15 %–40 % lower for daily samples in models relative to observations, suggesting an underestimation in stratospheric heating in the models due to the smaller simulated aerosol. These potential biases are based on aerosol size alone and do not take into account differences in the aerosol number. The overall agreement of E3SMv2-SPA with observations and its similar performance to the well-validated CESM2-WACCM makes E3SMv2-SPA a viable alternative to simulating climate impacts from stratospheric sulfate aerosols.

Characterisation of urban aerosol size distribution by radiocarbon and PIXE analyses in a middle-European urban environment for source identification: a pilot study

This study, conducted in Debrecen, Hungary, aimed to analyse atmospheric particulate matter (APM or PM) through radiocarbon and PIXE analyses during the winter smog (23–25 January) and spring (15–18 May) seasons. The information presented in this pilot study aims to provide insight into the importance of utilising detailed characteristics of the mass size distributions of fossil carbon (ff) and contemporary carbon (fC) content. Additionally, it seeks to compare these characteristics with the size distributions of various elements to enable even more accurate PM source identification. In winter, APM concentrations were 86.27 μg/m3 (total), 17.07 μg/m3 (fC) and 10.4 μg/m3 (ff). In spring, these values changed to 29.5 μg/m3, 2.64 μg/m3 and 7.01 μg/m3, respectively. Notably, differences in mass size distribution patterns were observed between the two seasons, suggesting varied sources for contemporary carbon. Biomass burning emerged as a crucial source during the smog period, supported by similar MMAD (Mass Median Aerodynamic Diameter) values and a strong correlation (r = 0.95, p < 0.01) between potassium and fC. In spring, a significant change in the concentration and distribution of fC occurred, with a broad, coarse mode and a less prominent accumulation mode. Ff was found to have similar distributions as PM, with nearly the same MMADs, during both periods. Finally, a comprehensive comparison of modal characteristics identified specific sources for the various components, including biomass burning, vehicle exhaust, coal and oil combustion, vehicle non-exhaust, road dust, tyre abrasion, mineral dust and biogenic emission. This study showcases how using radiocarbon and PIXE analysis in size distribution data can enhance our understanding of the sources of PM and their effects on different size fractions of PM.

Comparison of scanning aerosol lidar and in situ measurements of aerosol physical properties and boundary layer heights

Abstract. The spatiotemporal distribution of aerosol particles in the atmosphere has a great impact on radiative transfer, clouds, and air quality. Modern remote sensing methods, as well as airborne in situ measurements by unpiloted aerial vehicles (UAV) or balloons, are suitable tools to improve our understanding of the role of aerosol particles in the atmosphere. To validate the measurement capabilities of three relatively new measurement systems and to bridge the gaps that are often encountered between remote sensing and in situ observation, as well as to investigate aerosol particles in and above the boundary layer, we conducted two measurement campaigns and collected a comprehensive dataset employing a scanning aerosol lidar, a balloon-borne radiosonde with the Compact Optical Backscatter Aerosol Detector (COBALD), an optical particle counter (OPC) on a UAV, and a comprehensive set of ground-based instruments. The extinction coefficients calculated from near-ground-level aerosol size distributions measured in situ are well correlated with those retrieved from lidar measurements, with a slope of 1.037 ± 0.015 and a Pearson correlation coefficient of 0.878, respectively. Vertical profiles measured by an OPC-N3 on a UAV show similar vertical particle distributions and boundary layer heights to lidar measurements. However, the sensor, OPC-N3, shows a larger variability in the aerosol backscatter coefficient measurements, with a Pearson correlation coefficient of only 0.241. In contrast, the COBALD data from a balloon flight are well correlated with lidar-derived backscatter data from the near-ground level up to the stratosphere, with a slope of 1.063 ± 0.016 and a Pearson correlation coefficient of 0.925, respectively. This consistency between lidar and COBALD data reflects the good data quality of both methods and proves that lidar can provide reliable and spatial distributions of aerosol particles with high spatial and temporal resolutions. This study shows that the scanning lidar has the capability to retrieve backscatter coefficients near the ground level (from 25 to 50 m above ground level) when it conducts horizontal measurement, which is not possible for vertically pointing lidar. These near-ground-level retrievals compare well with ground-level in situ measurements. In addition, in situ measurements on the balloon and UAV validated the scanning lidar retrievals within and above the boundary layer. The scanning aerosol lidar allows us to measure aerosol particle distributions and profiles from the ground level to the stratosphere with an accuracy equal to or better than in situ measurements and with a similar spatial resolution.

The Role of Deposition of Cosmogenic 10Be for the Detectability of Solar Proton Events

AbstractThe manifestation of extreme solar proton events (SPEs) in Beryllium‐10 (10Be) ice core data contains valuable information about the strength and incidence of SPEs or local characteristics of the atmosphere. To extract this information, the signals of enhanced production of cosmogenic 10Be due to the SPEs have to be detected, hence distinguished from the variability of the background production by galactic cosmic rays (GCRs). Here, we study the transport and deposition of 10Be from GCRs, using the ECHAM/MESSy Atmospheric Chemistry climate model, and discuss the detectability of extreme SPEs (similar to the CE 774/775 SPE) in 10Be ice core data depending on the ice core location, seasonal appearance of the SPE, atmospheric aerosol size distribution and phase of the 11‐year solar cycle. We find that sedimentation can be a major deposition mechanism of GCR generated 10Be, especially at high latitudes, depending on the aerosols to which 10Be attaches after production. The comparison of our results to four ice core records of 10Be from Greenland and Antarctica shows good agreement for both 10Be from GCRs and solar energetic particles (SEP). From our results we deduce that the location of detection and the season of occurrence of the SPE have a considerable effect on its detectability, as well as the aerosol size distribution the produced cosmogenic nuclides meet in the atmosphere. Furthermore, we find that SPEs occurring in the phase of highest activity during the 11‐year solar cycle are more detectable than SPEs that arise in the phase of lowest activity.