Particle Number Size Distributions Research Articles

Attribution of aerosol particle number size distributions to main sources using an 11-year urban dataset

Abstract. Source apportionment was performed using size-segregated atmospheric particle number concentrations (PNCs) in 27 size channels over a diameter range of 6–1000 nm augmented by air pollutants with a time resolution of 1 h in Budapest for 11 full years. The input dataset was treated for the effect of the local meteorology using dispersion correction. Both the uncorrected dataset and corrected dataset were evaluated using positive matrix factorization for separate seasons. Six source types including nucleation, two road vehicle emission sources separated into a semi-volatile fraction and a solid-core fraction, a diffuse urban source, a secondary inorganic aerosol (SIA) source, and an ozone-associated secondary aerosol source were identified, characterized and quantified. The dispersion correction did not considerably change the profiles, diel variations or patterns of the sources, while it substantially modified the relative shares of the nucleation source in all seasons. The mean relative contributions of the traffic emissions (60 %) indicate that on-road motor vehicles were the leading source of particle numbers. The nucleation was responsible for 24 % of the PNC annually as a lower estimate. It exhibited a compound character consisting of photochemically induced nucleation and traffic-related nucleation. Its contributions were the highest in spring and the lowest in winter. The shares of the urban diffuse and SIA source types were the largest in autumn and winter and in spring and summer, respectively, but they were typically ⪅ 10 %. The O3-associated secondary aerosol made up the smallest (⪅ 3 %) contributions. The conditional bivariate probability function analysis showed considerable spatial variations in the source origin. The combination of the size-segregated particle number concentrations, wide overall range of the size channels, considerably long dataset, dispersion correction and modelling over separate seasons led jointly to a unique adaptation of the source apportionment and yielded novel and valuable insights into the urban aerosol sources and processes both for Budapest and in general.

Optofluidic Force Induction Meets Raman Spectroscopy and Inductively Coupled Plasma-Mass Spectrometry: A New Hyphenated Technique for Comprehensive and Complementary Characterizations of Single Particles.

Nanoparticles are produced at accelerating rates, are increasingly integrated into scientific and industrial applications, and are widely discharged into the environment. Analytical techniques are required to characterize parameters such as particle number concentrations, mass and size distributions, molecular and elemental compositions, and particle stability. This is not only relevant to investigate their utility for various industrial or medical applications and for controlling the manufacturing processes but also to assess toxicity and environmental fate. Different analytical strategies aim to characterize certain facets of particles but are difficult to combine to retrieve relevant parameters coherently and to provide a more comprehensive picture. In this work, we demonstrate the first online hyphenation of optofluidic force induction (OF2i) with Raman spectroscopy and inductively coupled plasma-time-of-flight-mass spectrometry (ICP-TOFMS) to harness their complementary technology-specific advantages and to promote comprehensive particle characterizations. We optically trapped individual particles on a weakly focused vortex laser beam by aligning a microfluidic flow antiparallelly to the laser propagation direction. The position of particles in this optical trap depended on the hydrodynamic diameter and therefore enabled size calibration as well as matrix elimination. Additionally, laser light scattered on particles was analyzed in a single particle (SP) Raman spectroscopy setup for the identification of particulate species and phases. Finally, particles were characterized regarding elemental composition and their distributions in mass and size using SP ICP-TOFMS. In a proof of concept, we analyzed polystyrene-based microplastic and TiO2 nanoparticles and demonstrated the opportunities provided through the coupling of OF2i with SP Raman and SP ICP-TOFMS.

Characterization of the airborne aerosol inlet and transport system used during the A-LIFE aircraft field experiment

Abstract. Atmospheric aerosol particles have a profound impact on Earth's climate by scattering and absorbing solar and terrestrial radiation and by impacting the properties of clouds. Research aircraft such as the Deutsches Zentrum für Luft- und Raumfahrt e.V. (DLR) Falcon are widely used to study aerosol particles in the troposphere and lower stratosphere. However, transporting a representative sample to the instrumentation inside the aircraft remains a challenge due to high airspeeds and changing ambient conditions. In particular, for high-quality coarse-mode aerosol measurements, knowledge about losses or enhancements in the aerosol sampling system is crucial. In this study, the sampling efficiency of the aerosol inlet aboard the Falcon research aircraft is characterized for the first time with state-of-the art in situ measurements including sizing instruments operated behind the Falcon aerosol inlet and mounted at the aircraft wing not affected by the aerosol inlet. Sampling efficiencies were derived for different true airspeed ranges by comparing the in-cabin and ”full”-size-range particle number size distributions during 174 flight sequences with a major contribution of mineral dust particles during the ”Absorbing aerosol layers in a changing climate: aging, lifetime and dynamics” project (A-LIFE). Additionally, experimentally derived Stokes numbers were used to calculate the cutoff diameter of the aerosol sampling system for different particle densities as a function of true airspeed. As expected, the results show that the velocity of the research aircraft has a major impact on the sampling of coarse-mode aerosol particles with in-cabin instruments. For true airspeeds up to about 190 m s−1, aerosol particles larger than about 1 µm are depleted in the sampling system of the Falcon during the A-LIFE project. In contrast, for true airspeeds higher than 190 m s−1, an enhancement of particles up to a diameter of 4 µm is observed. For even larger particles, the enhancement effect at the inlet is still present, but inertial and gravitational particle losses in the transport system get more and more pronounced, which leads to a decreasing overall sampling efficiency. In summary, aerosol particles are either depleted or enhanced in the Falcon aerosol inlet, whereas transport in sampling lines always leads to a loss of particles. Here, we have considered both effects and determined the cutoff diameter for the A-LIFE transport system (i.e., the sampling lines only), the cutoff diameter of the Falcon aerosol inlet (i.e., the effect of the inlet only), and the combined effect of the inlet and sampling lines.

A traffic-induced shift of ultrafine particle sources under COVID-19 soft lockdown in a subtropical urban area

During the unprecedented COVID-19 city lockdown, a unique opportunity arose to dissect the intricate dynamics of urban air quality, focusing on ultrafine particles (UFPs) and volatile organic compounds (VOCs). This study delves into the nuanced interplay between traffic patterns and UFP emissions in a subtropical urban setting during the spring-summer transition of 2021. Leveraging meticulous roadside measurements near a traffic nexus, our investigation unravels the intricate relationship between particle number size distribution (PNSD), VOCs mixing ratios, and detailed vehicle activity metrics. The soft lockdown era, marked by a 20–27% dip in overall traffic yet a surprising surge in early morning motorcycle activity, presented a natural experiment. We observed a consequential shift in the urban aerosol regime: the decrease in primary emissions from traffic substantially amplified the role of aged particles and secondary aerosols. This shift was particularly pronounced under stagnant atmospheric conditions, where reduced dilution exacerbated the influence of alternative emission sources, notably solvent evaporation, and was further accentuated with the resumption of normal traffic flows. A distinct seasonal trend emerged as warmer months approached, with aromatic VOCs such as toluene, ethylbenzene, and xylene not only increasing but also significantly contributing to more frequent particle growth events. These findings spotlight the criticality of targeted strategies at traffic hotspots, especially during periods susceptible to weak atmospheric dilution, to curb UFP and precursor emissions effectively. As we stand at the cusp of widespread vehicle electrification, this study underscores the imperative of a holistic approach to urban air quality management, embracing the complexities of primary emission reductions and the resultant shifts in atmospheric chemistry.

Amazonian aerosol size distributions in a lognormal phase space: characteristics and trajectories

Abstract. This study introduces a first glance at Amazonian aerosols in the N–Dg–σ phase space. Aerosol data, measured from May 2021 to April 2022 at the Amazon Tall Tower Observatory (ATTO), were fitted by a multi-modal lognormal function and separated into three modes: the sub-50 nm, the Aitken (50–100 nm), and the accumulation modes. The fit results were then evaluated in the N–Dg–σ phase space, which represents a three-dimensional space based on the three lognormal fit parameters. These parameters represent, for a given mode i, the number concentration (Ni), the median geometric diameter (Dg,i), and the geometric standard deviation (σi). Each state of a particle number size distribution (PNSD) is represented by a single dot in this space, while a collection of dots shows the delimitation of all PNSD states under given conditions. The connections in ensembles of data points show trajectories caused by pseudo-forces, such as precipitation regimes and vertical movement. We showed that all three modes have a preferential arrangement in this space, reflecting their intrinsic behaviors in the atmosphere. These arrangements were interpreted as volumetric figures, elucidating the boundaries of each mode. Time trajectories in seasonal and diurnal cycles revealed that fits with the sub-20 nm mode are associated with rainfall events that happen in the morning and in the afternoon. But in the morning they grow rapidly into the Aitken mode, and in the afternoon they remain below 50 nm. Also, certain modes demonstrated well-defined curves in the space, e.g., the seasonal trajectory of the accumulation mode follows an ellipsoid, while the diurnal cycle of the sub-50 nm mode in the dry season follows a linear trajectory. As an effect of the precipitation on the PNSDs and vice versa, N and Dg were found to increase for the sub-50 nm mode and to decrease for the Aitken and accumulation modes after the precipitation peak. Afternoons with precipitation were preceded by mornings with larger particles of the accumulation mode, whose Dg was ∼ 10 nm larger than in days without precipitation. Nevertheless, this large Dg in the morning seems to influence subsequent rainfall only in the dry season, while in the wet season both N and Dg seem to have the same weight of influence. The observed patterns of the PNSDs in the N–Dg–σ phase space showed to be a promising tool for the characterization of atmospheric aerosols, to contribute to our understanding of the main processes in aerosol–cloud interactions, and to open new perspectives on aerosol parameterizations and model validation.

A bipolar SMPS network for measuring atmospheric aerosols using natural air ions

To study atmospheric aerosols, it is essential to build networks that are continuously monitoring particle number size distribution (PNSD). PNSDs are often measured using electrical mobility spectrometers such as scanning mobility particle sizer (SMPS) which includes a neutralizer that conditions the charge state of particles to the pre-assumed distributions. During long-term atmospheric measurement, the charge state can deviate from these assumed values. Measuring both positively and negatively charged particles using a bipolar SMPS helps to capture the variations in aerosol charge state. In this study, we set up a network of bipolar SMPSs at three urban sites and three suburban sites in six Chinese cities. Removing the conventional neutralizer, the bipolar SMPS utilizes the natural aerosol charging process by atmospheric ions. Newly developed aerosol classifiers and detectors were used. Harmonized quality assurance procedures were adopted to assure the performance and the data quality, including laboratory calibrations and intercomparisons, maintenance and monitoring during field measurements, and data inversion and validation. PNSDs are effectively measured by bipolar SMPSs using natural charging process at all six sites. During six months of field measurement in these sites, ion mobility ratios fluctuate significantly while the daily averaged values are stable around 1.0. Particle number concentrations integrated from PNSDs are consistent with those directly measured by the detectors (within a variation of 10%).

Long term trends in source apportioned particle number concentrations in Rochester NY

During the past two decades, efforts have been made to further reduce particulate air pollution across New York State through various Federal and State policy implementations. Air quality has also been affected by economic drivers like the 2007–2009 recession and changing costs for different approaches to electricity generation. Prior work has focused on particulate matter with aerodynamic diameter ≤2.5 μm. However, there is also interest in the effects of ultrafine particles on health and the environment and analyses of changes in particle number concentrations (PNCs) are also of interest to assess the impacts of changing emissions. Particle number size distributions have been measured since 2005. Prior apportionments have been limited to seasonal analyses over a limited number of years because of software limitations. Thus, it has not been possible to perform trend analyses on the source-specific PNCs. Recent development have now permitted the analysis of larger data sets using Positive Matrix Factorization (PMF) including its diagnostics. Thus, this study separated and analyzed the hourly averaged size distributions from 2005 to 2019 into two data sets; October to March and April to September. Six factors were resolved for both data sets with sources identified as nucleation, traffic 1, traffic 2, fresh secondary inorganic aerosol (SIA), aged SIA, and O3-rich aerosol. The resulting source-specific PNCs were combined to provide continuous data sets and analyzed for trends. The trends were then examined with respect to the implementation of regulations and the timing of economic drivers. Nucleation was strongly reduced by the requirement of ultralow (<15 ppm) sulfur on-road diesel fuel in 2006. Secondary inorganic particles and O3-rich PNCs show strong summer peaks. Aged SIA was constant and then declined substantially in 2015 but rose in 2019. Traffic 1 and 2 have steadily declined bur rose in 2019.

Long-Term Characterization of Indoor Air Quality at a Research Area Building: Comparing Reference Instruments and Low-Cost Sensors

Indoor particle number size distribution (0.3-10 μm), equivalent black carbon (eBC), and Ångström absorption exponent (AAE) data were collected in real conditions, over a ten-month period at a research area building, in a semirural site, to characterize indoor aerosol loading. Additionally, during the campaign, emissions from four indoor sources commonly used at the site (incense, traditional cigarettes, electronic cigarettes, and heat-not-burn products) were studied during short-term experiments with the support of ultrafine particle (UFP) monitoring. Two particle low-cost sensors (PM LCS), Sensirion SPS30 (0.3-10 μm), were evaluated in the long-term campaign and during fast emission processes, to assess their accuracy and reliability. Penetration and infiltration of both fine and coarse particles from outdoor traffic, domestic heating, and dust resuspension were inferred as the main sources of indoor aerosols on a long-term basis. Moreover, long-range transported dust aerosols were found to influence indoor coarse number concentration. Among the source events, heat-not-burn (HNB) product resulted in the lowest effect on indoor air quality, whereas the highest AAE values from incense and traditional cigarettes suggest the brown carbon (BrC) production. The highest emission of UFP was caused by electronic cigarettes (e-cig), which spanned particles from the ultrafine to the coarse fractions. This was likely due to the release of metal and silicate from the coil. Analysis of number size distributions of the four experiments revealed the emission of fine particles (0.3-1 μm) and super micron particles. SPS30s performance was satisfactory in terms of accuracy, precision, and durability, indicating that these devices are suitable for monitoring indoor air quality. Additionally, the two PM LCS were able to detect all simulated fast emission sources.

Inter-annual trends of ultrafine particles in urban Europe

Ultrafine particles (UFP, those with diameters ≤ 100 nm), have been reported to potentially penetrate deeply into the respiratory system, translocate through the alveoli, and affect various organs, potentially correlating with increased mortality. The aim of this study is to assess long-term trends (5–11 years) in mostly urban UFP concentrations based on measurements of particle number size distributions (PNSD). Additionally, concentrations of other pollutants and meteorological variables were evaluated to support the interpretations. PNSD datasets from 12 urban background (UB), 5 traffic (TR), 3 suburban background (SUB) and 1 regional background (RB) sites in 15 European cities and 1 in the USA were evaluated. The non-parametric Theil-Sen’s method was used to detect monotonic trends. Meta-analyses were carried out to assess the overall trends and those for different environments. The results showed significant decreases in NO, NO2, BC, CO, and particle concentrations in the Aitken (25–100 nm) and the Accumulation (100–800 nm) modes, suggesting a positive impact of the implementation of EURO 5/V and 6/VI vehicle standards on European air quality. The growing use of Diesel Particle Filters (DPFs) might also have clearly reduced exhaust emissions of BC, PM, and the Aitken and Accumulation mode particles. However, as reported by prior studies, there remains an issue of poor control of Nucleation mode particles (smaller than 25 nm), which are not fully reduced with current DPFs, without emission controls for semi-volatile organic compounds, and might have different origins than road traffic. Thus, contrasting trends for Nucleation mode particles were obtained across the cities studied. This mode also affected the UFP and total PNC trends because of the high proportion of Nucleation mode particles in both concentration ranges. It was also found that the urban temperature increasing trends might have also influenced those of PNC, Nucleation and Aitken modes.

Analysis of gaseous emission and particle number size distributions in metal casting processes with binder jetting moulds

The impact on indoor air quality during metal casting processes using the 3D printing (3DP) binder jetting technique to manufacture moulds is analyzed in this research. This study investigates the particle size distribution and gas concentration during the manufacturing stages of 3DP moulds, with focus on particle deposition in the human respiratory system. The goal is to understand the risks associated with particle and gas emissions in binder jetting 3D printing, and thus improve worker safety. The results indicate that particle emission rates are lowest during printing (0.01 1011particles min−1) but increase during post-processing and melting-pouring phases (3.07 1011 particles min−1). During melting and pouring, the emission of particles was mainly in the range 7.9–71 nm, with values 10 times higher than in the previous phases. The study calculates the deposition of inhaled particles in different parts of the respiratory tract and reveals a 2.39 times higher extrathoracic mass deposition during 3DP mould manufacturing stages compared to melting-pouring stages. Additionally, alveolar mass deposition is higher during melting-pouring stages due to an increase in ultrafine emission rates. The study emphasizes the importance of insulation equipment and workplace ventilation in indoor spaces, particularly during heating processes that generate ultrafine particles through nucleation, so that health risks can be mitigated.

Influence of a large commercial airport on the ultrafine particle number concentration in a distant residential area under different wind conditions and the impact of the COVID-19 pandemic

Exposure to ultrafine particles has a significant influence on human health. In regions with large commercial airports, air traffic and ground operations can represent a potential particle source. The particle number concentration was measured in a low-traffic residential area about 7 km from Frankfurt Airport with a Condensation Particle Counter in a long-term study. In addition, the particle number size distribution was determined using a Fast Mobility Particle Sizer.The particle number concentrations showed high variations over the entire measuring period and even within a single day. A maximum 24 h-mean of 24,120 cm−3 was detected. Very high particle number concentrations were in particular measured when the wind came from the direction of the airport. In this case, the particle number size distribution showed a maximum in the particle size range between 5 and 15 nm. Particles produced by combustion in jet engines typically have this size range and a high potential to be deposited in the alveoli. During a period with high air traffic volume, significantly higher particle number concentrations could be measured than during a period with low air traffic volume, as in the COVID-19 pandemic.A large commercial airport thus has the potential to lead to a high particle number concentration even in a distant residential area. Due to the high particle number concentrations, the critical particle size, and strong concentration fluctuations, long-term measurements are essential for a realistic exposure analysis.

Analysing the impact of day-night road traffic variation on ultrafine particle number size distribution and concentration at an urban site in the megacity Delhi

Air quality is the biggest threat in many urban cities globally. This study measured and analyzed aerosol number size distribution between 10 to 1090 nm in the megacity Delhi during 2022. The study examined the particle number concentration in the ultrafine (<100 nm) and accumulation (100–1000 nm) ranges during day and night in terms of source's intensity, emission patterns and local meteorological conditions. Nucleation mode particles (Nnuc, 10–30 nm) contributed ∼50 % during daytime in summer periods due to increased fresh traffic emissions. In the daytime, particle concentration was dominated by smaller sizes, such as Nnuc and Aitken mode particles (Natk, 30–100 nm), while in the nighttime, the particles were found in Aitken and Accumulation (Nacc, 100–1000 nm) modes. Nnuc and Natk were reduced by ∼45 % and 4 % at night, while Nacc increased by ∼34 %. The mean normalized aerosol number size distribution confirmed these findings, showing clearly that Nnuc dominated during the daytime, especially during peak rush hours, and during the night particles concentration was increased up to the sizes of 300 nm particles. The aerosol number size distribution and the changes experienced in the percentage of the concentration of the different particle size ranges highlight the role of engine exhaust emissions in the atmospheric aerosol population in urban areas. The findings of the study help to identify the different source's intensity and behavior during day and nighttime, which can be used for policy formulation and decision-making to mitigate air quality and its associated health impacts.

The investigation of diesel soot emission using instrument combination of multi-wavelength photoacoustic spectroscopy and scanning mobility particle sizer

The parallel measurements of wavelength dependent optical absorption, particle number size distribution have made by a multi wavelength photoacoustic spectrometer (4λ-PAS) and scanning mobility particle sizer (SMPS) respectively at different modes of a diesel engine using two different types of fuel. The thermal evolution of the emission was also investigated using posterior temperature treatment of emission. The bimodal size distribution of emitted particles at a set reference temperature has been observed regardless of the applied fuel at idle. However, the emitted particulate assembly had lognormal size distribution falls into the accumulation mode at all other defined engine modes and both fuel types. The total number- and volume concentration (TNC and TVC) showed retrograde tendency with the increasing torque and rpm independently of the applied fuel types. The TNC values decreased up to 50% for both fuels with engine operation changes from idle engine mode(em#1) to low engine mode(em#2). With further increase in torque and rpm of engine, the change in TNC is negligible. On the other hand, the TVC remains more or less the same for idle to low engine mode transition and increased more than 60% for high mode (em#3) transition. The Optical Absorption Coefficient (OAC) values measured at the operational wavelengths of the 4λ-PAS instrument decreased at all wavelengths with increasing rpm and torque. The wavelength dependency quantified by Aerosol Ängström Exponent (AAE) was applied here for qualitative analysis of the carbonaceous emission and showed decreased values towards the higher engine speed and torque output of the engine. The proposed technique can be used as real-time, precise and accurate measurement of light absorption by DPM aerosols, which opens up novel possibilities for the volatility and thermal evolution investigation of diesel emissions.

Two new multirotor uncrewed aerial vehicles (UAVs) for glaciogenic cloud seeding and aerosol measurements within the CLOUDLAB project

Abstract. Uncrewed aerial vehicles (UAVs) have become widely used in a range of atmospheric science research applications. Because of their small size, flexible range of motion, adaptability, and low cost, multirotor UAVs are especially well-suited for probing the lower atmosphere. However, their use so far has been limited to conditions outside of clouds, first because of the difficulty of flying beyond visual line of sight and second because of the challenge of flying in icing conditions in supercooled clouds. Here, we present two UAVs for cloud microphysical research: one UAV (the measurement UAV) equipped with a Portable Optical Particle Spectrometer (POPS) and meteorological sensors to probe the aerosol and meteorological properties in the boundary layer and one UAV (the seeding UAV) equipped with seeding flares to produce a plume of particles that can nucleate ice in supercooled clouds. A propeller heating mechanism on both UAVs allows for operating in supercooled clouds with icing conditions. These UAVs are an integral part of the CLOUDLAB project in which glaciogenic cloud seeding of supercooled low stratus clouds is utilized for studying aerosol–cloud interactions and ice crystal formation and growth. In this paper, we first show validations of the POPS on board the measurement UAV, demonstrating that the rotor turbulence has a small effect on measured particle number concentrations. We then exemplify the applicability for profiling the planetary boundary layer, as well as for sampling and characterizing aerosol plumes, in this case, the seeding plume. We also present a new method for filtering out high-concentration data to ensure good data quality of POPS. We explain the different flight patterns that are possible for both UAVs, namely horizontal or vertical leg patterns or hovering, with an extensive and flexible parameter space for designing the flight patterns according to our scientific goals. Finally, we show two examples of seeding experiments: first characterizing an out-of-cloud seeding plume with the measurement UAV flying horizontal transects through the plume and, second, characterizing an in-cloud seeding plume with downstream measurements from a POPS and a holographic imager mounted on a tethered balloon. Particle number concentrations and particle number size distributions of the seeding plume from the experiments reveal that we can successfully produce and measure the seeding plume, both in-cloud (with accompanying elevated ice crystal number concentrations) and out-of-cloud. The methods presented here will be useful for probing the lower atmosphere, for characterizing aerosol plumes, and for deepening our cloud microphysical understanding through cloud seeding experiments, all of which have the potential to benefit the atmospheric science community.

Evaluation of a Partector Pro for atmospheric particle number size distribution and number concentration measurements at an urban background site

Abstract. Particle number size distributions, total number concentrations and mean particle sizes have been measured for 70 d at an urban background site in Mülheim-Styrum, Germany, with a handheld Partector Pro of the first generation and a TSI mobility particle size spectrometer (MPSS). The aim of the study was to evaluate the performance of the Partector Pro against the MPSS. The results show that the size distributions, measured with the Partector Pro, agree with the MPSS mostly within ± 25 % for particle sizes between 10 and 113.5 nm, whereas higher, systematic differences were observed for larger particles. The measurement accuracy was shown to be dependent on the geometric mean diameter and the geometric standard deviation of the aerosol. Best results were found for the most abundant size distributions with geometric mean particle diameters ≥ 30 nm and geometric standard deviations larger than 1.8. The total number concentration, measured by the Partector Pro, was found to be in excellent agreement with the MPSS with a slope of the linear fit of 0.9977 and a regression coefficient of R2=0.9956. The agreement of the geometric mean particle diameter, determined with the Partector Pro and the MPSS was good but moderately dependent on the particle size distribution. For mean particle sizes between 20 and 50 nm, the bias was within ±15 %. Higher deviations of up to 30 % were observed when the geometric mean particle sizes exceeded 70 nm and when the geometric standard deviations exceeded approximately 2.7.

Source apportionment of fine and ultrafine particle number concentrations in a major city of the Eastern Mediterranean

Ultrafine particles (UFP) are recognized as an emerging pollutant able to induce serious health effects. However, quantitative information regarding the contributions of UFP sources is generally limited. This study evaluates statistical (k-means clustering) and receptor models (Positive Matrix Factorization - PMF) using particle number size distributions (PNSD), along with chemical speciation data, measured at an urban background supersite in Athens, Greece, aiming to characterize their sources. PNSD measurements (10–487 nm) were performed during three distinct periods (warm, cold, and lockdown cold). Traffic and residential biomass burning (BB) produced high UFP number concentrations (NUFP) in the cold period (+107 % compared to summer), while the lockdown restrictions reduced NUFP (−42 %). The five groups produced by cluster analysis that were common among periods were linked to high- and low-traffic, new particle formation (NPF), urban background and regional aerosols. PMF source apportionment identified 5 and 6 factors during warm and cold periods, respectively, indicating that traffic particles dominated NUFP (64–78 % in all periods), while accumulation-mode particles and volume concentrations were controlled by processed aerosol, and especially in the cold periods by BB emissions. A nucleation factor linked to NPF contributed 7–11 % to NUFP. Comparing the two cold periods (business-as-usual, lockdown), important lockdown reductions (−46 %) were seen for fresh traffic contributions to total number concentration (Ntotal). The impact of the source attributed to NPF also eroded (−41 % for Ntotal). Due to the large reduction (−47 % for Ntotal) observed also for the BB source during the lockdown (reduced wood usage due to a milder winter), the relative contributions of all sources did not change considerably (fractional reductions <7 % for Ntotal). The quantitative results, bolstered by source apportionment combining PNSD and online chemical composition measurements, indicate the potential to constrain UFP levels by regulating traffic and residential emissions, with a large upside for population exposure control.

Significant spatial gradients in new particle formation frequency in Greece during summer

Abstract. Extensive continuous particle number size distribution measurements took place during two summers (2020 and 2021) at 11 sites in Greece for the investigation of the frequency and the spatial extent of new particle formation (NPF). The study area is characterized by high solar intensity and fast photochemistry and has moderate to low fine particulate matter levels during the summer. The average PM2.5 levels were relatively uniform across the examined sites. The NPF frequency during summer varied from close to zero in the southwestern parts of Greece to more than 60 % in the northern, central, and eastern regions. The mean particle growth rate for each station varied between 3.4 and 8 nm h−1, with an average rate of 5.7 nm h−1. At most of the sites there was no statistical difference in the condensation sink between NPF event and non-event days, while lower relative humidity was observed during the events. The high-NPF-frequency sites in the north and northeast were in close proximity to both coal-fired power plants (high emissions of SO2) and agricultural areas with some of the highest ammonia emissions in the country. The southern and western parts of Greece, where NPF was infrequent, were characterized by low ammonia emissions, while moderate levels of sulfuric acid were estimated (107 molec. cm−3) in the west. Although the emissions of biogenic volatile organic compounds were higher in western and southern sectors, they did not appear to lead to enhanced frequency of NPF. The infrequent events at these sites occurred when the air masses had spent a few hours over areas with agricultural activities and thus elevated ammonia emissions. Air masses arriving at the sites directly from the sea were not connected with atmospheric NPF. These results support the hypothesis that ammonia and/or amines limit new particle formation in the study area.

Particle Number Size Distribution in Three Different Microenvironments of London

We estimated the particle number distributions (PNDs), particle number concentrations (PNCs), physicochemical characteristics, meteorological effects, and respiratory deposition doses (RDD) in the human respiratory tract for three different particle modes: nucleation (N6–30), accumulation (N30–300), and coarse (N300–10,000) modes. This study was conducted in three different microenvironments (MEs) in London (indoor, IN; traffic intersection, TI; park, PK) measuring particles in the range of 6 nm–10,000 nm using an electrical low-pressure impactor (ELPI+). Mean PNCs were 1.68 ± 1.03 × 104 #cm−3, 7.00 ± 18.96 × 104 #cm−3, and 0.76 ± 0.95 × 104 #cm−3 at IN, TI, and PK, respectively. The PNDs were high for nucleation-mode particles at the TI site, especially during peak traffic hours. Wind speeds ranging from 0 to 6 ms−1 exhibit higher PNCs for nucleation- and accumulation-mode particles at TI and PK sites. Physicochemical characterisation shows trace metals, including Fe, O, and inorganic elements, that were embedded in a matrix of organic material in some samples. Alveolar RDD was higher for the nucleation and accumulation modes than the coarse-mode particles. The chemical signatures from the physicochemical characterisation indicate the varied sources at different MEs. These findings enhance our understanding of the different particle profiles at each ME and should help devise ways of reducing personal exposure at each ME.

In situ measurements of perturbations to stratospheric aerosol and modeled ozone and radiative impacts following the 2021 La Soufrière eruption

Abstract. Stratospheric aerosols play important roles in Earth's radiative budget and in heterogeneous chemistry. Volcanic eruptions modulate the stratospheric aerosol layer by injecting particles and particle precursors like sulfur dioxide (SO2) into the stratosphere. Beginning on 9 April 2021, La Soufrière erupted, injecting SO2 into the tropical upper troposphere and lower stratosphere, yielding a peak SO2 loading of 0.3–0.4 Tg. The resulting volcanic aerosol plumes dispersed predominately over the Northern Hemisphere (NH), as indicated by the CALIOP/CALIPSO satellite observations and model simulations. From June to August 2021 and May to July 2022, the NASA ER-2 high-altitude aircraft extensively sampled the stratospheric aerosol layer over the continental United States during the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) mission. These in situ aerosol measurements provide detailed insights into the number concentration, size distribution, and spatiotemporal variations of particles within volcanic plumes. Notably, aerosol surface area density and number density in 2021 were enhanced by a factor of 2–4 between 380–500 K potential temperature compared to the 2022 DCOTSS observations, which were minimally influenced by volcanic activity. Within the volcanic plume, the observed aerosol number density exhibited significant meridional and zonal variations, while the mode and shape of aerosol size distributions did not vary. The La Soufrière eruption led to an increase in the number concentration of small particles (&lt;400 nm), resulting in a smaller aerosol effective diameter during the summer of 2021 compared to the baseline conditions in the summer of 2022, as observed in regular ER-2 profiles over Salina, Kansas. A similar reduction in aerosol effective diameter was not observed in ER-2 profiles over Palmdale, California, possibly due to the values that were already smaller in that region during the limited sampling period in 2022. Additionally, we modeled the eruption with the SOCOL-AERv2 aerosol–chemistry–climate model. The modeled aerosol enhancement aligned well with DCOTSS observations, although the direct comparison was complicated by issues related to the model's background aerosol burden. This study indicates that the La Soufrière eruption contributed approximately 0.6 % to Arctic and Antarctic ozone column depletion in both 2021 and 2022, which is well within the range of natural variability. The modeled top-of-atmosphere 1-year global average radiative forcing was −0.08 W m−2 clear-sky and −0.04 W m−2 all-sky. The radiative effects were concentrated in the tropics and NH midlatitudes and diminished to near-baseline levels after 1 year.

A seven-year-based characterization of aerosol light scattering properties at a rural central European site

Our study investigates the temporal variability of aerosol light scattering properties measured at three wavelengths (total scattering coefficient, backscattering coefficient, Ångström scattering exponent, hemispheric backscattering ratio and asymmetry parameter) at the rural background site of the National Atmospheric Observatory Košetice over a period of over seven years (2012–2019). The influence of fog and cloudiness on aerosol light scattering properties (ASP), together with their comparison to particle number size distribution was also investigated. The overall medians of total scattering (σsp) and backscattering coefficient (σbsp), hemispheric backscattering ratio (b) and asymmetry parameter (g) measured at 550 nm and Ångström scattering exponent (SAE_450/700) were 35.20 Mm−1, 5.07 Mm−1, 0.14 and 0.57 and 1.82, respectively. σsp and g decreased by 2.05 Mm−1/year, and 0.009/year, respectively, whereas b increased by 0.004/year. The selected aerosol properties were strongly correlated with particle number, mass, area and volume concentrations in the 200–800 nm mode. A decrease in SAE_450/700 implies a shift towards larger particle sizes, and evolutions in b and g suggest a higher backscattering portion to total scattering. The highest σsp and σbsp levels were observed in the cold seasons together with higher concentrations of air pollutants (carbonaceous aerosol, SO2 and NOx). This could be explained by enhanced emissions from human activities such as domestic heating combined with the higher stability of the atmosphere (poor atmospheric dispersion). In the summer, decreases in particle size and higher rates of backscatter fraction were attributed to secondary organic aerosol (SOA) formation. The accumulation mode showed the strongest aerosol scattering potential, with SAE_450/700 values < 2. Aerosol light scattering was significantly higher during overcast and foggy days compared to fine, cloudy, partly cloudy and no-fog days, possibly due to the particle hygroscopic growth under high relative humidity (shift of particle size towards larger sizes), which in turn can lead to a lower aerosol backscattering fraction. Source identification linked the changes in ASP to the synoptic situation over Europe rather than to specific sources of pollution.