Aerosol Particle Number Size Distributions Research Articles

Exploring the use of ground-based remote sensing to identify new particle formation events: A case study in the Beijing area

New Particle Formation (NPF) is an important process of secondary aerosol production in the atmosphere, which has significant impacts on the Earth's radiation balance, air quality, and climate change. In this study, we develop a method to identify NPF events based on ground-based remote sensing. We propose a proxy to characterize NPF events utilizing ground-based remote sensing of gaseous precursors and aerosol optical depth (AOD). This proxy is applied to identify the NPF events in Beijing in the winter of 2022 and tested by comparison with in-situ observations of aerosol particle number size distributions (PNSD) from SMPS. The comparison shows that the NPF events for regional nucleation can be identified effectively when the threshold for sulfur dioxide and organic gases (i.e. formaldehyde) are determined as 0.44 × 10−4 and 1.07 × 10−4. Based on these thresholds, the NPF events can be identified at a high percentage (84 %) compared with in-situ observations. The relationship between identification of NPF events and meteorological conditions shows that NPF events in Beijing winter occurred more frequently under weather conditions with north-west wind direction, high wind speed and low relative humidity.

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.

Optical Properties and Refractive Index of Wintertime Aerosol at a Highly Polluted North‐Indian Site

AbstractEstimation of aerosol radiative forcing continues to suffer from large uncertainties, partially from a lack of observations of aerosol optical properties. Limited measurements of the atmospheric aerosol imaginary refractive index (iRI) have been made, especially in some of the world's most polluted regions. In this study, we measured aerosol optical and micro‐physical properties at a regional site, Rohtak, India, representative of polluted cities in the Indo‐Gangetic plains in northern India. The average PM2.5 measured during the campaign was 163 μg/m3 with a single‐scatter albedo of 0.7, indicating the presence of strongly absorbing aerosol components. Measurements of aerosol absorption, scattering, and particle number size distributions were used to estimate the effective refractive index using an established Mie inversion technique. The calculated iRI was spectrally invariant in the visible region with values ranging between 0.076 and 0.145. Brown carbon absorption, estimated using an existing Mie optimization method, ranged 34–88 Mm−1, with strongly absorbing mass absorption cross‐sections (∼1.9 m2/g). Higher iRI were observed during periods with higher brown carbon absorption, which are likely directly emitted from combustion sources. Low volatility organic carbon fractions dominated during these periods, with likely persistence of atmospheric absorption. The iRI values are at the upper end of previously reported ranges of urban aerosol iRI. In a sensitivity analysis to measured parameters, the absorption had the dominant effect on estimated iRI. Measured single scatter albedos, were lower than those from climate model simulations over the region, demonstrating the need for intrinsic property measurements to evaluate and constrain climate models.

A full year of aerosol size distribution data from the central Arctic under an extreme positive Arctic Oscillation: insights from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition

Abstract. The Arctic environment is rapidly changing due to accelerated warming in the region. The warming trend is driving a decline in sea ice extent, which thereby enhances feedback loops in the surface energy budget in the Arctic. Arctic aerosols play an important role in the radiative balance and hence the climate response in the region, yet direct observations of aerosols over the Arctic Ocean are limited. In this study, we investigate the annual cycle in the aerosol particle number size distribution (PNSD), particle number concentration (PNC), and black carbon (BC) mass concentration in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. This is the first continuous, year-long data set of aerosol PNSD ever collected over the sea ice in the central Arctic Ocean. We use a k-means cluster analysis, FLEXPART simulations, and inverse modeling to evaluate seasonal patterns and the influence of different source regions on the Arctic aerosol population. Furthermore, we compare the aerosol observations to land-based sites across the Arctic, using both long-term measurements and observations during the year of the MOSAiC expedition (2019–2020), to investigate interannual variability and to give context to the aerosol characteristics from within the central Arctic. Our analysis identifies that, overall, the central Arctic exhibits typical seasonal patterns of aerosols, including anthropogenic influence from Arctic haze in winter and secondary aerosol processes in summer. The seasonal pattern corresponds to the global radiation, surface air temperature, and timing of sea ice melting/freezing, which drive changes in transport patterns and secondary aerosol processes. In winter, the Norilsk region in Russia/Siberia was the dominant source of Arctic haze signals in the PNSD and BC observations, which contributed to higher accumulation-mode PNC and BC mass concentrations in the central Arctic than at land-based observatories. We also show that the wintertime Arctic Oscillation (AO) phenomenon, which was reported to achieve a record-breaking positive phase during January–March 2020, explains the unusual timing and magnitude of Arctic haze across the Arctic region compared to longer-term observations. In summer, the aerosol PNCs of the nucleation and Aitken modes are enhanced; however, concentrations were notably lower in the central Arctic over the ice pack than at land-based sites further south. The analysis presented herein provides a current snapshot of Arctic aerosol processes in an environment that is characterized by rapid changes, which will be crucial for improving climate model predictions, understanding linkages between different environmental processes, and investigating the impacts of climate change in future Arctic aerosol studies.

Measurement report: A multi-year study on the impacts of Chinese New Year celebrations on air quality in Beijing, China

Abstract. This study investigates the influence of the Chinese New Year (CNY) celebrations on local air quality in Beijing from 2013 through 2019. CNY celebrations include burning of fireworks and firecrackers, which consequently has a significant short-term impact on local air quality. In this study, we bring together comprehensive observations at the newly constructed Aerosol and Haze Laboratory at Beijing University of Chemical Technology – West Campus (BUCT-AHL) and hourly measurements from 12 Chinese government air quality measurement stations throughout the Beijing metropolitan area. These datasets are used together to provide a detailed analysis of air quality during the CNY over multiple years, during which the city of Beijing prohibited the use of fireworks and firecrackers in an effort to reduce air pollution before CNY 2018. Datasets used in this study include particulate matter mass concentrations (PM2.5 and PM10), trace gases (NOx, SO2, O3, and CO), and meteorological variables for 2013–2019; aerosol particle size distributions; and concentrations of sulfuric acid and black carbon for 2018 and 2019. Studying the CNY over several years, which has rarely been done in previous studies, can show trends and effects of societal and policy changes over time, and the results can be applied to study problems and potential solutions of air pollution resulting from holiday celebrations. Our results show that during the 2018 CNY, air pollutant concentrations peaked during the CNY night (for example, PM2.5 reached a peak around midnight of over 250 µg cm−3, compared to values of less than 50 µg cm−3 earlier in the day). The pollutants with the most notable spikes were sulfur dioxide, particulate matter, and black carbon, which are emitted in burning of fireworks and firecrackers. Sulfuric acid concentration followed the sulfur dioxide concentration and showed elevated overnight concentration. Analysis of aerosol particle number size distribution showed direct emissions of particles with diameters around 100 nm in relation to firework burning. During the 2019 CNY, the pollution levels were somewhat lower (PM2.5 peaking at around 150 µg cm−3 on CNY compared to values around 100 µg cm−3 earlier in the day), and only minor peaks related to firework burning were observed. During both CNYs 2018 and 2019 secondary aerosol formation in terms of particle growth was observed. Meteorological conditions were comparable between these 2 years, suggesting that CNY-related emissions were less in 2019 compared to 2018. During the 7-year study period, it appears that there has been a general decrease in CNY-related emissions since 2016. For example, the peak in PM2.5 in 2016 was over 600 µg cm−3, and in the years following, the peak was less each year, with a peak around 150 µg cm−3 in 2019. This is indicative of the restrictions and public awareness of the air quality issues having a positive effect on improving air quality during the CNY. Going into the future, long-term observations will offer confirmation for these trends.

Investigation of new particle formation mechanisms and aerosol processes at Marambio Station, Antarctic Peninsula

Abstract. Understanding chemical processes leading to the formation of atmospheric aerosol particles is crucial to improve our capabilities in predicting the future climate. However, those mechanisms are still inadequately characterized, especially in polar regions. In this study, we report observations of neutral and charged aerosol precursor molecules and chemical cluster composition (qualitatively and quantitatively), as well as air ions and aerosol particle number concentrations and size distributions from the Marambio research station (64∘15′ S, 56∘38′ W), located north of the Antarctic Peninsula. We conducted measurements during the austral summer, between 15 January and 25 February 2018. The scope of this study is to characterize new particle formation (NPF) event parameters and connect our observations of gas-phase compounds with the formation of secondary aerosols to resolve the nucleation mechanisms at the molecular scale. NPF occurred on 40 % of measurement days. All NPF events were observed during days with high solar radiation, mostly with above-freezing temperatures and with low relative humidity. The averaged formation rate for 3 nm particles (J3) was 0.686 cm−3 s−1, and the average particle growth rate (GR3.8–12 nm) was 4.2 nm h−1. Analysis of neutral aerosol precursor molecules showed measurable concentrations of iodic acid (IA), sulfuric acid (SA), and methane sulfonic acid (MSA) throughout the entire measurement period with significant increase in MSA and SA concentrations during NPF events. We highlight SA as a key contributor to NPF processes, while IA and MSA likely only contribute to particle growth. Mechanistically, anion clusters containing ammonia and/or dimethylamine (DMA) and SA were identified, suggesting significant concentration of ammonia and DMA as well. Those species are likely contributing to NPF events since SA alone is not sufficient to explain observed nucleation rates. Here, we provide evidence of the marine origin of the measured chemical precursors and discuss their potential contribution to the aerosol phase.

New particle formation in coastal New Zealand with a focus on open-ocean air masses

Abstract. Even though oceans cover the majority of the Earth, most aerosol measurements are from continental sites. We measured aerosol particle number size distribution at Baring Head, in coastal New Zealand, over a total period of 10 months to study aerosol properties and new particle formation, with a special focus on aerosol formation in open-ocean air masses. Particle concentrations were higher in land-influenced air compared to clean marine air in all size classes, from sub-10 nm to cloud condensation nuclei sizes. When classifying the particle number size distributions with traditional methods designed for continental sites, new particle formation was observed at the station throughout the year with an average event frequency of 23 %. While most of these traditional event days had some land influence, we also observed particle growth starting from nucleation mode in 16 % of the data in clean marine air, and at least part of this growth was connected to nucleation in the marine boundary layer. Sub-10 nm particles accounted for 29 % of the total aerosol number concentration of particles larger than 1 nm in marine air during the spring. This shows that nucleation in marine air is frequent enough to influence the total particle concentration. Particle formation in land-influenced air was more intense and had on average higher growth rates than what was found for marine air. Particle formation and primary emissions increased particle number concentrations as a function of time spent over land during the first 1–2 d. After this, nucleation seems to start getting suppressed by the pre-existing particle population, but accumulation mode particle concentration keeps increasing, likely due to primary particle emissions. Further work showed that traditional NPF events were favoured by sunny conditions with low relative humidity and wind speeds. In marine air, formation of sub-10 nm particles was favoured by low temperatures, relative humidity, and wind speeds and could happen even during the night. Our future work will study the mechanisms responsible for particle formation at Baring Head with a focus on different chemical precursor species. This study sheds light on both new particle formation in open-ocean air masses coming from the Southern Ocean and local aerosol properties in New Zealand.

Analysis of aerosol particle number size distribution and source attribution at three megacities in China

Air pollution has been a major concern in China, especially in densely populated megacities. Particulate pollutants, generally known as aerosols, have sizes that range widely and complex physical and chemical compositions with high spatiotemporal variabilities. We have conducted a series of experiments using the same comprehensive observation system, measuring various aerosol properties in the three megacities of Beijing, Shanghai, and Guangzhou. Although there are differences in the total particle number concentration and particle number size distribution among the three sites due to differences in emission sources and sampling seasons, a high proportion of ultrafine particles was observed in all cities, i.e., 86.33%, 88.34%, and 81.1%, respectively. The high particle number concentration at the Beijing and Guangzhou sites was caused by an increase in nucleation-mode particles at nighttime. The concentration of nucleation-mode particles at nighttime was significantly higher than during the daytime. We call this phenomenon a nocturnal nucleation event, and combined with analyses of factors involved, attribute this event to traffic emissions. To investigate the pollution sources at each location, we identified and quantified the pollution contributions from different sources by applying the k-means clustering analysis to observational datasets of environmental quantities. Clustering results showed that traffic emissions were the main contributor in Beijing and Guangzhou, with direct and significant impacts ranging from 37% to 45%, respectively.

Aerosol release, distribution, and prevention during aerosol therapy: a simulated model for infection control

Aerosol therapy is used to deliver medical therapeutics directly to the airways to treat respiratory conditions. A potential consequence of this form of treatment is the release of fugitive aerosols, both patient derived and medical, into the environment and the subsequent exposure of caregivers and bystanders to potential viral infections. This study examined the release of these fugitive aerosols during a standard aerosol therapy to a simulated adult patient. An aerosol holding chamber and mouthpiece were connected to a representative head model and breathing simulator. A combination of laser and Schlieren imaging was used to non-invasively visualize the release and dispersion of fugitive aerosol particles. Time-varying aerosol particle number concentrations and size distributions were measured with optical particle sizers at clinically relevant positions to the simulated patient. The influence of breathing pattern, normal and distressed, supplemental air flow, at 0.2 and 6 LPM, and the addition of a bacterial filter to the exhalation port of the mouthpiece were assessed. Images showed large quantities of fugitive aerosols emitted from the unfiltered mouthpiece. The images and particle counter data show that the addition of a bacterial filter limited the release of these fugitive aerosols, with the peak fugitive aerosol concentrations decreasing by 47.3–83.3%, depending on distance from the simulated patient. The addition of a bacterial filter to the mouthpiece significantly reduces the levels of fugitive aerosols emitted during a simulated aerosol therapy, p≤ .05, and would greatly aid in reducing healthcare worker and bystander exposure to potentially harmful fugitive aerosols.

Atmospheric aerosol, gases, and meteorological parameters measured during the LAPSE-RATE campaign by the Finnish Meteorological Institute and Kansas State University

Abstract. Small unmanned aerial systems (sUASs) are becoming very popular as affordable and reliable observation platforms. The Lower Atmospheric Process Studies at Elevation – a Remotely-piloted Aircraft Team Experiment (LAPSE-RATE), conducted in the San Luis Valley (SLV) of Colorado (USA) between 14 and 20 July 2018, gathered together numerous sUASs, remote-sensing equipment, and ground-based instrumentation. Flight teams from the Finnish Meteorological Institute (FMI) and the Kansas State University (KSU) co-operated during LAPSE-RATE to measure and investigate the properties of aerosol particles and gases at the surface and in the lower atmosphere. During LAPSE-RATE the deployed instrumentation operated reliably, resulting in an observational dataset described below in detail. Our observations included aerosol particle number concentrations and size distributions, concentrations of CO2 and water vapor, and meteorological parameters. All datasets have been uploaded to the Zenodo LAPSE-RATE community archive (https://zenodo.org/communities/lapse-rate/, last access: 21 August 2020). The dataset DOIs for FMI airborne measurements and surface measurements are available here: https://doi.org/10.5281/zenodo.3993996, Brus et al. (2020a), and those for KSU airborne measurements and surface measurements are available here: https://doi.org/10.5281/zenodo.3736772, Brus et al. (2020b).

Faucet aerator design influences aerosol size distribution and microbial contamination level

Faucet aerators have been linked to multiple opportunistic pathogen outbreaks in hospital, especially Pseudomonas aeruginosa, their complex structure promoting biofilm development. The importance of bacteria aerosolization by faucet aerators and their incidence on the risk of infection remain to be established. In this study, ten different types of aerators varying in complexity, flow rates and type of flow were evaluated in a controlled experimental setup to determine the production of aerosols and the level of contamination. The aerosol particle number density and size distribution were assessed using a particle spectrometer. The bacterial load was quantified with a 14-stage cascade impactor, where aerosol particles were captured and separated by size, then analysed by culture and flow cytometry. The water was seeded with Pseudomonas fluorescens as a bacterial indicator. Aerosol particle size and mean mass distribution varied depending on the aerator model. Devices without aeration or with laminar flow produced the lowest number and mass of aerosol particles when measured with spectrometry. Models with aeration displayed wide differences in their potential production of aerosol particles. A new aerator with a low flow, no air inlet in its structure, and a spray stream produced 12 to 395 times fewer aerosol particles containing bacteria. However, the impact of low flow on biofilm development and incorporation of pathogens should be further investigated. Repeated use of aerators resulted in fouling which increased the quantity of bacteria released through aerosol particles. An in-depth mechanical cleaning including complete dismantling of the aerator was required to recover initial performances. Aerators should be selected to minimize aerosol production, considering the ease of maintenance and the main water usage at each sink. Low flow aerators produced a lower number of contaminated aerosol particles when new but may be more susceptible to fouling and quickly lose their initial advantage.

A 3D study on the amplification of regional haze and particle growth by local emissions

The role of new particle formation (NPF) events and their contribution to haze formation through subsequent growth in polluted megacities is still controversial. To improve the understanding of the sources, meteorological conditions, and chemistry behind air pollution, we performed simultaneous measurements of aerosol composition and particle number size distributions at ground level and at 260 m in central Beijing, China, during a total of 4 months in 2015–2017. Our measurements show a pronounced decoupling of gas-to-particle conversion between the two heights, leading to different haze processes in terms of particle size distributions and chemical compositions. The development of haze was initiated by the growth of freshly formed particles at both heights, whereas the more severe haze at ground level was connected directly to local primary particles and gaseous precursors leading to higher particle growth rates. The particle growth creates a feedback loop, in which a further development of haze increases the atmospheric stability, which in turn strengthens the persisting apparent decoupling between the two heights and increases the severity of haze at ground level. Moreover, we complemented our field observations with model analyses, which suggest that the growth of NPF-originated particles accounted up to ∼60% of the accumulation mode particles in the Beijing–Tianjin–Hebei area during haze conditions. The results suggest that a reduction in anthropogenic gaseous precursors, suppressing particle growth, is a critical step for alleviating haze although the number concentration of freshly formed particles (3–40 nm) via NPF does not reduce after emission controls.

What can we learn about urban air quality with regard to the first outbreak of the COVID-19 pandemic? A case study from central Europe

Abstract. Motor vehicle road traffic in central Budapest was reduced by approximately 50 % of its ordinary level for several weeks as a consequence of various limitation measures introduced to mitigate the first outbreak of the COVID-19 pandemic in 2020. The situation was utilised to assess the real potentials of urban traffic on air quality. Concentrations of NO, NO2, CO, O3, SO2 and particulate matter (PM) mass, which are ordinarily monitored in cities for air quality considerations, aerosol particle number size distributions, which are not rarely measured continuously on longer runs for research purposes, and meteorological properties usually available were collected and jointly evaluated in different pandemic phases. The largest changes occurred over the severest limitations (partial lockdown in the Restriction phase from 28 March to 17 May 2020). Concentrations of NO, NO2, CO, total particle number (N6–1000) and particles with a diameter < 100 nm declined by 68 %, 46 %, 27 %, 24 % and 28 %, respectively, in 2020 with respect to the average reference year comprising 2017–2019. Their quantification was based on both relative difference and standardised anomaly. The change rates expressed as relative concentration difference due to relative reduction in traffic intensity for NO, NO2, N6–1000 and CO were 0.63, 0.57, 0.40 and 0.22 (%/%), respectively. Of the pollutants which reacted in a sensitive manner to the change in vehicle circulation, it is the NO2 that shows the most frequent exceedance of the health limits. Intentional tranquillising of the vehicle flow has considerable potential for improving the air quality. At the same time, the concentration levels of PM10 mass, which is the most critical pollutant in many European cities including Budapest, did not seem to be largely affected by vehicles. Concentrations of O3 concurrently showed an increasing tendency with lower traffic, which was explained by its complex reaction mechanism. Modelling calculations indicated that spatial gradients of NO and NO2 within the city became further enhanced by reduced vehicle flow.

Sources and formation of nucleation mode particles in remote tropical marine atmospheres over the South China Sea and the Northwest Pacific Ocean

A fast mobility particle sizer operating at a one-second time resolution was used to measure aerosol particle number size distribution (5.6–560 nm) in marine conditions over the South China Sea (SCS) from 29 March to 2 May 2017 and in the tropic zone of the Northwest Pacific Ocean (NWPO) from 10 to 29 October 2018. The clean background number concentration of nucleation mode atmospheric particles (<30 nm) was approximately 0.6 × 103 cm−3 in these areas. Two nighttime and five daytime strong new particle formation (NPF) events were observed to occur extending over a spatial scale from 2 to 140 km in the SCS, with a net increase of nucleation mode particles of 4.5 × 104 cm−3 ± 3.4 × 104 cm−3 during five of the seven events. Nighttime NPF events were unlikely associated with sulfuric acid vapor because of lack of photochemical reactions. Daytime NPF events share several common features with nighttime NPF events, e.g., dramatic spatiotemporal variations in the number concentration of the nucleation mode particles. Without aerosol precursor measurements we cannot address the vapors driving the formation process. However, our results show no banana-shaped growth of the particles. The growth into larger particle sizes seems to be restricted by the availability of condensable components in the gas phase. The nucleation mode was observed and sometimes even dominated the number concentration over other particle modes in the marine atmosphere over the tropic zone of the NWPO. In addition, more data obtained during the two campaigns and other campaigns were also applied to strengthen the analysis in terms of origins, formation and absent growth of nucleation mode particles in the marine atmospheres over the two tropic zones.

Predicting cloud condensation nuclei number concentration based on conventional measurements of aerosol properties in the North China Plain

Cloud condensation nuclei (CCN) play an important role in the formation and evolution of cloud droplets. However, the dataset of global CCN number concentration (NCCN) is still scarce due to the lack of direct CCN measurements, hindering an accurate evaluation of its climate effects. Alternative approaches to determine NCCN have thus been proposed to calculate NCCN based on measurements of other aerosol properties, such as particle number size distribution, bulk aerosol chemical composition and aerosol optical properties. To better understand the interaction between haze pollution and climate, we performed direct CCN measurements in the winter of 2018 at the Gucheng site, a typical polluted suburban site in North China Plain (NCP). The results show that the average CCN concentrations were 3.81 × 103 cm−3, 5.35 × 103 cm−3, 9.74 × 103 cm−3, 1.27 × 104 cm−3, 1.44 × 104 cm−3 at measured supersaturation levels of 0.114%, 0.148%, 0.273%, 0.492% and 0.864%, respectively. Based on these observational data, we have further investigated two methods of calculating NCCN from: (1) bulk aerosol chemical composition and particle number size distribution; (2) bulk aerosol chemical composition and aerosol optical properties. Our results showed that both methods could well reproduce the observed concentration (R2 > 0.88) and variability of NCCN with a 9% to 23% difference in the mean value. Further error analysis shows that the estimated NCCN tends to be underestimated by about 20% during the daytime while overestimated by <10% at night compared with the measured NCCN. These results provide quantitative instructions for the NCCN prediction based on conventional aerosol measurements in the NCP.

Variation of size-segregated particle number concentrations in wintertime Beijing

Abstract. The spatial and temporal variability of the number size distribution of aerosol particles is an indicator of the dynamic behavior of Beijing's atmospheric pollution cocktail. This variation reflects the strength of different primary and secondary sources, such as traffic and new particle formation, as well as the main processes affecting the particle population. In this paper, we report size-segregated particle number concentrations observed at a newly developed Beijing station during the winter of 2018. Our measurements covered particle number size distributions over the diameter range of 1.5 nm–1 µm (cluster mode, nucleation mode, Aitken mode and accumulation mode), thus being descriptive of a major fraction of the processes taking place in the atmosphere of Beijing. Here we focus on explaining the concentration variations in the observed particle modes, by relating them to the potential aerosol sources and sinks, and on understanding the connections between these modes. We considered haze days and new particle formation event days separately. Our results show that during the new particle formation (NPF) event days increases in cluster mode particle number concentration were observed, whereas during the haze days high concentrations of accumulation mode particles were present. There was a tight connection between the cluster mode and nucleation mode on both NPF event and haze days. In addition, we correlated the particle number concentrations in different modes with concentrations of trace gases and other parameters measured at our station. Our results show that the particle number concentration in all the modes correlated with NOx, which reflects the contribution of traffic to the whole submicron size range. We also estimated the contribution of ion-induced nucleation in Beijing, and we found this contribution to be negligible.

Investigation of Atmospheric Aerosol Size Distributions from Ground-Based Solar Spectrometer Measurements Synthesized with Satellite Data

Data collected by a ground-based solar spectrometer at Collegeville, MN, was used to generate Aerosol Optical Depths (AODs) throughout the 2017 calendar year. The AOD data was then visualized at 13 selected wavelengths throughout the year and analyzed in comparison to satellite imagery, upper air charts and backwards trajectories of air masses moving towards Central Minnesota in order to determine key dates of interest that correspond to times before (20170615), during (20170729), and at the conclusion of (20170914) forest fires that burned in British Columbia (BC) during the summer of 2017. The data from these specific days were analyzed further by inputting the maximum and minimum AODs for each day into a Parameter Based Particle Swarm Optimization (PBPSO) algorithm in order to generate bimodal lognormal particle size distributions. The bimodal distributions were chosen because they carry more information about the aerosol loads across the entire spectrum of particle radii. The resulting distributions show an increase in number density and decrease in median radius in the Aitken mode during the BC forest fires and a relatively constant (within uncertainty) number density of accumulation mode particles at daily maximum AODs. Comparing the resulting bimodal lognormal distribution for daily minimum AODs (where evaporation and other diurnal effects are at a minimum) shows an increased number density of Aitken mode particles by two orders of magnitude from pre- to post-forest fires. This measured increase in the number density of smaller radii particles due to forest fires illustrates the PBPSO’s capability of distinguishing variations in atmospheric aerosol particle number size distributions in the Aitken mode based on data collected by the Kipp-Zonen PGS-100 solar spectrometer. KEYWORDS: Atmospheric Aerosol; Particle Swarm Optimization; Aerosol Optical Depth; Solar Spectrometer; Size Distributions; Forest Fire; Satellite Imagery; Upper Air Charts; Backward Trajectory

A proxy for atmospheric daytime gaseous sulfuric acid concentration in urban Beijing

Abstract. Gaseous sulfuric acid (H2SO4) is known as one of the key precursors for atmospheric new particle formation (NPF) processes, but its measurement remains challenging. Therefore, a proxy method that is able to derive gaseous sulfuric acid concentrations from parameters that can be measured relatively easily and accurately is highly desirable for the atmospheric chemistry community. Although such methods are available for clean atmospheric environments, a proxy that works well in a polluted atmosphere, such as that found in Chinese megacities, is yet to be developed. In this study, the gaseous sulfuric acid concentration was measured in February–March 2018, in urban Beijing using a nitrate based – long time-of-flight chemical ionization mass spectrometer (LToF-CIMS). A number of atmospheric parameters were recorded concurrently including the ultraviolet radiation B (UVB) intensity, the concentrations of O3, NOx (sum of NO and NO2), SO2, and HONO, and aerosol particle number size distributions. A proxy for atmospheric daytime gaseous sulfuric acid concentration was derived via a statistical analysis method using the UVB intensity, [SO2], the condensation sink (CS), [O3], and [HONO] (or [NOx]) as the predictor variables, where square brackets denote the concentrations of the corresponding species. In this proxy method, we considered the formation of gaseous sulfuric acid from reactions of SO2 and OH radicals during the daytime, and the loss of gaseous sulfuric acid due to its condensation onto the preexisting particles. In addition, we explored the formation of OH radicals from the conventional gas-phase photochemistry using O3 as a proxy and from the photolysis of HONO using HONO (and subsequently NOx) as a proxy. Our results showed that the UVB intensity and [SO2] are dominant factors in the production of gaseous sulfuric acid, and that the simplest proxy could be constructed with the UVB intensity and [SO2] alone. When the OH radical production from both homogenously and heterogeneously formed precursors were considered, the relative errors were reduced by up to 20 %.

A Method of Aerosol Particle Number Size Distribution Inversed by PM2.5 Mass Concentration in PRD

The aerosol particle number size distribution(PNSD) is of great importance in calculating atmospheric radiation and optics. It can effectively supplement the inadequate observation of PNSD using the widely known aerosol mass concentration (PM2.5) measurement to invert PNSD. It would be valuable for research that needs PNSD data, like atmospheric visibility calculation. This paper created a PNSD inversed method based on the statistics and parameterization of the dry aerosol PM2.5 and PNSD dataset from the Guangzhou urban site's simultaneous measurements from November 2014 to January 2015. The inversed results appeared good in the accumulation mode, whereas more differences showed with higher PM2.5 loading. The applicability and stability of this method makes it preferable. It would provide advanced technical support for the visibility calculation and application in PRD.

Infrequent new particle formation over the remote boreal forest of Siberia

Aerosol particle number size distributions (PNSD) were investigated to verify, if extremely low-volatility organic vapors (ELVOC) from natural sources alone could induce new particle formation and growth events over the remote boreal forest region of Siberia, hundreds of kilometers away from significant anthropogenic sources. We re-evaluated observations determined at a height of 300 m of the remote observatory ZOTTO (Zotino Tall Tower Observatory, http://www.zottoproject.org). We found that new particle formation events occurred only on 11 days in a 3-year period, suggesting that homogeneous nucleation with a subsequent condensational growth could not be the major process, maintaining the particle number concentration in the planetary boundary layer of the remote boreal forest area of Siberia.