Showing papers by "Pauli Paasonen published in 2021"

Is reducing new particle formation a plausible solution to mitigate particulate air pollution in Beijing and other Chinese megacities

Abstract: Atmospheric gas-to-particle conversion is a crucial or even dominant contributor to haze formation in Chinese megacities in terms of aerosol number, surface area and mass. Based on our comprehensive observations in Beijing during 15 January 2018-31 March 2019, we are able to show that 80-90% of the aerosol mass (PM2.5) was formed via atmospheric reactions during the haze days and over 65% of the number concentration of haze particles resulted from new particle formation (NPF). Furthermore, the haze formation was faster when the subsequent growth of newly formed particles was enhanced. Our findings suggest that in practice almost all present-day haze episodes originate from NPF, mainly since the direct emission of primary particles in Beijing has considerably decreased during recent years. We also show that reducing the subsequent growth rate of freshly formed particles by a factor of 3-5 would delay the buildup of haze episodes by 1-3 days. Actually, this delay would decrease the length of each haze episode, so that the number of annual haze days could be approximately halved. Such improvement in air quality can be achieved with targeted reduction of gas-phase precursors for NPF, mainly dimethyl amine and ammonia, and further reductions of SO2 emissions. Furthermore, reduction of anthropogenic organic and inorganic precursor emissions would slow down the growth rate of newly-formed particles and consequently reduce the haze formation.

Sulfuric acid–amine nucleation in urban Beijing

Abstract: . New particle formation (NPF) is one of the major sources of atmospheric ultrafine particles. Due to the high aerosol and trace gas concentrations, the mechanism and governing factors for NPF in the polluted atmospheric boundary layer may be quite different from those in clean environments, which is however less understood. Herein, based on long-term atmospheric measurements from January 2018 to March 2019 in Beijing, the nucleation mechanism and the influences of H2SO4 concentration, amine concentrations, and aerosol concentration on NPF are quantified. The collision of H2SO4 –amine clusters is found to be the dominating mechanism to initialize NPF in urban Beijing. The coagulation scavenging due to the high aerosol concentration is a governing factor as it limits the concentration of H2SO4 –amine clusters and new particle formation rates. The formation of H2SO4 –amine clusters in Beijing is sometimes limited by low amine concentrations. Summarizing the synergistic effects of H2SO4 concentration, amine concentrations, and aerosol concentration, we elucidate the governing factors for H2SO4 –amine nucleation for various conditions.

The Synergistic Role of Sulfuric Acid, Bases, and Oxidized Organics Governing New-Particle Formation in Beijing

Abstract: Intense and frequent new particle formation (NPF) events have been observed in polluted urban environments, yet the dominant mechanisms are still under debate. To understand the key species and governing processes of NPF in polluted urban environments, we conducted comprehensive measurements in downtown Beijing during January–March, 2018. We performed detailed analyses on sulfuric acid cluster composition and budget, as well as the chemical and physical properties of oxidized organic molecules (OOMs). Our results demonstrate that the fast clustering of sulfuric acid (H2SO4) and base molecules triggered the NPF events, and OOMs further helped grow the newly formed particles toward climateand health-relevant sizes. This synergistic role of H2SO4, base species, and OOMs in NPF is likely representative of polluted urban environments where abundant H2SO4 and base species usually co-exist, and OOMs are with moderately low volatility when produced under high NOx concentrations. Plain Language Summary Atmospheric new particle formation (NPF) is a dominant source of atmospheric ultrafine particles worldwide. Those particles profoundly influence climate and human health. NPF includes two consecutive processes, that is, the formation of new particles (∼2 nm in diameter) and their subsequent growth to larger sizes. Extensive studies conducted in the laboratory and in forested areas have shown that many gaseous species can participate in NPF, such as sulfuric acid, ammonia, amines, and oxidize organic molecules. However, the actual roles of these vapors may vary significantly from location to location and are largely unclear in urban environments. Here, based on measurements of sulfuric acid, sulfuric acid clusters, and oxidize organic molecules, we demonstrate that sulfuric acid and base molecules were responsible for the initial formation of new particles during a wintertime field campaign in Beijing. The majority of oxidized organic molecules had a minor YAN ET AL. © 2021. The Authors. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. The Synergistic Role of Sulfuric Acid, Bases, and Oxidized Organics Governing New-Particle Formation in Beijing Chao Yan , Rujing Yin, Yiqun Lu , Lubna Dada , Dongsen Yang, Yueyun Fu, Jenni Kontkanen , Chenjuan Deng, Olga Garmash , Jiaxin Ruan, Rima Baalbaki , Meredith Schervish, Runlong Cai, Matthew Bloss, Tommy Chan , Tianzeng Chen , Qi Chen, Xuemeng Chen, Yan Chen, Biwu Chu, Kaspar Dällenbach, Benjamin Foreback, Xucheng He, Liine Heikkinen , Tuija Jokinen, Heikki Junninen, Juha Kangasluoma , Tom Kokkonen , Mona Kurppa, Katrianne Lehtipalo , Haiyan Li, Hui Li , Xiaoxiao Li, Yiliang Liu, Qingxin Ma , Pauli Paasonen , Pekka Rantala , Rosaria E. Pileci , Anton Rusanen, Nina Sarnela , Pauli Simonen , Shixian Wang, Weigang Wang , Yonghong Wang , Mo Xue, Gan Yang, Lei Yao, Ying Zhou, Joni Kujansuu, Tuukka Petäjä, Wei Nie , Yan Ma, Maofa Ge , Hong He, Neil M. Donahue , Douglas R. Worsnop, Veli-Matti Kerminen, Lin Wang , Yongchun Liu, Jun Zheng , Markku Kulmala , Jingkun Jiang , and Federico Bianchi Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Aerosol and Haze Laboratory, Beijing University of Chemical Technology, Beijing, China, Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland, School of Environment, State Key Joint Laboratory of Environment Simulation and Pollution Control, Tsinghua University, Beijing, China, Department of Environmental Science & Engineering, Fudan University, Shanghai, China, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Nanjing University of Information Science & Technology, Nanjing, China, Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, USA, Research Center for EcoEnvironmental Sciences, Chinese Academy of Science, Beijing, China, School of Environmental Sciences, Peking University, Beijing, China, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China, Laboratory of Environmental Physics, Institute of Physics, University of Tartu, Tartu, Estonia, Finnish Meteorological Institute, Helsinki, Finland, Laboratory of Atmospheric Chemistry, Paul Scherrer Institute (PSI), Villigen, Switzerland, Aerosol Physics Laboratory, Physics Unit, Tampere University, Tampere, Finland, School of Atmospheric Sciences, Joint International Research Laboratory of Atmospheric and Earth System Sciences, Nanjing University, Nanjing, China, Aerodyne Research Inc., Billerica, MA, USA Key Points: • Process-level understanding of new particle formation (NPF) in wintertime Beijing was obtained based on measurement state-of-theart instruments • The analysis of sulfuric acid cluster composition and budget showed that sulfuric acid-base clustering initiated NPF • Condensable organic vapors were characterized and demonstrated to have a crucial influence on the growth of newly formed particles Supporting Information: Supporting Information may be found in the online version of this article.

Significance of the organic aerosol driven climate feedback in the boreal area

Abstract: Aerosol particles cool the climate by scattering solar radiation and by acting as cloud condensation nuclei. Higher temperatures resulting from increased greenhouse gas levels have been suggested to lead to increased biogenic secondary organic aerosol and cloud condensation nuclei concentrations creating a negative climate feedback mechanism. Here, we present direct observations on this feedback mechanism utilizing collocated long term aerosol chemical composition measurements and remote sensing observations on aerosol and cloud properties. Summer time organic aerosol loadings showed a clear increase with temperature, with simultaneous increase in cloud condensation nuclei concentration in a boreal forest environment. Remote sensing observations revealed a change in cloud properties with an increase in cloud reflectivity in concert with increasing organic aerosol loadings in the area. The results provide direct observational evidence on the significance of this negative climate feedback mechanism. Vegetation emits organic vapors which can form aerosols in the atmosphere and influence cloud properties. Here, the authors show observational evidence that warmer temperatures lead to increased emissions of these aerosols in boreal forests which cause surface cooling, demonstrating a negative climate feedback mechanism.

Long-term measurement of sub-3 nm particles and their precursor gases in the boreal forest

Abstract: . The knowledge of the dynamics of sub-3nm particles in the atmosphere is crucial for our understanding of first steps of atmospheric new particle formation. Therefore, accurate and stable long-term measurements of the smallest atmospheric particles are needed. In this study, we analyzed over five years of particle concentrations in size classes 1.1–1.3 nm, 1.3–1.7 nm and 1.7–2.5 nm obtained with the Particle Size Magnifier (PSM) and three years of precursor vapor concentrations measured with the Chemical Ionization Atmospheric Pressure Interface Time-of-Flight mass spectrometer (CI-APi-ToF) at the SMEAR II station in Hyytiala, Finland. The results show that the 1.1–1.3 nm particle concentrations have a daytime maximum during all seasons, which is due to increased photochemical activity. There are significant seasonal differences in median concentrations of 1.3–1.7 nm and 1.7–2.5 nm particles, underlining the different frequency of new particle formation between seasons. In particular, concentrations of 1.3–1.7 nm and 1.7–2.5 nm particles are notably higher in spring than during other seasons. Aerosol precursor vapors have notable diurnal and seasonal differences as well. Sulfuric acid and highly oxygenated organic molecule (HOM) monomer concentrations have clear daytime maxima, while HOM dimers have their maxima during the night. HOM concentrations for both monomers and dimers are the highest during summer and the lowest during winter. Higher median concentrations during summer result from increased biogenic activity in the surrounding forest. Sulfuric acid concentrations are the highest during spring and summer, with autumn and winter concentrations being two to three times lower. A correlation analysis between the sub-3nm concentrations and aerosol precursor vapor concentrations indicates that HOMs, particularly their dimers, and sulfuric acid play a significant role in new particle formation in the boreal forest. Our analysis also suggests that there might be seasonal differences in new particle formation pathways that need to be investigated further.

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

Abstract: 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.

Toward Building a Physical Proxy for Gas-Phase Sulfuric Acid Concentration Based on Its Budget Analysis in Polluted Yangtze River Delta, East China

Abstract: Gaseous sulfuric acid (H2SO4) is a crucial precursor for secondary aerosol formation, particularly for new particle formation (NPF) that plays an essential role in the global number budget of aerosol particles and cloud condensation nuclei. Due to technology challenges, global-wide and long-term measurements of gaseous H2SO4 are currently very challenging. Empirical proxies for H2SO4 have been derived mainly based on short-term intensive campaigns. In this work, we performed comprehensive measurements of H2SO4 and related parameters in the polluted Yangtze River Delta in East China during four seasons and developed a physical proxy based on the budget analysis of gaseous H2SO4. Besides the photo-oxidation of SO2, we found that primary emissions can contribute considerably, particularly at night. Dry deposition has the potential to be a non-negligible sink, in addition to condensation onto particle surfaces. Compared with the empirical proxies, the newly developed physical proxy demonstrates extraordinary stability in all the seasons and has the potential to be widely used to improve the understanding of global NPF fundamentally.

Measurement report: The influence of traffic and new particle formation on the size distribution of 1-800 nm particles in Helsinki - a street canyon and an urban background station comparison

Abstract: . Most of the anthropogenic air pollution sources are located in urban environments. The contribution of these sources to the population of atmospheric particles in the urban environment is poorly known. In this study, we investigated the aerosol particle number concentrations in a diameter range from 1 to 800 nm at a street canyon site and at a background station within 1 km from each other in Helsinki, Finland. We use these number size distribution data together with complementary trace gas data and develop a method to estimate the relative contributions of traffic and atmospheric new particle formation (NPF) to the concentrations of sub-3 nm particles. During the daytime, the particle concentrations were higher at the street canyon site than at the background station in all analyzed modes: sub-3 nm particles, nucleation mode (3–25 nm), Aitken mode (25–100 nm), and accumulation mode (100–800 nm). The population of sub-3 nm and nucleation mode particles was linked to local sources such as traffic, while the accumulation mode particles were more related to non-local sources. Aitken mode particles were dominated by local sources at the street canyon site, while at the background station they were mainly influenced by non-local sources. The results of this study support earlier research showing direct emissions of the sub-3 nm particles from traffic. However, by using our new method, we show that, during NPF events, traffic contribution to the total sub-3 nm particle concentration can be small and during daytime (6:00–20:00) in spring it does not dominate the sub-3 nm particle population at either of the researched sites. In the future, the contribution of traffic to particle number concentrations in different urban environments can be estimated with a similar approach, but determining the relationships between the gas and particle concentrations from observations needs to be conducted with longer data sets from different urban environments.

Trends of Planetary Boundary Layer Height Over Urban Cities of China From 1980–2018

Abstract: Boundary layer height (BLH) is an important parameter in climatology and air pollution research, especially in urban city. We calculated the BLH with a bulk Richardson number (Ri) method over urban cities of China during 1980-2018 using European Centre for Medium-Range Weather Forecasts (ECMWF) ERA-interim data after carefully validation with sounding data obtained from two meteorology stations in eastern China during 2010-2018. The values of BLH between these two types of data have correlation coefficients in the range of 0.65-0.87, which indicates that it is reasonable to analyze long-term trends of the BLH from ERA data sets. Using ERA-interim calculated BLH, we found that there is an increasing trend in the daytime BLH in most cities of eastern China, particularly during the spring season. A correlation analysis between the BLH and temperature, wind speed, relative humidity and visibility revealed that the variability in meteorological parameters, as well as in aerosol concentrations over highly polluted eastern China, play important roles in the development of the BLH.

Measurement Report: A Multi-Year Study on the Impacts of Chinese New Year Celebrations on Air Quality in Beijing, China

Abstract: . We investigated the influence of the Chinese New Year (CNY) celebrations on local air quality in Beijing from 2013 through 2019, bringing together comprehensive observations at the newly-constructed Aerosol and Haze Laboratory at Beijing University of Chemical Technology – West Campus (BUCT-AHL) and data from Chinese government air quality measurement stations. In this study, these datasets are used together to provide a detailed analysis of air quality during the CNY over multiple years. Before CNY in 2018, the city of Beijing prohibited the use of fireworks and firecrackers in an effort to reduce air pollution. In 2018 air pollutant concentrations still showed a significant peak during the CNY night, even though not as strong as in previous years, but in 2019, the pollution levels were notably lower. During the studied 7-year study period, it appears that there has been a long-term decrease in CNY related emissions since 2016. Based on our analysis, the pollutants with the most notable spike during CNY were sulfur dioxide and particulate matter, including black carbon. Sulfuric acid concentration followed the sulfur dioxide concentration and showed elevated overnight concentration in CNY 2018, but not notably in 2019. Additionally, spectrometer data and analysis of aerosol particle number size distribution shows direct emissions of particles with diameters around 20 nm during CNY in 2018 and 2019. Meteorological conditions were comparable between the latest two years, indicating that air quality associated with the CNY may be improving, perhaps a positive effect of the restrictions. The longer observations in the future will provide confirmation for these trends.

Measurement Report: New particle formation characteristics at an urban and a mountain station in Northern China

Abstract: . Atmospheric new particle formation (NPF) events have attracted increasing attention for their contribution to the global aerosol number budget, and therefore their effects on climate, air quality, and human health. NPF events are regarded as a regional phenomenon, occurring over a large area. However, the spatial variation of NPF intensity has not been investigated in detail by incorporating both urban and regional measurements. Urban environments have more heterogeneous and freshly emitted NPF precursors as compared to environments with less anthropogenic activity. Here, we provide a comparison of NPF event characteristics – NPF event frequency, particle formation rate, and growth rate – by comparing an urban Beijing site and a background mountain site separated by ~80 km from June 14 to July 14, 2019 as well as give insights into the connection between both locations. During the measurement period, 12 and 13 NPF events were observed at the urban and background mountain sites, respectively, with 9 NPF events observed on the same day at both sites. Although the median condensation sink during the first two hours of the common NPF events was around 0.01 s−1 at both sites, there were notable differences in particle formation rates between the two locations (median of 5.42 cm−3 s−1 at the urban site and 1.13 cm−3 s−1 at the mountain site during the first two hours of common NPF events). Yet, the particle growth rates in the 7–15 nm range for common NPF events were comparable (median of 7.6 nm.h−1 at the urban site and 6.5 nm.h−1 at the mountain site as median values). To understand whether the observed events were connected, we compared air mass trajectories as well as meteorological conditions at both stations. Favorable conditions for the occurrence of regional NPF events were largely affected by air mass transport. Overall, our results demonstrate a clear inhomogeneity of regional NPF within a distance of ~100 km, which should be considered in regional-scale aerosol models when estimating the budget of aerosol load and cloud condensation nuclei.

The effect of urban morphological characteristics on the spatial variation of PM2.5 air quality in downtown Nanjing

Abstract: The effects of the urban morphological characteristics on the spatial variation of near-surface PM2.5 air quality were examined. Unlike previous studies, we performed the analyses in real urban environments using continuous observations covering the whole scale of urban densities typically found in cities. We included data from 31 measurement stations divided into 8 different wind sectors with individually defined morphological characteristics leading to highly varying urban characteristics. The urban morphological characteristics explained up to 73% of the variance in normalized PM2.5 concentrations in street canyons, indicating that the spatial variation of the near-surface PM2.5 air quality was mostly defined by the characteristics studied. The fraction of urban trees nearby the stations was found to be the most important urban morphological characteristic in explaining the PM2.5 air quality, followed by the height-normalized roughness length as the second important parameter. An increase in the fraction of trees within 50 m of the stations from 25 percentile to 75 percentile (i.e. by the interquartile range, IQR) increased the normalized PM2.5 concentration by up to 24% in the street canyons. In open areas, an increase in the trees by the IQR actually decreased the normalized PM2.5 by 6% during the pre-COVID period. An increase in the height-normalized roughness length by the IQR increased the normalized PM2.5 by 9% in the street canyons. The results obtained in this study can help urban planners to identify the key urban characteristics affecting the near-surface PM2.5 air quality and also help researchers to evaluate how representative the existing measurement stations are compared to other parts of the cities.

Clear, transparent, and timely communication for fair authorship decisions : a practical guide

Abstract: . Authorship conflicts are a common occurrence in academic publishing, and they can have serious implications for the careers and well-being of the involved researchers as well as the collective success of research organizations. In addition to not inviting relevant contributors to co-author a paper, the order of authors as well as honorary, gift, and ghost authors are all widely recognized problems related to authorship. Unfair authorship practices disproportionately affect those lower in the power hierarchies – early career researchers, women, researchers from the Global South, and other minoritized groups. Here we propose an approach to preparing author lists based on clear, transparent, and timely communication. This approach aims to minimize the potential for late-stage authorship conflicts during manuscript preparation by facilitating timely and transparent decisions on potential co-authors and their responsibilities. Furthermore, our approach can help avoid imbalances between contributions and credits in published papers by recording planned and executed responsibilities. We present authorship guidelines which also include a novel authorship form along with the documentation of the formulation process for a multidisciplinary and interdisciplinary center with more than 250 researchers. Other research groups, departments, and centers can use or build on this template to design their own authorship guidelines as a practical way to promote fair authorship practices.