Condensation Sink Research Articles

On the potential of the Cluster Ion Counter (CIC) to observe local new particle formation, condensation sink and growth rate of newly formed particles

Abstract. The Cluster Ion Counter (CIC) is a simple three-channel instrument designed to observe ions in the electrical mobility equivalent diameter range from 1.0 to 5 nm. With the three channels, we can observe concentrations of both ion clusters (sub-2 nm ions) and intermediate ions. Furthermore, as derived here, we can estimate condensation sink (CS), intensity of local new particle formation, growth rate of newly formed particles from 2 to 3 nm and formation rate of 2 nm ions. We compared CIC measurements with those of a multichannel ion spectrometer, the Neutral cluster and Air Ion Spectrometer (NAIS), and found that the concentrations agreed well between the two instruments, with correlation coefficients of 0.89 and 0.86 for sub-2 nm and 2.0–2.3 nm ions, respectively. According to the observations made in Hyytiälä, Finland, and Beijing, China, the ion source rate was estimated to be about two to four ion pairs cm−3 s−1. The new CIC is a simple and cheap instrument that can be used in different environments to obtain information about small ion dynamics, local intermediate ion formation and CS in a robust way when combined with the theoretical framework presented here.

Chemical characterization and sources of background aerosols in the eastern Mediterranean

Measurements of the composition of the gas and particulate phases were conducted from May 9 to June 4 of 2016 at the Finokalia (Greece) remote coastal site in the eastern Mediterranean, continuing the effort to track long term changes of the atmospheric chemical composition in the area. Finokalia is influenced by air masses arriving in the site from regional sources in Europe, Africa, and other locations. In this study, a series of instruments and analysis techniques were used for the first time at the Finokalia site to characterize the composition of the organic aerosol (OA). The PM1 was composed of ammonium sulfate/bisulfate (60%), followed by organics (35%) and black carbon (BC) (4%). The OA was highly oxidized with an average oxygen-to-carbon (O:C) ratio of 0.81. Source apportionment of high-resolution organic aerosol mass spectra via positive matrix factorization (PMF) identified four factors: less oxidized oxygenated organic aerosol (LO-OOA), more oxidized oxygenated organic aerosol (MO-OOA), marine-related oxygenated organic aerosol (marine-OOA) and hydrocarbon-like organic aerosol (HOA). The LO-OOA (O:C = 0.92) was the dominant factor for most of the campaign (51% of the PM1 OA), while the MO-OOA (O:C = 1.1) was responsible for 11% of the OA. The marine-OOA factor was also highly oxidized (O:C = 1.03), contributing on average 24% to the total OA and was found to be well correlated with sulfate (R2 = 0.83). The anthropogenic HOA factor (O:C = 0.36) was related to activities in the island of Crete. Its mass spectrum was quite similar (R2 = 0.86–0.95) to those of other HOA factors in the literature and its average concentration was 0.2 μg m−3 (14% of OA). High molecular weight compounds were found, suggesting the presence of oligomers in agreement with the presence of a highly oxidized quenching agent. Aromatic VOCs, like benzene, toluene, and xylenes were on average 0.17, 0.66 and 0.36 ppb, respectively with toluene concentrations indicating the presence of a local source despite the remote nature of the site. New particle formation (NPF) was observed during 26% of the days. The air masses during NPF events passed over the island of Crete and the Balkans and were characterized by a low condensation sink (5.9 ± 2.2 10−3 s−1). Nucleation mode particle concentrations during NPF days had an additional evening peak between 17:00 and 22:00, which was accompanied by an HOA peak implying the influence of a source of sub-25 nm particles in the extended area. These findings show that even a relatively remote site like Finokalia is occasionally affected by sources located tens of kilometers away, something that should be taken into account in the interpretation of past and future measurements in this location.

New particle formation induced by anthropogenic–biogenic interactions on the southeastern Tibetan Plateau

Abstract. New particle formation (NPF) plays a crucial role in the atmospheric aerosol population and has significant implications on climate dynamics, particularly in climate-sensitive zones such as the Tibetan Plateau (TP). However, our understanding of NPF on the TP is still limited due to a lack of comprehensive measurements and verified model simulations. To fill this knowledge gap, we conducted an integrated study combining comprehensive field measurements and chemical transport modeling to investigate NPF events on the southeastern TP during the pre-monsoon season. NPF was observed to occur frequently on clear-sky days on the southeastern TP, contributing significantly to the cloud condensation nuclei (CCN) budget in this region. The observational evidence suggests that highly oxygenated organic molecules (HOMs) from monoterpene oxidation participate in the nucleation on the southeastern TP. After updating the monoterpene oxidation chemistry and nucleation schemes in the meteorology–chemistry model, the model well reproduces observed NPF and reveals an extensive occurrence of NPF across the southeastern TP. The dominant nucleation mechanism is the synergistic nucleation of sulfuric acid, ammonia, and HOMs, driven by the transport of anthropogenic precursors from South Asia and the presence of abundant biogenic gases. By investigating the vertical distribution of NPF, we find a significant influence of vertical transport on the southeastern TP. More specifically, strong nucleation near the surface leads to an intense formation of small particles, which are subsequently transported upward. These particles experience enhanced growth to larger sizes in the upper planetary boundary layer (PBL) due to favorable conditions such as lower temperatures and a reduced condensation sink. As the PBL evolves, the particles in larger sizes are brought back to the ground, resulting in a pronounced increase in near-surface particle concentrations. This study highlights the important roles of anthropogenic–biogenic interactions and meteorological dynamics in NPF on the southeastern TP.

Elucidating the mechanisms of atmospheric new particle formation in the highly polluted Po Valley, Italy

Abstract. New particle formation (NPF) is a major source of aerosol particles and cloud condensation nuclei in the troposphere, playing an important role in both air quality and climate. Frequent NPF events have been observed in heavily polluted urban environments, contributing to the aerosol number concentration by a significant amount. The Po Valley region in northern Italy has been characterized as a hotspot for high aerosol loadings and frequent NPF events in southern Europe. However, the mechanisms of NPF and growth in this region are not completely understood. In this study, we conducted a continuous 2-month measurement campaign with state-of-the-art instruments to elucidate the NPF and growth mechanisms in northern Italy. Our results demonstrate that frequent NPF events (66 % of all days during the measurement campaign) are primarily driven by abundant sulfuric acid (8.5×106 cm−3) and basic molecules in this area. In contrast, oxygenated organic molecules from the atmospheric oxidation of volatile organic compounds (VOCs) appear to play a minor role in the initial cluster formation but contribute significantly to the consecutive growth process. Regarding alkaline molecules, amines are insufficient to stabilize all sulfuric acid clusters in the Po Valley. Ion cluster measurements and kinetic models suggest that ammonia (10 ppb) must therefore also play a role in the nucleation process. Generally, the high formation rates of sub-2 nm particles (87 cm−3 s−1) and nucleation-mode growth rates (5.1 nm h−1) as well as the relatively low condensational sink (8.9×10-3 s−1) will result in a high survival probability for newly formed particles, making NPF crucial for the springtime aerosol number budget. Our results also indicate that reducing key pollutants, such as SO2, amine and NH3, could help to substantially decrease the particle number concentrations in the Po Valley region.

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.

Exploring the influence of physical and chemical factors on new particle formation in a polluted megacity

In polluted environments, the condensation sink, along with relative humidity and aerosol liquid water content, plays a key role in suppressing new particle formation events, which appear largely unaffected by aerosol chemical composition.

Impact of desert dust on new particle formation events and the cloud condensation nuclei budget in dust-influenced areas

Abstract. Detailed knowledge on the formation of new aerosol particles in the atmosphere from precursor gases, and their subsequent growth, commonly known as new particle formation (NPF) events, is one of the largest challenges in atmospheric aerosol science. High pre-existing particle loadings are expected to suppress the formation of new atmospheric aerosol particles due to high coagulation and condensation (CS) sinks. However, NPF events are regularly observed in conditions with high concentrations of pre-existing particles and even during intense desert dust intrusions that imply discrepancies between the observations and theory. In this study, we present a multi-site analysis of the occurrence of NPF events under the presence of desert dust particles in dust-influenced areas. Characterization of NPF events at five different locations highly influenced by desert dust outbreaks was done under dusty and non-dusty conditions using continuous measurements of aerosol size distribution in both fine and coarse size fractions. Contrary to common thought, our results show that the occurrence of NPF events is highly frequent during desert dust outbreaks, showing that NPF event frequencies during dusty conditions are similar to those observed during non-dusty conditions. Furthermore, our results show that NPF events also occur during intense desert dust outbreaks at all the studied sites, even at remote sites where the amounts of precursor vapours are expected to be low. Our results show that the condensation sink associated with coarse particles (CSC) represents up to the 60 % of the total CS during dusty conditions, which highlights the importance of considering coarse-fraction particles for NPF studies in desert-dust-influenced areas. However, we did not find a clear pattern of the effect of desert dust outbreaks on the strength of NPF events, with differences from site to site. The particle growth rate (GR) did not present a clear dependence on the CS during dusty and non-dusty conditions. This result, together with the fact that desert dust has different effects on the growth and formation rates at each site, suggests different formation and growth mechanisms at each site between dusty and non-dusty conditions, probably due to differences in precursor vapours' origins and concentrations as well as changes in the oxidative capacity of pre-existing particles and their effectiveness acting as CS. Further investigation based on multiplatform measurement campaigns and chamber experiments with state-of-the-art gaseous and particulate physical and chemical properties measurements is needed to better understand the role of catalyst components present in desert dust particles in NPF. Finally, our results reveal a significant impact of NPF events on the cloud condensation nuclei (CCN) budget during desert dust outbreaks at the studied sites. Therefore, since desert dust contributes to a major fraction of the global aerosol mass load, and since there is a foreseeable increase in the frequency, duration and intensity of desert dust episodes due to climate change, it is imperative to improve our understanding of the effect of desert dust outbreaks on NPF and the CCN budget for better climate change prediction.

Examining the vertical heterogeneity of aerosols over the Southern Great Plains

Abstract. Atmospheric aerosols affect the global energy budget by scattering and absorbing sunlight (direct effects) and by changing the microphysical structure, lifetime, and coverage of clouds (indirect effects). Both aerosol direct and indirect effects are affected by the vertical distribution of aerosols in the atmosphere, which is further influenced by a range of processes, such as aerosol dynamics, long-range transport, and entrainment. However, many observations of these processes are based on ground measurements, limiting our ability to understand the vertical distribution of aerosols and simulate their impact on clouds and climate. In this work, we examined the vertical heterogeneity of aerosols over the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) using data collected from the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) campaign. The vertical profiles of meteorological and aerosol physiochemical properties up to 2500 m above are examined based on the 38 flights conducted during the HI-SCALE campaign. The aerosol properties over the SGP show strong vertical heterogeneity and seasonal variabilities. The aerosol concentrations at the surface are the highest due to strong emissions at ground level. In general, the mode diameter of aerosols during summer (∼ 100 nm) is larger than that during spring (∼ 30 nm), a result of enhanced condensational growth due to enriched volatile organic compounds in summer. The concentration of aerosols below 30 nm in the boundary layer (BL) (e.g., below 1000 m) during spring is higher than that during summer, a result of the stronger new particle formation (NPF) events due to the reduced condensation sink in spring. In the BL, the size of the aerosols gradually increases with altitude due to condensational growth and cloud processing. However, the chemical composition of the aerosols remained similar, with organics and sulfates representing 59.8 ± 2.2 % and 22.7 ± 2.1 %, respectively, of the total mass in the BL. Through the vertical profiles of aerosol properties, we observed NPF events in the upper BL during 7 out of 38 research flights, where the newly formed particles continue to grow as they are mixed down to the surface. There is also an indication that deep convection brings aerosols from the free troposphere (FT) to the surface, where they grow to contribute to the cloud condensation nuclei (CCN). Overall, the vertical heterogeneity of aerosols over the SGP is influenced by aerosol dynamics (new particle formation, growth, and cloud processing) and transport processes (mixing in the BL, long-range transport, entrainment, and convective downward transport). Case studies showing the influence of these factors are discussed.

Exposure to urban nanoparticles at low PM_1 concentrations as a source of oxidative stress and inflammation

Exposures to fine particulate matter (PM_1) have been associated with health impacts, but the understanding of the PM_1 concentration-response (PM_1-CR) relationships, especially at low PM_1, remains incomplete. Here, we present novel data using a methodology to mimic lung exposure to ambient air (2<PM_1< 60 upmug m^{-3}), with minimized sampling artifacts for nanoparticles. A reference model (Air Liquid Interface cultures of human bronchial epithelial cells, BEAS-2B) was used for aerosol exposure. Non-linearities observed in PM_1-CR curves are interpreted as a result of the interplay between the aerosol total oxidative potential (OP_t) and its distribution across particle size (d_p). A d_p-dependent condensation sink (CS) is assessed together with the distribution with d_p of reactive species . Urban ambient aerosol high in OP_t, as indicated by the DTT assay, with (possibly copper-containing) nanoparticles, shows higher pro-inflammatory and oxidative responses, this occurring at lower PM_1 concentrations (< 5 upmug m^{-3}). Among the implications of this work, there are recommendations for global efforts to go toward the refinement of actual air quality standards with metrics considering the distribution of OP_t with d_p also at relatively low PM_1.

New particle formation in the tropical free troposphere during CAMP2Ex: statistics and impact of emission sources, convective activity, and synoptic conditions

Abstract. Nucleation in the free troposphere (FT) and subsequent growth of new particles represent a globally important source of cloud condensation nuclei (CCN). Whereas new particle formation (NPF) has been shown to occur frequently in the upper troposphere over tropical oceans, there have been few studies of NPF at lower altitudes. In addition, the impact of urban emissions and biomass burning on the NPF in tropical marine FT remains poorly understood. In this study, we examine NPF in the lower and mid-troposphere (3–8.5 km) over the tropical ocean and coastal region using airborne measurements during the recent Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex). NPF was mostly observed above 5.5 km and coincided with elevated relative humidity (RH) and reduced condensation sink (CS), suggesting that NPF occurs in convective cloud outflow. The frequency of NPF increases with altitude, reaching ∼ 50 % above 8 km. An abrupt decrease in NPF frequency coincides with early monsoon transition and is attributed to increased CS resulting from reduced convective activity and more frequent transport of aged urban plumes. Surprisingly, a large fraction of NPF events in background air were observed in the early morning, and the NPF is likely made possible by very low CS despite low actinic flux. Convectively detrained biomass-burning plumes and fresh urban emissions enhance NPF as a result of elevated precursor concentrations and scavenging of pre-existing particles. In contrast, NPF is suppressed in aged urban plumes where the reactive precursors are mostly consumed, while CS remains relatively high. This study shows a strong impact of urban and biomass-burning emissions on the NPF in tropical marine FT. The results also illustrate the competing influences of different variables and interactions among anthropogenic emissions, convective clouds, and meteorology, which lead to NPF under a variety of conditions in tropical marine environments.

A dynamic parameterization of sulfuric acid–dimethylamine nucleation and its application in three-dimensional modeling

Abstract. Sulfuric acid (SA) is a governing gaseous precursor for atmospheric new particle formation (NPF), a major source of global ultrafine particles, in environments studied around the world. In polluted urban atmospheres with high condensation sinks (CSs), the formation of stable SA–amine clusters, such as SA–dimethylamine (DMA) clusters, usually initializes intense NPF events. Coagulation scavenging and cluster evaporation are dominant sink processes of SA–amine clusters in urban atmospheres, yet these loss processes are not quantitatively included in the present parameterizations of SA–amine nucleation. We herein report a parameterization of SA–DMA nucleation, based on cluster dynamic simulations and quantum chemistry calculations, with certain simplifications to greatly reduce the computational costs. Compared with previous SA–DMA nucleation parameterizations, this new parameterization was able to reproduce the dependences of particle formation rates on temperature and CSs. We then incorporated it in a three-dimensional (3-D) chemical transport model to simulate the evolution of the particle number size distributions. Simulation results showed good consistency with the observations in the occurrence of NPF events and particle number size distributions in wintertime Beijing and represented a significant improvement compared to that using a parameterization without coagulation scavenging. Quantitative analysis shows that SA–DMA nucleation contributes significantly to nucleation rates and aerosol population during the 3-D simulations in Beijing (&gt;99 % and &gt;60 %, respectively). These results broaden the understanding of NPF in urban atmospheres and stress the necessity of including the effects of coagulation scavenging and cluster stability in simulating SA–DMA nucleation in 3-D simulations. Representing these processes is thus likely to improve model performance in particle source apportionment and quantification of aerosol effects on air quality, human health, and climate.

Characterization of dust-related new particle formation events based on long-term measurement in the North China Plain

Abstract. Mineral dust is a major natural atmospheric aerosol that impacts the Earth's radiation balance. The significant scavenging process of fine particles by the strong wind during the dust episodes provided a relatively clean environment that was favourable for new particle formation (NPF) occurrence. In this study, the NPF occurred following the dust episodes (dust-related NPF), and other cases under clean and polluted conditions were classified based on the long-term particle number size distribution (PNSD) in urban Beijing in spring from 2017 to 2021. It was found that the observed formation (Jobs) and growth rate (GR) of dust-related NPF events were approximately 50 % and 30 % lower than the values of other NPF days, respectively. A typical severe dust storm that originated from Mongolia and swept over northern China on 15–16 March 2021 was analysed, to illustrate how the dust storm influences the NPF event. The maximum hourly mean PM10 mass concentration reached 8000 µg m−3 during this dust storm. The occurrence of an NPF event after a dust storm was facilitated due to the low condensation sink (∼ 0.005 s−1) caused by the strong dilution process of pre-existing particles. However, a downward trend of particle hygroscopicity was found during dust storm and NPF event as compared with the polluted episode, resulting in an increasing trend of the critical diameter at different supersaturations (ss), where aerosols are activated as cloud condensation nuclei (CCN), although the NPF event occurred when dust faded. The critical diameter was elevated by approximately 6 %–10 % (ss = 0.2 % and 0.7 %) during the dust storm, resulting in a lower CCN activation ratio, especially at low supersaturation. Modifications of the nucleation and growth process, as well as the particle-size distribution and hygroscopicity of the dust particles, provide valuable information that reveals the underlying climate and air quality effects of Asian mineral dust.

Measurement report: The 4-year variability and influence of the Winter Olympics and other special events on air quality in urban Beijing during wintertime

Abstract. Comprehensive measurements are vital to obtain big enough datasets for better understanding the complex atmosphere and further improving the air quality. To investigate the 4-year variation of air quality and the influences of special events (Beijing Winter Olympics, COVID lockdown and Chinese New Year) on it during the wintertime in polluted urban air, we conducted comprehensive observations in Beijing, China, during 1 January–20 February, in the years from 2019 to 2022. The mass concentration of PM2.5 and its composition (organics, nitrate, sulfate, ammonium, chloride and black carbon) and the number size distributions of particles (down to ∼1 nm) and ions, gaseous pollutants (CO, NOx, SO2, O3) and condensable vapors (sulfuric acid and oxygenated organic molecules), as well as meteorological parameters, were simultaneously measured. The days before 22 January without any special events in each year were selected to investigate the 4-year variability of air quality. We found that the concentrations of CO, NOx, total oxygenated organic molecules (OOMs), total PM2.5, organics, chloride and black carbon and the number concentration of sub-3 nm particles (N1.3−3) showed similar variations, decreasing from 2019 to 2021 and then increasing in 2022. For SO2, however, its concentration decreased year by year due to the significant emission reduction, further leading to the decrease of gaseous sulfuric acid and particulate sulfate from 2019 to 2022. O3 concentration showed an opposite 4-year variation compared with NOx. Meanwhile, both the oxygen and nitrogen contents of oxygenated organic molecules increased year by year, implying that not only the oxidation state of those compounds increased, but also NOx was involved more efficiently in their formation processes. With higher sulfuric acid concentrations and new particle formation (NPF) frequencies in 2021 than in 2022, and with the lowest concentrations of background aerosols and the lowest ambient temperatures in 2021, N1.3−3 was still the lowest in 2021. Unlike N1.3−3, the ion concentrations in both 0.8–2 and 2–4 nm size ranges were higher in 2021 than in the other years. Then, the days after 4 February were chosen to explore the influence of special events. The non-event days within this date range in 2019 and 2021 were chosen as the reference period. Due to the favorable meteorological conditions together with reductions in anthropogenic emissions, there were basically no haze events during the Olympics. Therefore, CO, NOx, SO2, total OOMs, accumulation-mode particles (N100−1000), and total PM2.5 and its composition were much lower, while ion concentrations were much higher compared with the reference period. Although there was also emission reduction during COVID, especially for NOx, the enhancement of secondary inorganic aerosol formation, together with unfavorable meteorological conditions, caused severe haze events during this period. Hence, CO, total OOMs and all PM2.5 compositions during COVID increased dramatically compared with the reference period. Influenced by SO2, condensation sink and sunlight, sulfuric acid concentration was found to be comparable between the Olympics and the reference period but was lower during COVID and Chinese New Year. Additionally, N1.3−3 was almost at the same level during different periods, indicating that the special events only had little impact on the NPF processes. These results provide useful information to the development of more targeted pollution control plans.

Measurement Report: Wintertime new particle formation in the rural area of the North China Plain – influencing factors and possible formation mechanism

Abstract. The high concentration of fine particles and gaseous pollutants makes polluted areas, such as the urban setting of North China Plain (NCP) of China, a different environment for new particle formation (NPF) compared to many clean regions. Such conditions also hold for other polluted environments in this region (for instance, the rural area of NCP), yet the underlying mechanisms for NPF remain less understood, owing to the limited observations of particles in the sub−3 nm range. Comprehensive measurements, particularly covering the particle number size distribution down to 1.3 nm, were conducted at a rural background site of Gucheng (GC) in the North China Plain (NCP) from 12 November to 24 December 2018. In total, five NPF events during the 39 effective days of measurements for the campaign were identified, with the mean particle nucleation rate (J1.3) and growth rate (GR1.3–2.4) being 22.0 cm−3 s−1 and 3.9 nm h−1, respectively. During these 5 d, NPF concurrently occurred at an urban site in Beijing. Sharing similar sources and transport paths of air masses arriving at our site to that of urban Beijing, we hypothesize that NPF events during these days in this region might be a regional phenomenon. The simultaneous occurrence of NPF in both places implies that H2SO4-amine nucleation, concluded for urban Beijing there, could probably be the dominating mechanism for NPF at our rural site. The higher concentration of sulfuric acid during many non-event days compared to that of event days indicates that the content of sulfuric acid may not necessarily lead to NPF events under current atmosphere. Only when the condensation sink or coagulation sink was significantly lowered, atmospheric NPF occurred, implying that condensation sinks (CSs) and coagulation sinks (CoagSs) are the dominating factors controlling the occurrence of NPF for the present rural environment of the NCP, which is quite similar to the feature seen in urban Beijing.

Revealing the sources and sinks of negative cluster ions in an urban environment through quantitative analysis

Abstract. Atmospheric cluster ions are important constituents in the atmosphere, and their concentrations and compositions govern their role in atmospheric chemistry. However, there is currently limited quantitative research on atmospheric ion compositions, sources, and sinks, especially in the urban atmosphere where pollution levels and human populations are intense. In this study, we measured the compositions of negative cluster ions and neutral molecules using an atmospheric pressure interface high-resolution time-of-flight mass spectrometer (APi-TOF) and a chemical ionization mass spectrometer in urban Beijing. Quantitative analysis of cluster ions was performed by their comparison with condensation sink (CS), reagent ions, and neutral molecules. We demonstrate the feasibility of quantifying cluster ions with different compositions using in situ-measured ion mobility distributions from a neutral cluster and air ion spectrometer (NAIS). The median concentration of negative cluster ions was 85 (61–112 for 25 %–75 %) cm−3 during the measurement period, which was negatively correlated with CS. The negative cluster ions mainly consisted of inorganic nitrogen-containing ions, inorganic sulfur-containing ions, and organic ions in the form of adducts with NO3- or HSO4-. The CHON-related organic ions accounted for over 70 % of the total organic ions. Although the molecules clustered with NO3- and HSO4- had similar compositions, we found that HSO4- clustered more efficiently with CHO and CHONnonNPs species (CHON excluding nitrated phenols), while NO3- clustered more efficiently with nitrated phenols (CHONNPs). Additionally, most organic ions were positively correlated with neutral molecules, resulting in similar diurnal cycles of organic ions and neutral molecules. However, an exception was found for CHONNPs, the concentration of which is also significantly influenced by the reagent ions NO3-. The charge fractions are generally higher for molecules with higher molecular weight and a higher oxidation state, and the opposite diurnal variations in charging fractions between H2SO4 and organic species indicate a charging competition between them. Finally, we choose HSO4- and C3H3O4- as representatives to calculate the contribution of different formation and loss pathways. We found their losses are condensational loss onto aerosol particles (73 %–75 %), ion–molecule reaction losses (19 %), and ion–ion recombination losses (6 %–8 %).

New Particle Formation Occurrence in the Urban Atmosphere of Beijing During 2013–2020

AbstractNew particle formation (NPF) has strong influences on air quality and global climate. However, it was still ambiguous under which atmospheric condition NPF can occur, due to lack of long‐term observation data analysis. The long‐term measurement of NPF was conducted from 2013 to 2020 at PeKing University Urban Atmosphere Environment MonitoRing Station in Beijing, during which strong pollution control measures were conducted. However, the NPF frequency (NPF‐freq) remained stable within 40.4%–48.9% in an average of 42.5%. The occurrence of NPF events was characterized by lower levels of NOx, condensational sink, relative humidity, and higher levels of wind speed and north wind proportion. SO2 may act as one limiting factor only in summer. An H2SO4‐base nucleation indicator, I275K was calculated. It was found that I275K &gt; 243 can separate the NPF and non‐NPF days quite well during the 8 years, with bias at 17%. Accordingly, it was also revealed that the simultaneous control of SO2 and PM2.5 (serving as condensation sink) in Beijing happened to cause the stable level of I275K, as well as the NPF frequency during 2013–2020. The results implicated that along with the reduction of primary emission, the secondary NPF process may become more important in aerosol evolution by its stable frequency, and the precise control of gaseous precursors is required for particle pollution mitigation in the future.

Genesis of New Particle Formation Events in a Semi-Urban Location in Eastern Himalayan Foothills

New particle formation (NPF) events identified using scanning mobility particle sizer (SMPS) measurements, their subsequent growth and other characteristics over Dibrugarh, a semi-urban location in the eastern Himalayan foothills (EHF), during November–December 2016 are presented. The mean total number concentration of ultrafine aerosols was found to be high during morning and evening rush hours. The NPF occurrence frequency was found to be 14%. The temporal evolution of the hourly average aerosol number size distribution revealed that the nucleation burst occurred at a lower size spectrum, supporting the existence of NPF burst events. It continued to grow through coagulation loss and condensation sink with an average growth rate of 17.16 ± 12.29 nm/hr. The satellite-based observations showed a high concentration of the NPF precursors NO2, SO2, and HCHO during the NPF days. The backward air mass trajectories confirmed that the sources of emissions were confined within an area of radius ~100 km surrounding the observation site. These locally generated precursors and their associated photochemistry could be a probable reason for NPF occurrence at the study site.

High frequency of new particle formation events driven by summer monsoon in the central Tibetan Plateau, China

Abstract. New particle formation (NPF) is an important source of cloud condensation nuclei (CCN), which affects Earth's radiative balance and global climate. The mechanism and CCN contribution of NPF at the high-altitude mountains, especially in the Tibetan Plateau (TP), was unclear due to lack of measurements. In this study, intensive measurements were conducted at the Nam Co station (4730 m a.s.l.) in the central TP during both the pre-monsoon and summer monsoon seasons. The frequencies of NPF events exhibited evident seasonal differences with 15 % in the pre-monsoon season and 80 % in the monsoon season. The comprehensive analysis of the measured condensation sink (CS), gaseous precursors and meteorological conditions, supplemented by the model simulations of SO2 and volatile organic compound (VOC), points to the organic involved nucleation as the dominant mechanism. Condensation sink and gaseous sulfuric acid could have no significant effect on the occurrence of NPF events. The frequent NPF events in the summer monsoon season may result from the higher frequency of southerly and southwesterly air masses, which brought the organic precursors to participate in the NPF process. It had increased the aerosol number concentrations and CCN at supersaturation of 1.2 % by more than 2 and 0.6 times compared with those in the pre-monsoon season, respectively. Considering that the smaller particles formed by NPF may further grow and reach CCN size during the following days due to the low-level coagulation sink, the amount of potential CCN in the monsoon season could be much larger than our local measurement results. Our results emphasized the importance of considering the seasonal effect of NPF when simulating the amounts of aerosols and CCN in the high-altitude atmosphere. Long-term investigations with a full set of instrumentation are required for deeper scientific understanding of NPF process and its role in the global budget in the TP.

Sulfur Dioxide Transported From the Residual Layer Drives Atmospheric Nucleation During Haze Periods in Beijing

AbstractNew particle formation (NPF) is a global phenomenon that significantly influences climate. NPF also contributes to haze, with pronounced negative impacts on human health. Theory and observations both show that nucleation is favored during clean days and inhibited during haze episodes due to a high pre‐existing condensation sink (CS). Here we show that the surprising occurrence of NPF during haze days in Beijing is associated with a high concentration of sulfuric acid dimers. With both field observations and model simulations, we demonstrate that downward mixing of sulfur dioxide (SO2) from the residual layer aloft enhances ground level SO2, which in turn elevates sulfuric acid dimer after rapid SO2 oxidation in the polluted air. Our results address a key gap between the source of SO2 and its atmospheric oxidation products during haze conditions in a megacity, Beijing, providing a missing link in a complete chain describing NPF in the polluted atmosphere.

Significant effects of transport on nanoparticles during new particle formation events in the atmosphere of Beijing

The mechanisms of new particle formation (NPF) events that occurred under high aerosol loadings (“polluted” NPF) in the atmosphere have been unclear, which has inhibited the precision of particle pollution control. To deepen the understanding of how the “polluted” NPF events occur, a one-month comprehensive measurement was conducted in the atmosphere of Beijing during the summer of 2016. The “clean” NPF events (frequency = 22%) (condensation sink, CS < 0.015 s−1) were found to be caused by local nucleation and growth. The “polluted” NPF events (frequency = 28%) (CS > 0.015 s−1) were influenced by both local nucleation-growth and regional transport, and the contributions from the two factors to 6–25 nm particle number concentration were 60% and 40%, respectively. This study emphasized the importance of the transport for nanoparticles in relatively polluted atmospheres, and for that the regional joint particle pollution control would be an essential policy.