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Atmospheric particulates can be produced by emissions or form de novo. New particle formation usually occurs in relatively clean air. This is because preexisting particles in the atmosphere will scavenge the precursors of new particles and suppress their formation. However, observations in some heavily polluted megacities have revealed substantial rates of new particle formation despite the heavy loads of ambient aerosols. Yao et al. investigated new particle formation in Shanghai and describe the conditions that make this process possible. The findings will help inform policy decisions about how to reduce air pollution in these types of environments. Science , this issue p. 278 Atmospheric new particle formation in heavily polluted cities can occur in certain chemical environments. Atmospheric new particle formation (NPF) is an important global phenomenon that is nevertheless sensitive to ambient conditions. According to both observation and theoretical arguments, NPF usually requires a relatively high sulfuric acid (H 2 SO 4 ) concentration to promote the formation of new particles and a low preexisting aerosol loading to minimize the sink of new particles. We investigated NPF in Shanghai and were able to observe both precursor vapors (H 2 SO 4 ) and initial clusters at a molecular level in a megacity. High NPF rates were observed to coincide with several familiar markers suggestive of H 2 SO 4 –dimethylamine (DMA)–water (H 2 O) nucleation, including sulfuric acid dimers and H 2 SO 4 -DMA clusters. In a cluster kinetics simulation, the observed concentration of sulfuric acid was high enough to explain the particle growth to ~3 nanometers under the very high condensation sink, whereas the subsequent higher growth rate beyond this size is believed to result from the added contribution of condensing organic species. These findings will help in understanding urban NPF and its air quality and climate effects, as well as in formulating policies to mitigate secondary particle formation in China.

Formation of ultrafine particles (UFPs) in the urban atmosphere is expected to be less favored than in the rural atmosphere due to the high existing particle surface area acting as a sink for newly formed particles. Despite large condensation sink (CS) values, previous comparative studies between rural and urban sites reported higher frequency of new particle formation (NPF) events over urban sites in comparison to background sites as well as higher particle formation and growth rates attributed to the higher concentration of condensable species. The present study aims at a better understanding the environmental factors favoring, or disfavoring, atmospheric NPF over Lille, a large city in the north of France, and to analyze their impact on particle number concentration using a 4-year long-term dataset. The results highlight a strong seasonal variation of NPF occurrences with a maximum frequency observed during spring (27 events) and summer (53 events). It was found that high temperature (T>295 K), low relative humidity (RH <45 %), and high solar radiation are ideal to observe NPF events over Lille. Relatively high CS values (i.e., ∼2×10-2 s−1) are reported during event days suggesting that high CS does not inhibit the occurrence of NPF over the ATmospheric Observations in LiLLE (ATOLL) station. Moreover, the particle growth rate was positively correlated with temperatures most probably due to higher emission of precursors. Finally, the nucleation strength factor (NSF) was calculated to highlight the impact of those NPF events on particle number concentrations. NSF reached a maximum of four in summer, evidencing a huge contribution of NPF events to particle number concentration at this time of the year.

Atmospheric nucleation is the dominant source of aerosol particles in the global atmosphere and an important player in aerosol climatic effects. The key steps of this process occur in the sub—2-nanometer (nm) size range, in which direct size-segregated observations have not been possible until very recently. Here, we present detailed observations of atmospheric nanoparticles and clusters down to 1-nm mobility diameter. We identified three separate size regimes below 2-nm diameter that build up a physically, chemically, and dynamically consistent framework on atmospheric nucleation—more specifically, aerosol formation via neutral pathways. Our findings emphasize the important role of organic compounds in atmospheric aerosol formation, subsequent aerosol growth, radiative forcing and associated feedbacks between biogenic emissions, clouds, and climate.

Atmospheric new particle formation (NPF), which is observed in many environments globally, is an important source of boundary-layer aerosol particles and cloud condensation nuclei, which affect both the climate and human health. To better understand the mechanisms behind NPF, chamber experiments can be used to simulate this phenomenon under well-controlled conditions. Recent advancements in instrumentation have made it possible to directly detect the first steps of NPF of molecular clusters (~1–2 nm in diameter) and to calculate quantities such as the formation and growth rates of these clusters. Whereas previous studies reported particle formation rates as the flux of particles across a specified particle diameter or calculated them from measurements of larger particle sizes, this protocol outlines methods to directly quantify particle dynamics for cluster sizes. Here, we describe the instrumentation and analysis methods needed to quantify particle dynamics during NPF of sub-3-nm aerosol particles in chamber experiments. The methods described in this protocol can be used to make results from different chamber experiments comparable. The experimental setup, collection and post-processing of the data, and thus completion of this protocol, take from months up to years, depending on the chamber facility, experimental plan and level of expertise. Use of this protocol requires engineering capabilities and expertise in data analysis. This protocol describes the instrumentation and analysis methods needed to quantify particle dynamics during new particle formation of sub-3-nm aerosol particles in chamber experiments.

Aerosols and their interaction with clouds constitute the largest uncertainty in estimating the radiative forcing affecting the climate system. Secondary aerosol formation is responsible for a large fraction of the cloud condensation nuclei in the global atmosphere. Wetlands are important to the budgets of methane and carbon dioxide, but the potential role of wetlands in aerosol formation has not been investigated. Here we use direct atmospheric sampling at the Siikaneva wetland in Finland to investigate the emission of methane and volatile organic compounds, and subsequently formed atmospheric clusters and aerosols. We find that terpenes initiate stronger atmospheric new particle formation than is typically observed over boreal forests and that, in addition to large emissions of methane which cause a warming effect, wetlands also have a cooling effect through emissions of these terpenes. We suggest that new wetlands produced by melting permafrost need to be taken into consideration as sources of secondary aerosol particles when estimating the role of increasing wetland extent in future climate change.

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.

A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog 1 , 2 , but how it occurs in cities is often puzzling 3 . If the growth rates of urban particles are similar to those found in cleaner environments (1–10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below −15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid–base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms 4 , 5 . Measurements in the CLOUD chamber at CERN show that the rapid condensation of ammonia and nitric acid vapours could be important for the formation and survival of new particles in wintertime urban conditions, contributing to urban smog.

Field data from an iodine-rich, coastal environment point to the molecular steps involved in the formation of new aerosol particles from iodine vapours over coastal regions. Aerosol particle formation in coastal regions Sulfuric acid and organic vapours are thought to be involved in the formation of new aerosol particles in the atmosphere over continental regions, whereas iodine oxide vapours have been implicated in particle formation in coastal regions. But direct molecular-level observations of nucleation under atmospheric field conditions are lacking. Mikko Sipilä et al . report field data from Mace Head, Ireland, and supporting data from northern Greenland and Queen Maud Land, Antarctica, that allow for the identification of the molecular steps involved in new particle formation from iodine vapours in an iodine-rich, coastal atmospheric environment. Initial particle formation occurs primarily by uptake and sequential addition of iodic acid, followed by restructuring of molecules in clusters and subsequent evaporation of water. Homogeneous nucleation and subsequent cluster growth leads to the formation of new aerosol particles in the atmosphere 1 . The nucleation of sulfuric acid and organic vapours is thought to be responsible for the formation of new particles over continents 1 , 2 , whereas iodine oxide vapours have been implicated in particle formation over coastal regions 3 , 4 , 5 , 6 , 7 . The molecular clustering pathways that are involved in atmospheric particle formation have been elucidated in controlled laboratory studies of chemically simple systems 2 , 8 , 9 , 10 , but direct molecular-level observations of nucleation in atmospheric field conditions that involve sulfuric acid, organic or iodine oxide vapours have yet to be reported 11 . Here we present field data from Mace Head, Ireland, and supporting data from northern Greenland and Queen Maud Land, Antarctica, that enable us to identify the molecular steps involved in new particle formation in an iodine-rich, coastal atmospheric environment. We find that the formation and initial growth process is almost exclusively driven by iodine oxoacids and iodine oxide vapours, with average oxygen-to-iodine ratios of 2.4 found in the clusters. On the basis of this high ratio, together with the high concentrations of iodic acid (HIO 3 ) observed, we suggest that cluster formation primarily proceeds by sequential addition of HIO 3 , followed by intracluster restructuring to I 2 O 5 and recycling of water either in the atmosphere or on dehydration. Our study provides ambient atmospheric molecular-level observations of nucleation, supporting the previously suggested role of iodine-containing species in the formation of new aerosol particles 3 , 4 , 5 , 6 , 7 , 12 , 13 , 14 , 15 , 16 , 17 , 18 , and identifies the key nucleating compound.

Atmospheric new particle formation (NPF) occurs by the formation of nanometer-sized molecular clusters and their subsequent growth to larger particles. NPF involving sulfuric acid, bases and oxidized organic compounds is an important source of atmospheric aerosol particles. One of the mechanisms suggested to depict this process is nano-Köhler theory, which describes the activation of inorganic molecular clusters to growth by a soluble organic vapor. In this work, we studied the capability of nano-Köhler theory to describe the initial growth of atmospheric molecular clusters by simulating the dynamics of a cluster population in the presence of a sulfuric acid–base mixture and an organic compound. We observed nano-Köhler-type activation in our simulations when the saturation ratio of the organic vapor and the ratio between organic and inorganic vapor concentrations were in a suitable range. However, nano-Köhler theory was unable to predict the exact size at which the activation occurred in the simulations. In some conditions, apparent cluster growth rate (GR) started to increase close to the activation size determined from the simulations. Nevertheless, because the behavior of GR is also affected by other dynamic processes, GR alone cannot be used to deduce the cluster growth mechanism.

The link between biogenic volatile organic compounds in the atmosphere and their conversion to aerosol particles is unclear, but a direct reaction pathway is now described by which volatile organic compounds lead to low-volatility vapours that can then condense onto aerosol surfaces, producing secondary organic aerosol. From forest emission to aerosol Forests emit large quantities of volatile organic compounds to the atmosphere. The condensable oxidation products of volatile organic compounds emitted by forests can form secondary organic aerosols or SOAs that can affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. But our understanding of the link between biogenic volatile organic compounds and their conversion to aerosol particles remains limited. This study reveals that a direct reaction pathway can lead from volatile organic compounds to low-volatility vapours that can then condense onto aerosol surfaces producing secondary organic aerosol and can significantly enhance the formation and growth of aerosol particles over forested regions. Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol 1 , 2 , which is known to affect the Earth’s radiation balance by scattering solar radiation and by acting as cloud condensation nuclei 3 . The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours 4 , 5 , 6 , but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies 2 . We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere–aerosol–climate feedback mechanisms 6 , 7 , 8 , and the air quality and climate effects of biogenic emissions generally.