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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.

Frequency and intensity of warm and moist air-mass intrusions into the Arctic have increased over the past decades and have been related to sea ice melt. During our year-long expedition in the remote central Arctic Ocean, a record-breaking increase in temperature, moisture and downwelling-longwave radiation was observed in mid-April 2020, during an air-mass intrusion carrying air pollutants from northern Eurasia. The two-day intrusion, caused drastic changes in the aerosol size distribution, chemical composition and particle hygroscopicity. Here we show how the intrusion transformed the Arctic from a remote low-particle environment to an area comparable to a central-European urban setting. Additionally, the intrusion resulted in an explosive increase in cloud condensation nuclei, which can have direct effects on Arctic clouds’ radiation, their precipitation patterns, and their lifetime. Thus, unless prompt actions to significantly reduce emissions in the source regions are taken, such intrusion events are expected to continue to affect the Arctic climate. Warm and moist air-mass intrusions into the Arctic are more frequent than the past decades. Here, the authors show that warm air mass intrusions from northern Eurasia inject record amounts of aerosols into the central Arctic Ocean strongly impacting atmospheric chemistry and cloud properties.

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.

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.

An air pollutant proxy is a mathematical model that estimates an unobserved air pollutant using other measured variables. The proxy is advantageous to fill missing data in a research campaign or to substitute a real measurement for minimising the cost as well as the operators involved (i.e., virtual sensor). In this paper, we present a generic concept of pollutant proxy development based on an optimised data-driven approach. We propose a mutual information concept to determine the interdependence of different variables and thus select the most correlated inputs. The most relevant variables are selected to be the best proxy inputs, where several metrics and data loss are also involved for guidance. The input selection method determines the used data for training pollutant proxies based on a probabilistic machine learning method. In particular, we use a Bayesian neural network that naturally prevents overfitting and provides confidence intervals around its output prediction. In this way, the prediction uncertainty could be assessed and evaluated. In order to demonstrate the effectiveness of our approach, we test it on an extensive air pollution database to estimate ozone concentration.

Atmospheric new particle formation (NPF) has been observed to take place in practice all around the world. In continental locations, typically about 10–40% of the days are so-called NPF event days characterized by a clear particle formation and growth that continue for several hours, occurring mostly during daytime. The other days are either non-event days, or days for which it is difficult to decide whether NPF had occurred or not. Using measurement data from several locations (Hyytiälä, Järvselja, and near-city background and city center of Budapest), we were able to show that NPF tends to occur also on the days traditionally characterized as non-event days. One explanation is the instrument sensitivity towards low number concentrations in the sub-10 nm range, which usually limits our capability to detect such NPF events. We found that during such days, particle formation rates at 6 nm were about 2–20% of those observed during the traditional NPF event days. Growth rates of the newly formed particles were very similar between the traditional NPF event and non-event days. This previously overlooked phenomenon, termed as quiet NPF, contributes significantly to the production of secondary particles in the atmosphere.

We characterized new particle formation (NPF) events in the urban background of Amman during August 2016–July 2017. The monthly mean of submicron particle number concentration was 1.2 × 104–3.7 × 104 cm−3 (exhibited seasonal, weekly, and diurnal variation). Nucleation mode (10–15 nm) concentration was 0.7 × 103–1.1 × 103 cm−3 during daytime with a sharp peak (1.1 × 103–1.8 × 103 cm−3) around noon. We identified 110 NPF events (≈34% of all days) of which 55 showed a decreasing mode diameter after growth. The NPF event occurrence was higher in summer than in winter, and events were accompanied with air mass back trajectories crossing over the Eastern Mediterranean. The mean nucleation rate (J10) was 1.9 ± 1.1 cm−3 s−1 (monthly mean 1.6–2.7 cm−3 s−1) and the mean growth rate was 6.8 ± 3.1 nm/h (4.1–8.8 nm/h). The formation rate did not have a seasonal pattern, but the growth rate had a seasonal variation (maximum around August and minimum in winter). The mean condensable vapor source rate was 4.1 ± 2.2 × 105 molecules/cm3 s (2.6–6.9 × 105 molecules/cm3 s) with a seasonal pattern (maximum around August). The mean condensation sink was 8.9 ± 3.3 × 10−3 s−1 (6.4–14.8 × 10−3 s−1) with a seasonal pattern (minimum around June and maximum in winter).

Nucleation and subsequent growth of new aerosol particles in the atmosphere is a major source of cloud condensation nuclei and persistent large uncertainty in climate models. Newly formed particles need to grow rapidly to avoid scavenging by pre-existing aerosols and become relevant for the climate and air quality. In the continental atmosphere, condensation of oxygenated organic molecules is often the dominant mechanism for rapid growth. However, the huge variety of different organics present in the continental boundary layer makes it challenging to predict nanoparticle growth rates from gas-phase measurements. Moreover, recent studies have shown that growth rates of nanoparticles derived from particle size distribution measurements show surprisingly little dependency on potentially condensable vapors observed in the gas phase. Here, we show that the observed nanoparticle growth rates in the sub-10 nm size range can be predicted in the boreal forest only for springtime conditions, even with state-of-the-art mass spectrometers and particle sizing instruments. We find that, especially under warmer conditions, observed growth is slower than predicted from gas-phase condensation. We show that only a combination of simple particle-phase reaction schemes, phase separation due to non-ideal solution behavior, or particle-phase diffusion limitations can explain the observed lower growth rates. Our analysis provides first insights as to why atmospheric nanoparticle growth rates above 10 nm h −1 are rarely observed. Ultimately, a reduction of experimental uncertainties and improved sub-10 nm particle hygroscopicity and chemical composition measurements are needed to further investigate the occurrence of such a growth rate-limiting process.

The Arctic environment is transforming rapidly due to climate change. Aerosols’ abundance and physicochemical characteristics play a crucial, yet uncertain, role in these changes due to their influence on the surface energy budget through direct interaction with solar radiation and indirectly via cloud formation. Importantly, Arctic aerosol properties are also changing in response to climate change. Despite their importance, year-round measurements of their characteristics are sparse in the Arctic and often confined to lower latitudes at Arctic land-based stations and/or short high-latitude summertime campaigns. Here, we present unique aerosol microphysics and chemical composition datasets collected during the year-long Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition, in the central Arctic. These datasets, which include aerosol particle number concentrations, size distributions, cloud condensation nuclei concentrations, fluorescent aerosol concentrations and properties, and aerosol bulk chemical composition (black carbon, sulfate, nitrate, ammonium, chloride, and organics) will serve to improve our understanding of high-Arctic aerosol processes, with relevance towards improved modelling of the future Arctic (and global) climate.

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.