Explore the vast range of titles available.

The formation of new atmospheric aerosol particles and their subsequent growth have been observed frequently at various locations all over the world. The atmospheric nucleation rate (or formation rate) and growth rate (GR) are key parameters to characterize the phenomenon. Recent progress in measurement techniques enables us to measure atmospheric nucleation at the size (mobility diameter) of 1.5 (±0.4) nm. The detection limit has decreased from 3 to 1 nm within the past 10 years. In this protocol, we describe the procedures for identifying new-particle-formation (NPF) events, and for determining the nucleation, formation and growth rates during such events under atmospheric conditions. We describe the present instrumentation, best practices and other tools used to investigate atmospheric nucleation and NPF at a certain mobility diameter (1.5, 2.0 or 3.0 nm). The key instruments comprise devices capable of measuring the number concentration of the formed nanoparticles and their size, such as a suite of modern condensation particle counters (CPCs) and air ion spectrometers, and devices for characterizing the pre-existing particle number concentration distribution, such as a differential mobility particle sizer (DMPS). We also discuss the reliability of the methods used and requirements for proper measurements and data analysis. The time scale for realizing this procedure is 1 year.

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.

Volatile organic compounds play a significant role in atmospheric chemistry, influencing air quality and climate change. Accurate prediction of their physical properties is essential for understanding their behavior. This paper introduces VaPOrS (Vapor Pressure in Organics via SMILES) as a comprehensive tool designed to process SMILES notation of organic compounds, identify key functional groups, and apply group-contribution methods for property estimation. The core innovation of VaPOrS lies in its self-contained functional group recognition algorithm, which eliminates dependence on external cheminformatics libraries. The current approach enables fully auditable, easily modifiable, and computationally efficient detection of 30 functional groups required by the SIMPOL method. Compared to existing tools, VaPOrS avoids heavy SMILES-to-graph conversions and can obviate interface overhead, providing orders-of-magnitude speedups for large-scale atmospheric modeling scenarios. While this first implementation focuses on the SIMPOL method for estimating saturation vapor pressure and enthalpy of vaporization, the framework is readily extendable to other group-contribution schemes and thermodynamic properties (e.g., partition coefficients, volatility basis set models, solubility, Henry's law constants). The tool has been validated against manually counted functional groups and experimental saturation vapor pressure data for a diverse set of compounds. Results demonstrate excellent agreement with both the original SIMPOL model and experimental observations, while comparisons with existing tools highlight the robustness and accuracy of the new parsing functions. VaPOrS thus provides a generalizable and computationally efficient platform for property prediction of large molecular datasets, facilitating integration into chemical transport and climate models and streamlining the analysis of thousands of organic compounds in atmospheric science applications.

Atmospheric chemistry: forest isoprene clears the air Terrestrial vegetation releases vast amounts of volatile organic compounds (VOCs) into the atmosphere, mainly isoprene and derivatives such as monoterpenes and sesquiterpenes, some familiar as the aroma of pine trees. It has been suggested that these compounds are involved in the formation of organic aerosols, which act as 'seeds' for cloud formation and hence as cooling agents via an effect on radiative forcing. Experiments in a plant chamber simulating forest conditions show that isoprene can significantly inhibit new particle formation owing to its high hydroxyl radical reactivity. This surprising result may explain the observed seasonality in the frequency of aerosol nucleation events, as terpene emissions peak in summer, when there are fewer nucleation events than in autumn and spring. This work suggests that an increase in the isoprene content of VOCs in response to climate or land use change might reduce the potential for the formation of new aerosol particles, introducing a previously unrecognized element of climate warming. Volatile organic compounds, such as isoprene and monoterpenes, are emitted by terrestrial vegetation and have been suggested to be involved in organic aerosol formation, which in turn affects radiative forcing and climate. Simulation experiments conducted in a plant chamber now reveal that isoprene can significantly inhibit new particle formation; this may explain the observed seasonality in the frequency of aerosol nucleation events. It has been suggested that volatile organic compounds (VOCs) are involved in organic aerosol formation, which in turn affects radiative forcing and climate 1 . The most abundant VOCs emitted by terrestrial vegetation are isoprene and its derivatives, such as monoterpenes and sesquiterpenes 2 . New particle formation in boreal regions is related to monoterpene emissions 3 and causes an estimated negative radiative forcing 4 of about -0.2 to -0.9 W m -2 . The annual variation in aerosol growth rates during particle nucleation events correlates with the seasonality of monoterpene emissions of the local vegetation, with a maximum during summer 5 . The frequency of nucleation events peaks, however, in spring and autumn 5 . Here we present evidence from simulation experiments conducted in a plant chamber that isoprene can significantly inhibit new particle formation. The process leading to the observed decrease in particle number concentration is linked to the high reactivity of isoprene with the hydroxyl radical (OH). The suppression is stronger with higher concentrations of isoprene, but with little dependence on the specific VOC mixture emitted by trees. A parameterization of the observed suppression factor as a function of isoprene concentration suggests that the number of new particles produced depends on the OH concentration and VOCs involved in the production of new particles undergo three to four steps of oxidation by OH. Our measurements simulate conditions that are typical for forested regions and may explain the observed seasonality in the frequency of aerosol nucleation events, with a lower number of nucleation events during summer compared to autumn and spring 5 . Biogenic emissions of isoprene are controlled by temperature and light 2 , and if the relative isoprene abundance of biogenic VOC emissions increases in response to climate change or land use change, the new particle formation potential may decrease, thus damping the aerosol negative radiative forcing effect.

Atmospheric aerosol formation is known to occur almost all over the world, and the importance of these particles to climate and air quality has been recognized. Although almost all of the processes driving aerosol formation take place below a particle diameter of 3 nanometers, observations cover only larger particles. We introduce an instrumental setup to measure atmospheric concentrations of both neutral and charged nanometer-sized clusters. By applying the instruments in the field, we come to three important conclusions: (i) A pool of numerous neutral clusters in the sub-3 nanometer size range is continuously present; (ii) the processes initiating atmospheric aerosol formation start from particle sizes of ~1.5 nanometers; and (iii) neutral nucleation dominates over the ion-induced mechanism, at least in boreal forest conditions.

Oxidation flow reactors (OFRs) or environmental chambers can be used to estimate secondary aerosol formation potential of different emission sources. Emissions from anthropogenic sources, such as vehicles, often vary on short timescales. For example, to identify the vehicle driving conditions that lead to high potential secondary aerosol emissions, rapid oxidation of exhaust is needed. However, the residence times in environmental chambers and in most oxidation flow reactors are too long to study these transient effects ( ∼  100 s in flow reactors and several hours in environmental chambers). Here, we present a new oxidation flow reactor, TSAR (TUT Secondary Aerosol Reactor), which has a short residence time ( ∼  40 s) and near-laminar flow conditions. These improvements are achieved by reducing the reactor radius and volume. This allows studying, for example, the effect of vehicle driving conditions on the secondary aerosol formation potential of the exhaust. We show that the flow pattern in TSAR is nearly laminar and particle losses are negligible. The secondary organic aerosol (SOA) produced in TSAR has a similar mass spectrum to the SOA produced in the state-of-the-art reactor, PAM (potential aerosol mass). Both reactors produce the same amount of mass, but TSAR has a higher time resolution. We also show that TSAR is capable of measuring the secondary aerosol formation potential of a vehicle during a transient driving cycle and that the fast response of TSAR reveals how different driving conditions affect the amount of formed secondary aerosol. Thus, TSAR can be used to study rapidly changing emission sources, especially the vehicular emissions during transient driving.

Atmospheric emissions, including particle number and size distribution, from a 726 MWth coal-fired power plant were studied experimentally from a power plant stack and flue-gas plume dispersing in the atmosphere. Experiments were conducted under two different flue-gas cleaning conditions. The results were utilized in a plume dispersion and dilution model taking into account particle formation precursor (H2SO4 resulted from the oxidation of emitted SO2) and assessment related to nucleation rates. The experiments showed that the primary emissions of particles and SO2 were effectively reduced by flue-gas desulfurization and fabric filters, especially the emissions of particles smaller than 200 nm in diameter. Primary pollutant concentrations reached background levels in 200–300 s. However, the atmospheric measurements indicated that new particles larger than 2.5 nm are formed in the flue-gas plume, even in the very early phases of atmospheric ageing. The effective number emission of nucleated particles were several orders of magnitude higher than the primary particle emission. Modelling studies indicate that regardless of continuing dilution of the flue gas, nucleation precursor (H2SO4 from SO2 oxidation) concentrations remain relatively constant. In addition, results indicate that flue-gas nucleation is more efficient than predicted by atmospheric aerosol modelling. In particular, the observation of the new particle formation with rather low flue-gas SO2 concentrations changes the current understanding of the air quality effects of coal combustion. The results can be used to evaluate optimal ways to achieve better air quality, particularly in polluted areas like India and China.

In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3–3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20–54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·1015 (kgfuel)−1 in a roadside environment, 2.6·1015 (kgfuel)−1 in a street canyon, and 2.9·1015 (kgfuel)−1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·1012 (kgfuel)−1 to a high value of 4.3·1015 (kgfuel)−1. These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds.

Aerosol–cloud interactions are the largest source of uncertainty in the radiative forcing of the global climate. A phenomenon not included in the estimates of the total net forcing is the potential increase in upper tropospheric humidity (UTH) by anthropogenic aerosols via changes in the microphysics of deep convection. Using remote sensing data over the ocean east of China in summer, we show that increased aerosol loads are associated with an UTH increase of 2.2 ± 1.5 in units of relative humidity. We show that humidification of aerosols or other meteorological covariation is very unlikely to be the cause of this result, indicating relevance for the global climate. In tropical moist air such an UTH increase leads to a regional radiative effect of 0.5 ± 0.4 W m−2. We conclude that the effect of aerosols on UTH should be included in future studies of anthropogenic climate change and climate sensitivity.

Open biomass burning contributes significantly to air quality degradation and associated human health impacts over large areas. It is one of the largest sources of reactive trace gases and fine particles to Earth’s atmosphere and consequently a major source of cloud condensation nuclei on a global scale. However, there is a large uncertainty in the climate effect of open biomass burning aerosols due to the complexity of their constituents. Here, we present an exceptionally large dataset on southern African savannah and grassland fire plumes and their atmospheric evolution, based on 5.5 years of continuous measurements from 2010 to 2015. We find that the mass of submicrometre aerosols more than doubles on average, in only three hours of daytime ageing. We also evaluate biomass burning aerosol particle size distributions and find a large discrepancy between the observations and current model parameterizations, especially in the 30–100 nm range. We conclude that accounting for near-source secondary organic aerosol formation and using measurement-based size distribution parameterizations in smoke plumes is essential to better constrain the climate and air quality effects of savannah and grassland fires.