How Particles Nucleate and Grow

New particle formation (NPF) in the atmosphere i.e. nucleation of gas phase precursors and continuing condensa- tional growth is a crucial secondary transformation process. The freshly nucleated particles can grow into sizes where they can act as cloud condensation nuclei (CCN) and further influence cloud and climate-relevant properties. Hence, the detailed knowledge on the formation mechanisms of new particles and their subsequent growth will help us to improve our under- standing on the regional air pollution and global climate change. Recent-developed measurement techniques enable to ex- plore atmospheric nucleation by measuring particles/clusters down to 1 nm. NPF events have been observed in a variety of atmospheric environments. Several methods including field observation, laboratory simulations and model calculations are implemented to investigate the nucleation mechanisms and growth properties. Good agreement between particle formation rates and gaseous sulfuric acid concentrations is observed, indicating that sulfuric acid is a key compnent in the atmospheric nucleation process. In addition, the low-volatile organic vapors are found to be involved in new particle formation. However, the huge variations of the particle formation and growth rates in diverse atmospheric environments suggest that a consistent picture on formation mechanisms of new particles does not achieve. Long-term continuous measurements of NPF events have been first performed in the urban atmosphere of Beijing since 2004. Up to now, NPF events have been observed in many different environments, including coastal area, high-elevation mountain, rural site as well as urban region in China. The cur- rent nucleation mechanisms are developed based on the observation in clean environment. Hence, whether it could well ex- plain the NPF events occurred in the polluted atmosphere with strong oxidation capacity is a key issue to be addressed in further studies. This paper reviews the measurement techniques for investigating atmospheric new particle formation and growth, summarizes the observation results in various typical environments, introduces the current understanding of the nu- cleation mechanisms and discusses the main scientific questions that need further researches. Keywords new particle formation; nucleation mechanism; growth property; measurement technique; precursor 1 引言

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011–2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties.There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of −24% and −35% for particles with dry diameters > 50 and > 120nm, as well as −36% and −34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (< 0.1 %) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN0.2) compared to that for N3, maximizing over regions where new particle formation is important.An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter.Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120 nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer.In contrast to the large spread in simulated aerosol particle and CCN number concentrations, the CDNC derived from simulated CCN spectra is less diverse and in better agreement with CDNC estimates consistently derived from the observations (average NMB −13% and −22% for updraft velocities 0.3 and 0.6 ms−1, respectively). In addition, simulated CDNC is in slightly better agreement with observationally derived values at lower than at higher updraft velocities (index of agreement 0.64 vs. 0.65). The reduced spread of CDNC compared to that of CCN is attributed to the sublinear response of CDNC to aerosol particle number variations and the negative correlation between the sensitivities of CDNC to aerosol particle number concentration (∂Nd/∂Na) and to updraft velocity (∂Nd/∂w). Overall, we find that while CCN is controlled by both aerosol particle number and composition, CDNC is sensitive to CCN at low and moderate CCN concentrations and to the updraft velocity when CCN levels are high. Discrepancies are found in sensitivities ∂Nd/∂Na and ∂Nd/∂w; models may be predisposed to be too “aerosol sensitive” or “aerosol insensitive” in aerosol–cloud–climate interaction studies, even if they may capture average droplet numbers well. This is a subtle but profound finding that only the sensitivities can clearly reveal and may explain inter-model biases on the aerosol indirect effect.

Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei. Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes. Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases. However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere. It is thought that amines may enhance nucleation, but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid-amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid-dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.

Abstract. Atmospheric aerosol particles serving as Cloud Condensation Nuclei (CCN) are key elements of the hydrological cycle and climate. We measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign from 1–30 July 2006 at a rural site ~60 km northwest of the mega-city Guangzhou in southeastern China. CCN efficiency spectra (activated fraction vs. dry particle diameter; 20–290 nm) were recorded at water vapor supersaturations (S) in the range of 0.068% to 1.27%. The corresponding effective hygroscopicity parameters describing the influence of particle composition on CCN activity were in the range of κ≈0.1–0.5. The campaign average value of κ=0.3 equals the average value of κ for other continental locations. During a strong local biomass burning event, the average value of κ dropped to 0.2, which can be considered as characteristic for freshly emitted smoke from the burning of agricultural waste. At low S (≤0.27%), the maximum activated fraction remained generally well below one, indicating substantial portions of externally mixed CCN-inactive particles with much lower hygroscopicity – most likely soot particles (up to ~60% at ~250 nm). The mean CCN number concentrations (NCCN,S) ranged from 1000 cm−3 at S=0.068% to 16 000 cm−3 at S=1.27%, which is about two orders of magnitude higher than in pristine air. Nevertheless, the ratios between CCN concentration and total aerosol particle concentration (integral CCN efficiencies) were similar to the ratios observed in pristine continental air (~6% to ~85% at S=0.068% to 1.27%). Based on the measurement data, we have tested different model approaches for the approximation/prediction of NCCN,S. Depending on S and on the model approach, the relative deviations between observed and predicted NCCN,S ranged from a few percent to several hundred percent. The largest deviations occurred at low S with a simple power law. With a Köhler model using variable κ values obtained from individual CCN efficiency spectra, the relative deviations were on average less than ~10% and hardly exceeded 20%, confirming the applicability of the κ-Köhler model approach for efficient description of the CCN activity of atmospheric aerosols. Note, however, that different types of κ-parameters must be distinguished for external mixtures of CCN-active and -inactive aerosol particles (κa, κt, κcut). Using a constant average hygroscopicity parameter (κ=0.3) and variable size distributions as measured, the deviations between observed and predicted CCN concentrations were on average less than 20%. In contrast, model calculations using variable hygroscopicity parameters as measured and constant size distributions led to much higher deviations: ~70% for the campaign average size distribution, ~80% for a generic rural size distribution, and ~140% for a generic urban size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this study should enable efficient description of the CCN activity of atmospheric aerosols in detailed process models as well as in large-scale atmospheric and climate models.

Abstract. We have investigated the formation and early growth of atmospheric secondary aerosol particles building on atmospheric measurements. The measurements were part of the QUEST 2 campaign which took place in spring 2003 in Hyytiälä (Finland). During the campaign numerous aerosol particle formation events occurred of which 15 were accompanied by gaseous sulphuric acid measurements. Our detailed analysis of these 15 events is focussed on nucleation and early growth (to a diameter of 3 nm) of fresh particles. It revealed that new particle formation seems to be a function of the gaseous sulphuric acid concentration to the power from one to two when the time delay between the sulphuric acid and particle number concentration is taken into account. From the time delay the growth rates of freshly nucleated particles from 1 nm to 3 nm were determined. The mean growth rate was 1.2 nm/h and it was clearly correlated with the gaseous sulphuric acid concentration. We tested two nucleation mechanisms – recently proposed cluster activation and kinetic type nucleation – as possible candidates to explain the observed dependences, and determined experimental nucleation coefficients. We found that some events are dominated by the activation mechanism and some by the kinetic mechanism. Inferred coefficients for the two nucleation mechanisms are the same order of magnitude as chemical reaction coefficients in the gas phase and they correlate with the product of gaseous sulphuric acid and ammonia concentrations. This indicates that besides gaseous sulphuric acid also ammonia has a role in nucleation.

&amp;lt;p&amp;gt;The Cloud Condensation Nuclei (CCN) budget, the aerosol particles population that could become cloud droplets, can be influenced by primary aerosol particles emitted by different sources (anthropogenic or biogenic) or by secondary particles that have undergone growth processes or chemical transformations. Aerosol particles originated by nucleation of precursor gases in the atmosphere have been identified as an important source of CCN particles. The influence of New Particle Formation (NPF) events to CCN concentrations is highly dependent on the environment where it takes place. Specifically, the study of the influence of NPF events on CCN concentration at high-altitude sites, where atmospheric conditions favor the formation of clouds, is a very interesting scientific goal.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;&amp;amp;#160;&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;This study presents CCN measurements combined with aerosol size distribution at a high-altitude station in the South East of Spain: a remote high mountain site (Sierra Nevada; SNS, 2500 m a.s.l.). Due to its high altitude, the aerosol particles over SNS station are often representative of pristine free troposphere conditions, especially in winter and nighttime. During summer, SNS station is frequently influenced by transport of pollutants from Granada city to Sierra Nevada station as a result of mixing layer growth and the activation of the mountain-valley breeze phenomenon as well as by NPF events at midday (De Arruda Moreira et al., 2019; Casquero-Vera et al., 2020).&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;&amp;amp;#160;&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;In this study, we analyze the influence of NPF events to CCN concentrations during summer 2019 at the SNS high-altitude station. The study period (from June to August of 2019) was characterized by 67 NPF events, 16 undefined events and 13 non-events days. Following Rose et al. (2017) criteria, only those NPF events referred as type I, i.e. with clear particle growth from smallest sizes, were selected to investigate the contribution of NPF events on CCN concentrations. In this sense, we selected the 15 clearest NPF events for this analysis.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;&amp;amp;#160;&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;Results show clear differences in the diurnal evolution of CCN concentration between NPF event and non-event days, demonstrating the large influence of NPF to CCN concentrations, especially at high supersaturations (Rejano et al., 2021). NPF events have been estimated to increase the CCN concentrations by 175% at SS=0.5%, evidencing NPF events as one of the major CCN source at this mountain site&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;&amp;amp;#160;&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;&amp;amp;#160;&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;&amp;lt;strong&amp;gt;Acknowledgments&amp;lt;/strong&amp;gt;: This work was supported by the European Union's Horizon 2020 research and innovation programme through project ACTRIS 2 (grant agreement No 654109), by the Spanish Ministry of Economy and Competitiveness through projects CGL2016-81092-R, CGL2017-90884-REDT and RTI2018-101154-A-I00 and by University of Granada Plan Propio through Visiting Scholars program. The Spanish Ministry of Universities funds Fernando Rejano under the predoctoral program FPU (FPU19/05340).&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;&amp;amp;#160;&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;&amp;lt;strong&amp;gt;References&amp;lt;/strong&amp;gt;&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;Casquero-Vera, et al. (2020) Atmos. Chem. Phys. &amp;lt;strong&amp;gt;20, &amp;lt;/strong&amp;gt;14253&amp;amp;#8211;14271.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;De Arruda Moreira et al. (2019) Atmos. Chem. Phys. &amp;lt;strong&amp;gt;19&amp;lt;/strong&amp;gt;, 1263-1280.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;Rejano et al. (2021) Sci. Tot Envi., &amp;lt;strong&amp;gt;762&amp;lt;/strong&amp;gt;, 143100.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;Rose et al. (2017) Atmos. Chem. Phys. &amp;lt;strong&amp;gt;17&amp;lt;/strong&amp;gt;, 1529-1541.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;tract HTML here.&amp;lt;/p&amp;gt;

This study was part of the international field measurement Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing‐2006). We investigated a new particle formation event in a highly polluted air mass at a regional site south of the megacity Beijing and its impact on the abundance and properties of cloud condensation nuclei (CCN). During the 1‐month observation, particle nucleation followed by significant particle growth on a regional scale was observed frequently (∼30%), and we chose 23 August 2006 as a representative case study. Secondary aerosol mass was produced continuously, with sulfate, ammonium, and organics as major components. The aerosol mass growth rate was on average 19 μg m−3 h−1 during the late hours of the day. This growth rate was observed several times during the 1‐month intensive measurements. The nucleation mode grew very quickly into the size range of CCN, and the CCN size distribution was dominated by the growing nucleation mode (up to 80% of the total CCN number concentration) and not as usual by the accumulation mode. At water vapor supersaturations of 0.07–0.86%, the CCN number concentrations reached maximum values of 4000–19,000 cm−3 only 6–14 h after the nucleation event. During particle formation and growth, the effective hygroscopicity parameter κ increased from about 0.1–0.3 to 0.35–0.5 for particles with diameters of 40–90 nm, but it remained nearly constant at ∼0.45 for particles with diameters of ∼190 nm. This result is consistent with aerosol chemical composition data, showing a pronounced increase of sulfate.

In this study, the observation site Himalayan Cloud Observatory is located at the high-altitude location (30.34 N, 78.40 E, 1706 m above mean sea level) and established at Swami Ram Tirth Campus, Badshahithaul, Tehri Garhwal, Uttarakhand in the western Himalaya. We have identified and characterized the new particle formation events for 12-months period (January to December, 2021) of continuous monitoring of the aerosol size distribution using NanoScan Scanning Mobility Particle Sizer. Another year-long observation was carried out at the Himalayan Atmospheric and Space Physics Research Laboratory (HASPRL), Department of Physics, Hemvati Nandan Bahuguna Garhwal University (A Central University), Srinagar Garhwal, Uttarakhand, in the Alaknanda Valley (30°13'37.3"N, 78°48'14.2"E, 640 m AMSL), from January 1, 2023, to December 31, 2023.We have observed 51 new particle formation events out of 278 days of observations having 14% frequency of new particle formation occurrence. New particle formation events were most frequent in March-April-May (pre-monsoon) and least frequent in June-July-August-September (monsoon). This trend is linked to high temperatures, strong solar radiation, and low relative humidity in pre-monsoon, which enhance the formation of low-volatility organic compounds, while in monsoon, wet scavenging reduces aerosol precursor gases. The seasonal mean of growth rate (GR11.5-27.4 nm), formation rate (J11.5), coagulation sink (CoagS11.5-27.4) and condensation sink (CSTOT, 11.5-154 nm) during the study period were 1.27±0.23 nm h-1, 0.12±0.08 cm-3 s-1, 2.92±1.65×10-5 s-1 and 9.91±3.13×10-3 s-1 respectively. Seasonal distributions show particles within 11.5–100 nm predominantly originate from secondary emissions, while particles 100–154 nm result from both direct and nucleated process, highlighting the seasonal sources of particles at Himalayan Cloud Observatory. A significant reduction (by 25%) found in incoming solar radiation on non-event days limits the oxidation of precursor gases, thereby inhibiting particle formation. Polar bivariate analysis reveals that winter airmasses, transported via mountain winds from the southwest and northeast, introduce mixed particle sizes. In contrast, the localized concentration of particles with elevated GR11.5-27.4 nm and J11.5 during pre-monsoon highlights the role of aerosol precursors, condensable vapors, and favorable meteorological conditions, emphasizing new particle formation as the dominant particle source. Comparison with prior cloud condensation nuclei study at Himalayan Cloud Observatory reveals that new particle formation significantly supplements cloud condensation nuclei production beyond primary emissions, especially in pre-monsoon. The satellite-based observation of sulfur dioxide and formaldehyde complement and support the condensable vapours during event days at Himalayan Cloud Observatory. At HASPRL, smaller-sized aerosol particles showed an increase in the morning, likely due to emissions from anthropogenic sources originating from the southwest. In the evening, larger-sized aerosol particles were observed to increase, possibly resulting from various human activities such as vehicular emissions, transportation of sand and stone, and other anthropogenic emissions from the southeast. At HCO, particle transport is likely influenced by movement from valley and forested regions, with air masses traveling from the southeast to the southwest.In summary, this research offers fresh perspectives on the characterization of new particle formation events in the Himalayan region of Uttarakhand. These insights are crucial for comprehending secondary aerosol formation processes worldwide, particularly at the process level.

The hygroscopic and cloud condensation nuclei (CCN) properties of submicrometer atmospheric aerosol particles were investigated using an Ultrafine Tandem Differential Mobility Analyzer (UF‐TDMA) and a CCN counter at the Mace Head Monitoring Station on the west coast of Ireland during the New Particle Formation and Fate in the Coastal Environment (PARFORCE) field campaign in September 1998 and June 1999. These measurements give indirect in situ information on the composition and state of mixing of the aerosol particles. The UF‐TDMA was used for monitoring of hygroscopic diameter growth factors of aerosol particles with dry mobility diameters 8–20 nm when taken from dry state to a controlled humid environment (RH 90%). The CCN counter was used to study the activation of aerosol particles when exposed to supersaturated conditions (dry diameters of 15–150 nm). It was seen that in clean marine air masses during the observed particle formation events, the newly formed nucleation mode particles (8 and 10 nm) most often had low growth factors (between 1.0 and 1.1) resulting from low solubility. This indicates that the nucleation mode particles consist of nonsoluble or weakly soluble species, possible accompanied by a small soluble part; however, when nucleation mode particles were observed outside the event periods, the growth factors were higher (about 1.3–1.4). In contrast, the 20 nm particles usually clearly belonged to the Aitken mode (based on number size distribution measurements) and had hygroscopic properties similar to some common salts (growth factors 1.4–1.5).

Aircraft observations were performed over the sea near the southwest islands of Japan under Asian Atmospheric Particulate Environmental Change Experiment 2/Asian Pacific Regional Aerosol Characterization Experiment (APEX‐E2/ACE‐Asia) project during the period of 16–28 April 2001. The polluted air mass from east Asia was associated with very high concentrations of SO2 (1–10 ppb) and aerosol particles (3000–5000 cm−3) in the marine boundary layer. The cloud condensation nuclei (CCN) concentration at 0.3% supersaturation was as high as 800–2000 cm−3 during the penetrations of air pollutants from east Asia. The correlation coefficient between SO2 and aerosol particles was significant in such polluted atmosphere. Concentration of CCN (NCCN) was linearly related to concentration of aerosol particles (NAP) according to NCCN ∼ 0.75NAP. The ratio of CCN to aerosol condensation nuclei particle concentrations was lower than 0.3 in the relatively clean maritime atmosphere, but it was as high as ∼0.5 in the continentally influenced atmosphere in the boundary layer. These results indicated that the influence of anthropogenic pollutants from east Asia increased the contribution percentage of aerosol particles to CCN in the polluted atmosphere over the observation area. The observational results also indicated that a mean cloud droplet concentration (NC) in the continentally influenced clouds was ∼2 times as much as NC in the relatively clean maritime clouds. The slope of log‐log relationship between NC and NCCN was ∼0.39. This study strongly suggests that high CCN concentration formed many cloud droplets and decreased their effective radius at similar liquid water content under the outflow of air pollutants from east Asia.

How tiny aerosol particles form and grow from vapours produced by vegetation has been a mystery. The finding that highly oxygenated products form directly from volatile organic compounds may offer the solution. See Letter p.476 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.

The process of new particle formation from gas-phase precursors holds significant importance in Earth's atmosphere and introduces a notable source of uncertainty in climate change predictions. The growth of freshly formed molecular clusters should in theory be crucial for the climate impact of new particle formation, influencing the survival probability of these particles exponentially and determining their ability to act as cloud condensation nuclei. However, defining the fundamental aspects of nanoparticle growth is intricate. It involves a complex interplay of condensational and reactive vapor uptake, aerosol coagulation, sink processes, and a diverse array of potential gaseous precursors. Observational nanoparticle growth rates, derived from the evolution of the particle-size distribution, portray growth as a collective phenomenon. However, models often interpret these rates at a single-particle level, integrating them into simplified size-distribution representations (Stolzenburg et al., 2023). dditionally, many models only consider a limited subset of condensable vapors, while recent experimental observations identify an increasing number of potential contributors to new particle growth.Our objective here is to bridge the gap between experimental and modeling studies on nanoparticle growth. We compare three large-scale models (NorESM, ECHAM, and TM5) regarding their sensitivity to organic nanoparticle growth processes. Surprisingly, we find a much lower sensitivity than anticipated from box models. Through the inclusion of a sectional scheme into NorESM, we demonstrate that representing the complexity of size distribution dynamics leads to significantly different cloud condensation nuclei (CCN) levels. Furthermore, our results suggest that, on regional scales, sensitivity to organic growth is much higher. Inclusion of additional growth processes and/or a scaling of condensable vapor concentrations could yield a significantly altered climate response. In turn, comprehensive experimental observations from e.g. the open oceans are still lacking and we show that continental data exhibit surprisingly little variation in measured particle growth rates. The latter indicates limited sensitivity in current experimental approaches and potential unaccounted multi-phase chemistry in the growth process.Consequently, we propose specific guidance for future research to address questions regarding the buffered climate response in large-scale models and the unexpectedly low variation observed in global growth measurements. We advocate for more sensitivity studies and improved model-measurement comparisons.

Styrene miniemulsion polymerizations stabilized by sodium lauryl sulfate in combination with a reactive costabilizer, lauryl methacrylate (LMA) or stearyl methacrylate (SMA), were studied. A small amount of extremely hydrophobic dye was incorporated into monomer droplets (102 nm in diameter) to investigate particle nucleation and growth mechanisms. In addition to monomer droplet nucleation, particle nuclei generated in the aqueous phase (homogeneous nucleation) also play an important role in both LMA‐ and SMA‐containing polymerization systems. The way that these two nucleation mechanisms compete with each other is closely related to the water solubility of the costabilizer (LMA &gt; SMA). The fraction of latex particles originating from homogeneous nucleation increases with decreasing hydrophobicity of the costabilizer. Zeta potential data of latex particles and the molecular weight and molecular weight distribution of emulsion polymers provide supporting evidence for the proposed competitive particle nucleation and growth mechanisms.© 2002 Society of Chemical Industry

&amp;lt;p&amp;gt;Even though oceans cover over 70% of the Earth&amp;amp;#8217;s surface, the ways in which oceans interact with climate are not fully known. Marine micro-organisms such as phytoplankton can play an important role in regulating climate by releasing different chemical species into air. In air these chemical species can react and form new aerosol particles. If grown to large enough sizes, aerosols can influence climate by acting as cloud condensation nuclei which influence the formation and properties of clouds. Even though a connection of marine biology and climate through aerosol formation was first proposed already over 30 years ago, the processes related to this connection are still uncertain.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;To unravel how seawater properties affect aerosol formation and to identify which chemical species are responsible for aerosol formation, we built two Air-Sea-Interaction Tanks (ASIT) that isolate 1000 l of seawater and 1000 l of air directly above the water. The used seawater was collected from different locations during a ship campaign on board the R/V Tangaroa in the South West Pacific Ocean, close to Chatham Rise, east of New Zealand. Seawater from one location was kept in the tanks for 2-3 days and then changed. By using seawater collected from different locations, we could obtain water with different biological populations. To monitor the seawater, we took daily samples to determine its chemical and biological properties.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;The air in the tanks was continuously flushed with particle filtered air. This way the air had on average 40 min to interact with the seawater surface before being sampled. Our air sampling was continuous and consisted of aerosol and air chemistry measurements. The instrumentation included measurements of aerosol number concentration from 1 to 500 nm and&amp;amp;#160; chemical species ranging from ozone and sulphur dioxide to volatile organic compounds and chemical composition of molecular clusters.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;Joining the seawater and atmospheric data together can give us an idea of what chemical species are emitted from the water into the atmosphere and whether these species can form new aerosol particles. Our preliminary results show a small number of particles in the freshly nucleated size range of 1-3 nm in the ASIT headspaces, indicating that new aerosol particles can form in the ASIT headspaces. In this presentation, we will also explore which chemical species could be responsible for aerosol formation and which plankton groups could be related to the emissions of these species. Combining these results with ambient data and modelling work can shed light on how important new particle formation from marine sources is for climate.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;Acknowledgements: Sea2Cloud project is funded by European Research Council (ERC) under the European Union&amp;amp;#8217;s Horizon 2020 research and innovation programme (Grant agreement No. 771369).&amp;lt;/p&amp;gt;

This article summarizes and compares the analysis of the surfaces of natural aerosol particles from three different forest environments by vibrational sum frequency generation. The experiments were carried out directly on filter and impactor substrates, without the need for sample preconcentration, manipulation, or destruction. We discuss the important first steps leading to secondary organic aerosol (SOA) particle nucleation and growth from terpene oxidation by showing that, as viewed by coherent vibrational spectroscopy, the chemical composition of the surface region of aerosol particles having sizes of 1 μm and lower appears to be close to size-invariant. We also discuss the concept of molecular chirality as a chemical marker that could be useful for quantifying how chemical constituents in the SOA gas phase and the SOA particle phase are related in time. Finally, we describe how the combination of multiple disciplines, such as aerosol science, advanced vibrational spectroscopy, meteorology, and chemistry can be highly informative when studying particles collected during atmospheric chemistry field campaigns, such as those carried out during HUMPPA-COPEC-2010, AMAZE-08, or BEARPEX-2009, and when they are compared to results from synthetic model systems such as particles from the Harvard Environmental Chamber (HEC). Discussions regarding the future of SOA chemical analysis approaches are given in the context of providing a path toward detailed spectroscopic assignments of SOA particle precursors and constituents and to fast-forward, in terms of mechanistic studies, through the SOA particle formation process.