Finnish Meteorological Institute

Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high-time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.

Abstract This paper discusses the advantages and disadvantages of the different methods that separate net ecosystem exchange (NEE) into its major components, gross ecosystem carbon uptake (GEP) and ecosystem respiration ( R eco ). In particular, we analyse the effect of the extrapolation of night‐time values of ecosystem respiration into the daytime; this is usually done with a temperature response function that is derived from long‐term data sets. For this analysis, we used 16 one‐year‐long data sets of carbon dioxide exchange measurements from European and US‐American eddy covariance networks. These sites span from the boreal to Mediterranean climates, and include deciduous and evergreen forest, scrubland and crop ecosystems. We show that the temperature sensitivity of R eco , derived from long‐term (annual) data sets, does not reflect the short‐term temperature sensitivity that is effective when extrapolating from night‐ to daytime. Specifically, in summer active ecosystems the long‐term temperature sensitivity exceeds the short‐term sensitivity. Thus, in those ecosystems, the application of a long‐term temperature sensitivity to the extrapolation of respiration from night to day leads to a systematic overestimation of ecosystem respiration from half‐hourly to annual time‐scales, which can reach >25% for an annual budget and which consequently affects estimates of GEP. Conversely, in summer passive (Mediterranean) ecosystems, the long‐term temperature sensitivity is lower than the short‐term temperature sensitivity resulting in underestimation of annual sums of respiration. We introduce a new generic algorithm that derives a short‐term temperature sensitivity of R eco from eddy covariance data that applies this to the extrapolation from night‐ to daytime, and that further performs a filling of data gaps that exploits both, the covariance between fluxes and meteorological drivers and the temporal structure of the fluxes. While this algorithm should give less biased estimates of GEP and R eco , we discuss the remaining biases and recommend that eddy covariance measurements are still backed by ancillary flux measurements that can reduce the uncertainties inherent in the eddy covariance data.

Abstract Global climate change impacts can already be tracked in many physical and biological systems; in particular, terrestrial ecosystems provide a consistent picture of observed changes. One of the preferred indicators is phenology, the science of natural recurring events, as their recorded dates provide a high‐temporal resolution of ongoing changes. Thus, numerous analyses have demonstrated an earlier onset of spring events for mid and higher latitudes and a lengthening of the growing season. However, published single‐site or single‐species studies are particularly open to suspicion of being biased towards predominantly reporting climate change‐induced impacts. No comprehensive study or meta‐analysis has so far examined the possible lack of evidence for changes or shifts at sites where no temperature change is observed. We used an enormous systematic phenological network data set of more than 125 000 observational series of 542 plant and 19 animal species in 21 European countries (1971–2000). Our results showed that 78% of all leafing, flowering and fruiting records advanced (30% significantly) and only 3% were significantly delayed, whereas the signal of leaf colouring/fall is ambiguous. We conclude that previously published results of phenological changes were not biased by reporting or publication predisposition: the average advance of spring/summer was 2.5 days decade −1 in Europe. Our analysis of 254 mean national time series undoubtedly demonstrates that species' phenology is responsive to temperature of the preceding months (mean advance of spring/summer by 2.5 days°C −1 , delay of leaf colouring and fall by 1.0 day°C −1 ). The pattern of observed change in spring efficiently matches measured national warming across 19 European countries (correlation coefficient r =−0.69, P <0.001).

Abstract In recent decades, the warming in the Arctic has been much faster than in the rest of the world, a phenomenon known as Arctic amplification. Numerous studies report that the Arctic is warming either twice, more than twice, or even three times as fast as the globe on average. Here we show, by using several observational datasets which cover the Arctic region, that during the last 43 years the Arctic has been warming nearly four times faster than the globe, which is a higher ratio than generally reported in literature. We compared the observed Arctic amplification ratio with the ratio simulated by state-of-the-art climate models, and found that the observed four-fold warming ratio over 1979–2021 is an extremely rare occasion in the climate model simulations. The observed and simulated amplification ratios are more consistent with each other if calculated over a longer period; however the comparison is obscured by observational uncertainties before 1979. Our results indicate that the recent four-fold Arctic warming ratio is either an extremely unlikely event, or the climate models systematically tend to underestimate the amplification.

A proper choice of a proposal distribution for MCMC methods, e.g. for the Metropolis-Hastings algorithm, is well known to be a crucial factor for the convergence of the algorithm. In this paper we introduce an adaptive Metropolis Algorithm (AM), where the Gaussian proposal distribution is updated along the process using the full information cumulated so far. Due to the adaptive nature of the process, the AM algorithm is non-Markovian, but we establish here that it has the correct ergodic properties. We also include the results of our numerical tests, which indicate that the AM algorithm competes well with traditional MetropolisHastings algorithms, and demonstrate that AM provides an easy to use algorithm for practical computation. 1991 Mathematics Subject Classification: 65C05, 65U05. Keywords: adaptive MCMC, comparison, convergence, ergodicity, Markov Chain Monte Carlo, Metropolis-Hastings algorithm 1 Introduction It is generally acknowledged that the choice of an effective proposal...

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric\nlifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations).\nFor the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 TgCH4 yr-1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 TgCH4 yr-1 or 60% is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 TgCH4 yr-1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 TgCH4 yr-1 larger than our estimate for the previous decade (2000–2009), and 24 TgCH4 yr-1 larger than the one reported in the previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30% larger global emissions (737 TgCH4 yr-1, range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-based emissions indicates a predominance of tropical emissions (∼65% of the global budget, <30◦N) compared to mid-latitudes (∼30 %, 30–60◦ N) and high northern latitudes (∼4 %, 60–90◦N). The most important source of uncertainty in the methane budget is attributable to natural emissions, especially those from wetlands and other inland waters.\nSome of our global source estimates are smaller than those in previously published budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 TgCH4 yr-1 lower due to improved partition wetlands and other inland waters. Emissions from geological sources and wild animals are also found to be smaller by 7 TgCH4 yr-1 by 8 TgCH4 yr-1, respectively. However, the overall discrepancy between bottom-up and top-down estimates has been reduced by only 5% compared to Saunois et al. (2016), due to a higher estimate of emissions from inland waters, highlighting the need for more detailed research on emissions factors. Priorities for improving the methane budget include (i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; (ii) further development of process-based models for inland-water emissions; (iii) intensification of methane observations at local scales (e.g., FLUXNET-CH4 measurements) and urban-scale monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane to improve source partitioning.\nThe data presented here can be downloaded from https://doi.org/10.18160/GCP-CH4-2019 (Saunois et al.,\n2020) and from the Global Carbon Project

The Ozone Monitoring Instrument (OMI) flies on the National Aeronautics and Space Administration's Earth Observing System Aura satellite launched in July 2004. OMI is a ultraviolet/visible (UV/VIS) nadir solar backscatter spectrometer, which provides nearly global coverage in one day with a spatial resolution of 13 km/spl times/24 km. Trace gases measured include O/sub 3/, NO/sub 2/, SO/sub 2/, HCHO, BrO, and OClO. In addition, OMI will measure aerosol characteristics, cloud top heights, and UV irradiance at the surface. OMI's unique capabilities for measuring important trace gases with a small footprint and daily global coverage will be a major contribution to our understanding of stratospheric and tropospheric chemistry and climate change. OMI's high spatial resolution is unprecedented and will enable detection of air pollution on urban scale resolution. In this paper, the instrument and its performance will be discussed.

Abstract We present a dataset of daily resolution climatic time series that has been compiled for the European Climate Assessment (ECA). As of December 2001, this ECA dataset comprises 199 series of minimum, maximum and/or daily mean temperature and 195 series of daily precipitation amount observed at meteorological stations in Europe and the Middle East. Almost all series cover the standard normal period 1961–90, and about 50% extends back to at least 1925. Part of the dataset (90%) is made available for climate research on CDROM and through the Internet (at http://www.knmi.nl/samenw/eca ). A comparison of the ECA dataset with existing gridded datasets, having monthly resolution, shows that correlation coefficients between ECA stations and nearest land grid boxes between 1946 and 1999 are higher than 0.8 for 93% of the temperature series and for 51% of the precipitation series. The overall trends in the ECA dataset are of comparable magnitude to those in the gridded datasets. The potential of the ECA dataset for climate studies is demonstrated in two examples. In the first example, it is shown that the winter (October–March) warming in Europe in the 1976–99 period is accompanied by a positive trend in the number of warm‐spell days at most stations, but not by a negative trend in the number of cold‐spell days. Instead, the number of cold‐spell days increases over Europe. In the second example, it is shown for winter precipitation between 1946 and 1999 that positive trends in the mean amount per wet day prevail in areas that are getting drier and wetter. Because of its daily resolution, the ECA dataset enables a variety of empirical climate studies, including detailed analyses of changes in the occurrence of extremes in relation to changes in mean temperature and total precipitation. Copyright © 2002 Royal Meteorological Society.

, water, and energy exchange between the biosphere and the atmosphere, and other meteorological and biological measurements, from 212 sites around the globe (over 1500 site-years, up to and including year 2014). These sites, independently managed and operated, voluntarily contributed their data to create global datasets. Data were quality controlled and processed using uniform methods, to improve consistency and intercomparability across sites. The dataset is already being used in a number of applications, including ecophysiology studies, remote sensing studies, and development of ecosystem and Earth system models. FLUXNET2015 includes derived-data products, such as gap-filled time series, ecosystem respiration and photosynthetic uptake estimates, estimation of uncertainties, and metadata about the measurements, presented for the first time in this paper. In addition, 206 of these sites are for the first time distributed under a Creative Commons (CC-BY 4.0) license. This paper details this enhanced dataset and the processing methods, now made available as open-source codes, making the dataset more accessible, transparent, and reproducible.

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.

Climate change affects human health; however, there have been no large-scale, systematic efforts to quantify the heat-related human health impacts that have already occurred due to climate change. Here, we use empirical data from 732 locations in 43 countries to estimate the mortality burdens associated with the additional heat exposure that has resulted from recent human-induced warming, during the period 1991–2018. Across all study countries, we find that 37.0% (range 20.5–76.3%) of warm-season heat-related deaths can be attributed to anthropogenic climate change and that increased mortality is evident on every continent. Burdens varied geographically but were of the order of dozens to hundreds of deaths per year in many locations. Our findings support the urgent need for more ambitious mitigation and adaptation strategies to minimize the public health impacts of climate change. Current and future climate change is expected to impact human health, both indirectly and directly, through increasing temperatures. Climate change has already had an impact and is responsible for 37% of warm-season heat-related deaths between 1991 and 2018, with increases in mortality observed globally.

Amines at typical atmospheric concentrations of a only few molecules per trillion air molecules combine with sulphuric acid to form highly stable aerosol particles at rates similar to those observed in the lower atmosphere. Amines emitted into the atmosphere from anthropogenic sources are thought to enhance nucleation from trace atmospheric vapours, stimulate particle formation and influence the development and properties of clouds. Direct evidence for this under atmospheric conditions has been lacking; however, this study, using the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN, demonstrates that amines at atmospherically relevant concentrations can sufficiently increase nucleation rates to be able to account for the particle formation rates observed in the atmospheric environment. Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei1. 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 lifetimes2. Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases2. 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 atmosphere3. It is thought that amines may enhance nucleation4,5,6,7,8,9,10,11,12,13,14,15,16, 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.

The near‐Earth neutral line (NENL) model of magnetospheric substorms is reviewed. The observed phenomenology of substorms is discussed including the role of coupling with the solar wind and interplanetary magnetic field, the growth phase sequence, the expansion phase (and onset), and the recovery phase. New observations and modeling results are put into the context of the prior model framework. Significant issues and concerns about the shortcomings of the NENL model are addressed. Such issues as ionosphere‐tail coupling, large‐scale mapping, onset triggering, and observational timing are discussed. It is concluded that the NENL model is evolving and being improved so as to include new observations and theoretical insights. More work is clearly required in order to incorporate fully the complete set of ionospheric, near‐tail, midtail, and deep tail features of substorms. Nonetheless, the NENL model still seems to provide the best available framework for ordering the complex, global manifestations of substorms.

Abstract Terrestrial ecosystems sequester 2.1 Pg of atmospheric carbon annually. A large amount of the terrestrial sink is realized by forests. However, considerable uncertainties remain regarding the fate of this carbon over both short and long timescales. Relevant data to address these uncertainties are being collected at many sites around the world, but syntheses of these data are still sparse. To facilitate future synthesis activities, we have assembled a comprehensive global database for forest ecosystems, which includes carbon budget variables (fluxes and stocks), ecosystem traits (e.g. leaf area index, age), as well as ancillary site information such as management regime, climate, and soil characteristics. This publicly available database can be used to quantify global, regional or biome‐specific carbon budgets; to re‐examine established relationships; to test emerging hypotheses about ecosystem functioning [e.g. a constant net ecosystem production (NEP) to gross primary production (GPP) ratio]; and as benchmarks for model evaluations. In this paper, we present the first analysis of this database. We discuss the climatic influences on GPP, net primary production (NPP) and NEP and present the CO 2 balances for boreal, temperate, and tropical forest biomes based on micrometeorological, ecophysiological, and biometric flux and inventory estimates. Globally, GPP of forests benefited from higher temperatures and precipitation whereas NPP saturated above either a threshold of 1500 mm precipitation or a mean annual temperature of 10 °C. The global pattern in NEP was insensitive to climate and is hypothesized to be mainly determined by nonclimatic conditions such as successional stage, management, site history, and site disturbance. In all biomes, closing the CO 2 balance required the introduction of substantial biome‐specific closure terms. Nonclosure was taken as an indication that respiratory processes, advection, and non‐CO 2 carbon fluxes are not presently being adequately accounted for.

Abstract. Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.

Abstract Aerosol‐planetary boundary layer (PBL) interactions have been found to enhance air pollution in megacities in China. We show that black carbon (BC) aerosols play the key role in modifying the PBL meteorology and hence enhancing the haze pollution. With model simulations and data analysis from various field observations in December 2013, we demonstrate that BC induces heating in the PBL, particularly in the upper PBL, and the resulting decreased surface heat flux substantially depresses the development of PBL and consequently enhances the occurrences of extreme haze pollution episodes. We define this process as the “dome effect” of BC and suggest an urgent need for reducing BC emissions as an efficient way to mitigate the extreme haze pollution in megacities of China.

Nucleation is a fundamental step in atmospheric new-particle formation. However, laboratory experiments on nucleation have systematically failed to demonstrate sulfuric acid particle formation rates as high as those necessary to account for ambient atmospheric concentrations, and the role of sulfuric acid in atmospheric nucleation has remained a mystery. Here, we report measurements of new particles (with diameters of approximately 1.5 nanometers) observed immediately after their formation at atmospherically relevant sulfuric acid concentrations. Furthermore, we show that correlations between measured nucleation rates and sulfuric acid concentrations suggest that freshly formed particles contain one to two sulfuric acid molecules, a number consistent with assumptions that are based on atmospheric observations. Incorporation of these findings into global models should improve the understanding of the impact of secondary particle formation on climate.

Abstract. The Meteorological Synthesizing Centre-West (MSC-W) of the European Monitoring and Evaluation Programme (EMEP) has been performing model calculations in support of the Convention on Long Range Transboundary Air Pollution (CLRTAP) for more than 30 years. The EMEP MSC-W chemical transport model is still one of the key tools within European air pollution policy assessments. Traditionally, the model has covered all of Europe with a resolution of about 50 km × 50 km, and extending vertically from ground level to the tropopause (100 hPa). The model has changed extensively over the last ten years, however, with flexible processing of chemical schemes, meteorological inputs, and with nesting capability: the code is now applied on scales ranging from local (ca. 5 km grid size) to global (with 1 degree resolution). The model is used to simulate photo-oxidants and both inorganic and organic aerosols. In 2008 the EMEP model was released for the first time as public domain code, along with all required input data for model runs for one year. The second release of the EMEP MSC-W model became available in mid 2011, and a new release is targeted for summer 2012. This publication is intended to document this third release of the EMEP MSC-W model. The model formulations are given, along with details of input data-sets which are used, and a brief background on some of the choices made in the formulation is presented. The model code itself is available at www.emep.int, along with the data required to run for a full year over Europe.

Forest microclimates contrast strongly with the climate outside forests. To fully understand and better predict how forests' biodiversity and functions relate to climate and climate change, microclimates need to be integrated into ecological research. Despite the potentially broad impact of microclimates on the response of forest ecosystems to global change, our understanding of how microclimates within and below tree canopies modulate biotic responses to global change at the species, community and ecosystem level is still limited. Here, we review how spatial and temporal variation in forest microclimates result from an interplay of forest features, local water balance, topography and landscape composition. We first stress and exemplify the importance of considering forest microclimates to understand variation in biodiversity and ecosystem functions across forest landscapes. Next, we explain how macroclimate warming (of the free atmosphere) can affect microclimates, and vice versa, via interactions with land-use changes across different biomes. Finally, we perform a priority ranking of future research avenues at the interface of microclimate ecology and global change biology, with a specific focus on three key themes: (1) disentangling the abiotic and biotic drivers and feedbacks of forest microclimates; (2) global and regional mapping and predictions of forest microclimates; and (3) the impacts of microclimate on forest biodiversity and ecosystem functioning in the face of climate change. The availability of microclimatic data will significantly increase in the coming decades, characterizing climate variability at unprecedented spatial and temporal scales relevant to biological processes in forests. This will revolutionize our understanding of the dynamics, drivers and implications of forest microclimates on biodiversity and ecological functions, and the impacts of global changes. In order to support the sustainable use of forests and to secure their biodiversity and ecosystem services for future generations, microclimates cannot be ignored.

About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer. Although recent studies predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Köhler theory), has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10(-4.5) micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10(-4.5) to 10(-0.5) micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.