Items

Advanced search

Cluster analysis of European surface ozone observations for evaluation of MACC reanalysis data

The high density of European surface ozone monitoring sites provides unique opportunities for the investigation of regional ozone representativeness and for the evaluation of chemistry climate models. The regional representativeness of European ozone measurements is examined through a cluster analysis (CA) of 4 years of 3-hourly ozone data from 1492 European surface monitoring stations in the Airbase database; the time resolution corresponds to the output frequency of the model that is compared to the data in this study. K-means clustering is implemented for seasonal–diurnal variations (i) in absolute mixing ratio units and (ii) normalized by the overall mean ozone mixing ratio at each site. Statistical tests suggest that each CA can distinguish between four and five different ozone pollution regimes. The individual clusters reveal differences in seasonal–diurnal cycles, showing typical patterns of the ozone behavior for more polluted stations or more rural background. The robustness of the clustering was tested with a series of k-means runs decreasing randomly the size of the initial data set or lengths of the time series. Except for the Po Valley, the clustering does not provide a regional differentiation, as the member stations within each cluster are generally distributed all over Europe. The typical seasonal, diurnal, and weekly cycles of each cluster are compared to the output of the multi-year global reanalysis produced within the Monitoring of Atmospheric Composition and Climate (MACC) project. While the MACC reanalysis generally captures the shape of the diurnal cycles and the diurnal amplitudes, it is not able to reproduce the seasonal cycles very well and it exhibits a high bias up to 12 nmol mol−1. The bias decreases from more polluted clusters to cleaner ones. Also, the seasonal and weekly cycles and frequency distributions of ozone mixing ratios are better described for clusters with relatively clean signatures. Due to relative sparsity of CO and NOx measurements these were not included in the CA. However, simulated CO and NOx mixing ratios are consistent with the general classification into more polluted and more background sites. Mean CO mixing ratios are within 140–145 nmol mol−1 (CL1–CL3) and 130–135 nmol mol−1 (CL4 and CL5), and NOx mixing ratios are within 4–6 nmol mol−1 and 2–3 nmol mol−1, respectively. These results confirm that relatively coarse-scale global models are more suitable for simulation of regional background concentrations, which are less variable in space and time. We conclude that CA of surface ozone observations provides a powerful and robust way to stratify sets of stations, being thus more suitable for model evaluation.
Precipitation regime and stable isotopes at Dome Fuji, East Antarctica

A unique set of 1-year precipitation and stable water isotope measurements from the Japanese Antarctic station, Dome Fuji, has been used to study the impact of the synoptic situation and the precipitation origin on the isotopic composition of precipitation on the Antarctic Plateau. The Antarctic Mesoscale Prediction System (AMPS) archive data are used to analyse the synoptic situations that cause precipitation. These situations are investigated and divided into five categories. The most common weather situation during a precipitation event is an upper-level ridge that extends onto the Antarctic Plateau and causes strong northerly advection from the ocean. Most precipitation events are associated with an increase in temperature and wind speed, and a local maximum of δ18O. During the measurement period, 21 synoptically caused precipitation events caused 60 % of the total annual precipitation, whereas the remaining 40 % were predominantly attributed to diamond dust. By combining the synoptic analyses with 5-day back-trajectories, the moisture source regions for precipitation events were estimated. An average source region around a latitude of 55° S was found. The atmospheric conditions in the source region were used as initial conditions for running a Rayleigh-type isotopic model in order to reproduce the measured isotopic composition of fresh snow and to investigate the influence of the precipitation source region on the isotope ratios. The model represents the measured annual cycle of δ18O and the second-order isotopic parameter deuterium excess reasonably well, but yields on average too little fractionation along the transport/cooling path. While simulations with an isotopic general circulation model (GCM) (ECHAM5-wiso) for Dome Fuji are on average closer to the observations, this model cannot reproduce the annual cycle of deuterium excess. In the event-based analysis, no evidence of a correlation of the measured deuterium excess with the latitude of the moisture source region or the corresponding conditions was identified. Contrary to the assumption used for decades in ice core studies, a more northerly moisture source does not necessarily mean a larger temperature difference between source area and deposition site, thus a more depleted precipitation in heavy isotopes with a higher deuterium excess.
Synergistic use of Lagrangian dispersion and radiative transfer modelling with satellite and surface remote sensing measurements for the investigation of volcanic plumes: the Mount Etna eruption of 25–27 October 2013

In this paper we combine SO2 and ash plume dispersion modelling with satellite and surface remote sensing observations to study the regional influence of a relatively weak volcanic eruption from Mount Etna on the optical and micro-physical properties of Mediterranean aerosols. We analyse the Mount Etna eruption episode of 25–27 October 2013. The evolution of the plume along the trajectory is investigated by means of the FLEXible PARTicle Lagrangian dispersion (FLEXPART) model. The satellite data set includes true colour images, retrieved values of volcanic SO2 and ash, estimates of SO2 and ash emission rates derived from MODIS (MODerate resolution Imaging Spectroradiometer) observations and estimates of cloud top pressure from SEVIRI (Spinning Enhanced Visible and InfraRed Imager). Surface remote sensing measurements of aerosol and SO2 made at the ENEA Station for Climate Observations (35.52° N, 12.63° E; 50 m a.s.l.) on the island of Lampedusa are used in the analysis. The combination of these different data sets suggests that SO2 and ash, despite the initial injection at about 7.0 km altitude, reached altitudes around 10–12 km and influenced the column average aerosol particle size distribution at a distance of more than 350 km downwind. This study indicates that even a relatively weak volcanic eruption may produce an observable effect on the aerosol properties at the regional scale. The impact of secondary sulfate particles on the aerosol size distribution at Lampedusa is discussed and estimates of the clear-sky direct aerosol radiative forcing are derived. Daily shortwave radiative forcing efficiencies, i.e. radiative forcing per unit AOD (aerosol optical depth), are calculated with the LibRadtran model. They are estimated between −39 and −48 W m−2 AOD−1 at the top of the atmosphere and between −66 and −49 W m−2 AOD−1 at the surface, with the variability in the estimates mainly depending on the aerosol single scattering albedo. These results suggest that sulfate particles played a large role in the transported plume composition and radiative forcing, while the contribution by ash particles was small in the volcanic plume arriving at Lampedusa during this event.
Continental anthropogenic primary particle number emissions

Atmospheric aerosol particle number concentrations impact our climate and health in ways different from those of aerosol mass concentrations. However, the global, current and future anthropogenic particle number emissions and their size distributions are so far poorly known. In this article, we present the implementation of particle number emission factors and the related size distributions in the GAINS (Greenhouse Gas–Air Pollution Interactions and Synergies) model. This implementation allows for global estimates of particle number emissions under different future scenarios, consistent with emissions of other pollutants and greenhouse gases. In addition to determining the general particulate number emissions, we also describe a method to estimate the number size distributions of the emitted black carbon particles. The first results show that the sources dominating the particle number emissions are different to those dominating the mass emissions. The major global number source is road traffic, followed by residential combustion of biofuels and coal (especially in China, India and Africa), coke production (Russia and China), and industrial combustion and processes. The size distributions of emitted particles differ across the world, depending on the main sources: in regions dominated by traffic and industry, the number size distribution of emissions peaks in diameters range from 20 to 50 nm, whereas in regions with intensive biofuel combustion and/or agricultural waste burning, the emissions of particles with diameters around 100 nm are dominant. In the baseline (current legislation) scenario, the particle number emissions in Europe, Northern and Southern Americas, Australia, and China decrease until 2030, whereas especially for India, a strong increase is estimated. The results of this study provide input for modelling of the future changes in aerosol–cloud interactions as well as particle number related adverse health effects, e.g. in response to tightening emission regulations. However, there are significant uncertainties in these current emission estimates and the key actions for decreasing the uncertainties are pointed out.
Three-North Shelter Forest Program contribution to long-term increasing trends of biogenic isoprene emissions in northern China

To assess the long-term trends of isoprene emissions in northern China and the impact of the Three-North Shelter Forest Program (TNRSF) on these trends, a database of historical biogenic isoprene emissions from 1982 to 2010 was developed for this region using a biogenic emission model for gases and aerosols. The total amount of the biogenic isoprene emissions during the 3 decades was 4.4 Tg in northern China and 1.6 Tg in the TNRSF, with annual emissions ranging from 132 000 to 176 000 t yr−1 and from 45 000 to 70 000 t yr−1, respectively, in the two regions. Isoprene emission fluxes have increased substantially in many areas of the TNRSF over the last 3 decades due to the growing trees and vegetation coverage, especially in the central north China region where the highest emission incline reached to 58 % from 1982 to 2010. Biogenic isoprene emissions produced from anthropogenic forests tended to surpass those produced from natural forests, such as boreal forests in northeastern China. The estimated isoprene emissions suggest that the TNRSF has altered the long-term emission trend in north China from a decreasing trend during 1982 to 2010 (slope  =  −0.533, R2 = 0.05) to an increasing trend for the same period of time (slope  =  0.347, R2 = 0.014), providing strong evidence for the change in the emissions of biogenic volatile organic compounds (BVOCs) induced by the human activities on decadal or longer timescales.
Fennec dust forecast intercomparison over the Sahara in June 2011

In the framework of the Fennec international programme, a field campaign was conducted in June 2011 over the western Sahara. It led to the first observational data set ever obtained that documents the dynamics, thermodynamics and composition of the Saharan atmospheric boundary layer (SABL) under the influence of the heat low. In support to the aircraft operation, four dust forecasts were run daily at low and high resolutions with convection-parameterizing and convection-permitting models, respectively. The unique airborne and ground-based data sets allowed the first ever intercomparison of dust forecasts over the western Sahara. At monthly scale, large aerosol optical depths (AODs) were forecast over the Sahara, a feature observed by satellite retrievals but with different magnitudes. The AOD intensity was correctly predicted by the high-resolution models, while it was underestimated by the low-resolution models. This was partly because of the generation of strong near-surface wind associated with thunderstorm-related density currents that could only be reproduced by models representing convection explicitly. Such models yield emissions mainly in the afternoon that dominate the total emission over the western fringes of the Adrar des Iforas and the Aïr Mountains in the high-resolution forecasts. Over the western Sahara, where the harmattan contributes up to 80 % of dust emission, all the models were successful in forecasting the deep well-mixed SABL. Some of them, however, missed the large near-surface dust concentration generated by density currents and low-level winds. This feature, observed repeatedly by the airborne lidar, was partly forecast by one high-resolution model only.
Global atmospheric budget of simple monocyclic aromatic compounds

The global atmospheric budget and distribution of monocyclic aromatic compounds is estimated, using an atmospheric chemistry general circulation model. Simulation results are evaluated with an ensemble of surface and aircraft observations with the goal of understanding emission, production and removal of these compounds. Anthropogenic emissions provided by the RCP database represent the largest source of aromatics in the model (≃ 23 TgC year−1) and biomass burning from the GFAS inventory the second largest (≃ 5 TgC year−1). The simulated chemical production of aromatics accounts for ≃ 5 TgC year−1. The atmospheric burden of aromatics sums up to 0.3 TgC. The main removal process of aromatics is photochemical decomposition (≃ 27 TgC  year−1), while wet and dry deposition are responsible for a removal of ≃ 4 TgC year−1. Simulated mixing ratios at the surface and elsewhere in the troposphere show good spatial and temporal agreement with the observations for benzene, although the model generally underestimates mixing ratios. Toluene is generally well reproduced by the model at the surface, but mixing ratios in the free troposphere are underestimated. Finally, larger discrepancies are found for xylenes: surface mixing ratios are not only overestimated but also a low temporal correlation is found with respect to in situ observations.
Current estimates of biogenic emissions from eucalypts uncertain for southeast Australia

The biogenic emissions of isoprene and monoterpenes are one of the main drivers of atmospheric photochemistry, including oxidant and secondary organic aerosol production. In this paper, the emission rates of isoprene and monoterpenes from Australian vegetation are investigated for the first time using the Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGANv2.1); the CSIRO chemical transport model; and atmospheric observations of isoprene, monoterpenes and isoprene oxidation products (methacrolein and methyl vinyl ketone). Observations from four field campaigns during three different seasons are used, covering urban, coastal suburban and inland forest areas. The observed concentrations of isoprene and monoterpenes were of a broadly similar magnitude, which may indicate that southeast Australia holds an unusual position where neither chemical species dominates. The model results overestimate the observed atmospheric concentrations of isoprene (up to a factor of 6) and underestimate the monoterpene concentrations (up to a factor of 4). This may occur because the emission rates currently used in MEGANv2.1 for Australia are drawn mainly from young eucalypt trees (< 7 years), which may emit more isoprene than adult trees. There is no single increase/decrease factor for the emissions which suits all seasons and conditions studied. There is a need for further field measurements of in situ isoprene and monoterpene emission fluxes in Australia.
Impacts of the Manaus pollution plume on the microphysical properties of Amazonian warm-phase clouds in the wet season

The remote atmosphere over the Amazon can be similar to oceanic regions in terms of aerosol conditions and cloud type formations. This is especially true during the wet season. The main aerosol-related disturbances over the Amazon have both natural sources, such as dust transport from Africa, and anthropogenic sources, such as biomass burning or urban pollution. The present work considers the impacts of the latter on the microphysical properties of warm-phase clouds by analysing observations of the interactions between the Manaus pollution plume and its surroundings, as part of the GoAmazon2014/5 Experiment. The analysed period corresponds to the wet season (specifically from February to March 2014 and corresponding to the first Intensive Operating Period (IOP1) of GoAmazon2014/5). The droplet size distributions reported are in the range 1 µm ≤ D ≤ 50 µm in order to capture the processes leading up to the precipitation formation. The wet season largely presents a clean background atmosphere characterized by frequent rain showers. As such, the contrast between background clouds and those affected by the Manaus pollution can be observed and detailed. The focus is on the characteristics of the initial microphysical properties in cumulus clouds predominantly at their early stages. The pollution-affected clouds are found to have smaller effective diameters and higher droplet number concentrations. The differences range from 10 to 40 % for the effective diameter and are as high as 1000 % for droplet concentration for the same vertical levels. The growth rates of droplets with altitude are slower for pollution-affected clouds (2.90 compared to 5.59 µm km−1), as explained by the absence of bigger droplets at the onset of cloud development. Clouds under background conditions have higher concentrations of larger droplets (> 20 µm) near the cloud base, which would contribute significantly to the growth rates through the collision–coalescence process. The overall shape of the droplet size distribution (DSD) does not appear to be predominantly determined by updraught strength, especially beyond the 20 µm range. The aerosol conditions play a major role in that case. However, the updraughts modulate the DSD concentrations and are responsible for the vertical transport of water in the cloud. The larger droplets found in background clouds are associated with weak water vapour competition and a bimodal distribution of droplet sizes in the lower levels of the cloud, which enables an earlier initiation of the collision–coalescence process. This study shows that the pollution produced by Manaus significantly affects warm-phase microphysical properties of the surrounding clouds by changing the initial DSD formation. The corresponding effects on ice-phase processes and precipitation formation will be the focus of future endeavours.
Characterization of total ecosystem-scale biogenic VOC exchange at a Mediterranean oak–hornbeam forest

Recently, the number and amount of biogenically emitted volatile organic compounds (VOCs) has been discussed in great detail. Depending on the ecosystem, the published number varies between a dozen and several hundred compounds. We present ecosystem exchange fluxes from a mixed oak–hornbeam forest in the Po Valley, Italy. The fluxes were measured by a proton transfer reaction-time-of-flight (PTR-ToF) mass spectrometer and calculated using the eddy covariance (EC) method. Detectable fluxes were observed for up to 29 compounds, dominated by isoprene, which comprised over 60 % of the total upward flux (on a molar basis). The daily average of the total VOC upward flux was 10.4 nmol m−2 s−1. Methanol had the highest concentration and accounted for the largest downward flux. Methanol seemed to be deposited to dew, as the downward flux happened in the early morning, right after the calculated surface temperature came closest to the calculated dew point temperature. We estimated that up to 30 % of the upward flux of methyl vinyl ketone (MVK) and methacrolein (MACR) originated from atmospheric oxidation of isoprene. A comparison between two methods for the flux detection (manual and automated) was made. Their respective advantages and disadvantages were discussed and the differences in their results shown. Both provide comparable results.