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We quantify the impact of land-use change, determined by our growing demand for food and biofuel production, on isoprene emissions and subsequent atmospheric oxidant chemistry in 2015 and 2030, relative to 1990, ignoring compound climate change effects over that period. We estimate isoprene emissions from an ensemble (<i>n</i> = 1000) of land-use change realizations from 1990–2050, broadly guided by the IPCC AR4/SRES scenarios A1 and B1. We also superimpose land-use change required to address projected biofuel usage using two scenarios: (1) assuming that world governments make no changes to biofuel policy after 2009, and (2) assuming that world governments develop biofuel policy with the aim of keeping equivalent atmospheric CO<sub>2</sub> at 450 ppm. We present the median and interquartile range (IQR) statistics of the ensemble and show that land-use change between −1.50 × 10<sup>12</sup> m<sup>2</sup> to +6.06 × 10<sup>12</sup> m<sup>2</sup> was found to drive changes in the global isoprene burden of −3.5 to +2.8 Tg yr<sup>−1</sup> in 2015 and −7.7 to +6.4 Tg yr<sup>−1</sup> in 2030. We use land-use change realizations corresponding to the median and IQR of these emission estimates to drive the GEOS-Chem global 3-D chemistry transport model to investigate the perturbation to global and regional surface concentrations of isoprene, nitrogen oxides (NO+NO<sub>2</sub>), and the atmospheric concentration and deposition of ozone (O<sub>3</sub>). We show that across subcontinental regions the monthly surface O<sub>3</sub> increases by 0.1–0.8 ppb, relative to a zero land-use change calculation, driven by increases (decreases) in surface isoprene in high (low) NO<sub>x</sub> environments. At the local scale (4° × 5°) we find that surface O<sub>3</sub> increases by 5–12 ppb over temperate North America, China and boreal Eurasia, driven by large increases in isoprene emissions from short-rotation coppice crop cultivation for biofuel production.
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This study reports on the exploitation of GNSS (Global Navigation Satellite System) and a new potential application for weather forecasts and nowcasting. We focus on GPS observations (post-processing with a time resolution of 5 and 15 min and fast calculations with a time resolution of 5 min) and try to establish typical configurations of the water vapour field which characterise convective systems and particularly which supply precursors of their initiation are associated with deep convection. We show the critical role of GNSS horizontal gradients of the water vapour content to detect small scale structures of the troposphere (i. e. convective cells), and then we present our strategy to obtain typical water vapour configurations by GNSS called "H<sub>2</sub>O alert". These alerts are based on a dry/wet contrast taking place during a 30 min time window before the initiation of a convective system. GNSS observations have been assessed for the rainfall event of 28–29 June 2005 using data from the Belgian dense network (baseline from 5 to 30 km). To validate our GNSS H<sub>2</sub>O alerts, we use the detection of precipitation by C-band weather radar and thermal infrared radiance (cloud top temperature) of the 10.8-micrometers channel [Ch09] of SEVIRI instrument on Meteosat Second Generation. Using post-processed measurements, our H<sub>2</sub>O alerts obtain a score of about 80%. Final and ultra-rapid IGS (International GNSS Service) orbits have been tested and show equivalent results. Fast calculations (less than 10 min) have been processed for 29 June 2005 with a time resolution of 5 min. The mean bias (and standard deviation) between fast and reference post-processed ZTD (zenith total delay) and gradients are, respectively, 0.002 (± 0.008) m and 0.001 (± 0.004) m. The score obtained for the H<sub>2</sub>O alerts generated by fast calculations is 65%.
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Model-simulated transport of atmospheric trace components can be combined with observed concentrations to obtain estimates of ground-based sources using various inversion techniques. These approaches have been applied in the past primarily to obtain source estimates for long-lived trace gases such as CO<sub>2</sub>. We consider the application of similar techniques to source estimation for atmospheric aerosols, using as a case study the estimation of bacteria emissions from different ecosystem regions in the global atmospheric chemistry and climate model ECHAM5/MESSy-Atmospheric Chemistry (EMAC). <br><br> Source estimation via Markov Chain Monte Carlo is applied to a suite of sensitivity simulations, and the global mean emissions are estimated for the example problem of bacteria-containing aerosol particles. We present an analysis of the uncertainties in the global mean emissions, and a partitioning of the uncertainties that are attributable to particle size, activity as cloud condensation nuclei (CCN), the ice nucleation scavenging ratios for mixed-phase and cold clouds, and measurement error. <br><br> For this example, uncertainty due to CCN activity or to a 1 μm error in particle size is typically between 10% and 40% of the uncertainty due to observation uncertainty, as measured by the 5–95th percentile range of the Monte Carlo ensemble. Uncertainty attributable to the ice nucleation scavenging ratio in mixed-phase clouds is as high as 10–20% of that attributable to observation uncertainty. Taken together, the four model parameters examined contribute about half as much to the uncertainty in the estimated emissions as do the observations. This was a surprisingly large contribution from model uncertainty in light of the substantial observation uncertainty, which ranges from 81–870% of the mean for each of ten ecosystems for this case study. The effects of these and other model parameters in contributing to the uncertainties in the transport of atmospheric aerosol particles should be treated explicitly and systematically in both forward and inverse modelling studies.
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Mineral dust aerosols exert a significant effect on both solar and terrestrial radiation. By absorbing and scattering, the solar radiation aerosols reduce the amount of energy reaching the surface. In addition, aerosols enhance the greenhouse effect by absorbing and emitting outgoing longwave radiation. Desert dust forcing exhibits large regional and temporal variability due to its short lifetime and diverse optical properties, further complicating the quantification of the direct radiative effect (DRE). The complexity of the links and feedbacks of dust on radiative transfer indicate the need for an integrated approach in order to examine these impacts. <br><br> In order to examine these feedbacks, the SKIRON limited area model has been upgraded to include the RRTMG (Rapid Radiative Transfer Model – GCM) radiative transfer model that takes into consideration the aerosol radiative effects. It was run for a 6 year period. Two sets of simulations were performed, one without the effects of dust and the other including the radiative feedback. The results were first evaluated using aerosol optical depth data to examine the capabilities of the system in describing the desert dust cycle. Then the aerosol feedback on radiative transfer was quantified and the links between dust and radiation were studied. The study has revealed a strong interaction between dust particles and solar and terrestrial radiation, with several implications on the energy budget of the atmosphere. A profound effect is the increased absorption (in the shortwave and longwave) in the lower troposphere and the induced modification of the atmospheric temperature profile. These feedbacks depend strongly on the spatial distribution of dust and have more profound effects where the number of particles is greater, such as near their source.
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Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD (Cosmics Leaving Outdoor Droplets) chamber experiments at CERN (Centre européen pour la recherche nucléaire). The investigation was carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovskii–Stokes–Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ~0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
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Peroxyacetyl nitrate (CH<sub>3</sub>CO·O<sub>2</sub>NO<sub>2</sub>, abbreviated as PAN) is a trace molecular species present in the troposphere and lower stratosphere due primarily to pollution from fuel combustion and the pyrogenic outflows from biomass burning. In the lower troposphere, PAN has a relatively short lifetime and is principally destroyed within a few hours through thermolysis, but it can act as a reservoir and carrier of NO<sub>x</sub> in the colder temperatures of the upper troposphere, where UV photolysis becomes the dominant loss mechanism. Pyroconvective updrafts from large biomass burning events can inject PAN into the upper troposphere and lower stratosphere (UTLS), providing a means for the long-range transport of NO<sub>x</sub>. Given the extended lifetimes at these higher altitudes, PAN is readily detectable via satellite remote sensing. <br><br> A new PAN data product is now available for the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) version 3.0 data set. We report observations of PAN in boreal biomass burning plumes recorded during the BORTAS (quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) campaign (12 July to 3 August 2011). The retrieval method employed by incorporating laboratory-recorded absorption cross sections into version 3.0 of the ACE-FTS forward model and retrieval software is described in full detail. The estimated detection limit for ACE-FTS PAN is 5 pptv, and the total systematic error contribution to the ACE-FTS PAN retrieval is ~ 16%. <br><br> The retrieved volume mixing ratio (VMR) profiles are compared to coincident measurements made by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on the European Space Agency (ESA) Environmental Satellite (ENVISAT). The MIPAS measurements demonstrated good agreement with the ACE-FTS VMR profiles for PAN, where the measured VMR values are well within the associated measurement errors for both instruments and comparative measurements differ no more than 70 pptv. <br><br> The ACE-FTS PAN data set is used to obtain zonal mean distributions of seasonal averages from ~ 5–20 km. A strong seasonality is clearly observed for PAN concentrations in the global UTLS. Since the principal source of PAN in the UTLS is due to lofted biomass burning emissions from the pyroconvective updrafts created by large fires, the observed seasonality in enhanced PAN coincides with fire activity in different geographical regions throughout the year.
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The atmospheric records of four halons, H-1211 (CBrClF<sub>2</sub>), H-1301 (CBrF<sub>3</sub>), H-2402 (CBrF<sub>2</sub>CBrF<sub>2</sub>) and H-1202 (CBr<sub>2</sub>F<sub>2</sub>), measured from air collected at Cape Grim, Tasmania, between 1978 and 2011, are reported. Mixing ratios of H-1211, H-2402 and H-1202 began to decline in the early to mid-2000s, but those of H-1301 continue to increase up to mid-2011. These trends are compared to those reported by NOAA (National Oceanic and Atmospheric Administration) and AGAGE (Advanced Global Atmospheric Experiment). The observations suggest that the contribution of the halons to total tropospheric bromine at Cape Grim has begun to decline from a peak in 2008 of about 8.1 ppt. An extrapolation of halon mixing ratios to 2060, based on reported banks and predicted release factors, shows this decline becoming more rapid in the coming decades, with a contribution to total tropospheric bromine of about 3 ppt in 2060. Top-down global annual emissions of the halons were derived using a two-dimensional atmospheric model. The emissions of all four have decreased since peaking in the late 1980s–mid-1990s, but this decline has slowed recently, particularly for H-1301 and H-2402 which have shown no decrease in emissions over the past five years. The UEA (University of East Anglia) top-down model-derived emissions are compared to those reported using a top-down approach by NOAA and AGAGE and the bottom-up estimates of HTOC (Halons Technical Options Committee). The implications of an alternative set of steady-state atmospheric lifetimes are discussed. Using a lifetime of 14 yr or less for H-1211 to calculate top-down emissions estimates would lead to small, or even negative, estimated banks given reported production data. Finally emissions of H-1202, a product of over-bromination during the production process of H-1211, have continued despite reported production of H-1211 ceasing in 2010. This raises questions as to the source of these H-1202 emissions.
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Recent studies have shown very high frequencies of atmospheric new particle formation in different environments in South Africa. Our aim here was to investigate the causes for two or three consecutive daytime nucleation events, followed by subsequent particle growth during the same day. We analysed 108 and 31 such days observed in a polluted industrial and moderately polluted rural environments, respectively, in South Africa. The analysis was based on two years of measurements at each site. After rejecting the days having notable changes in the air mass origin or local wind direction, i.e. two major reasons for observed multiple nucleation events, we were able to investigate other factors causing this phenomenon. Clouds were present during, or in between most of the analysed multiple particle formation events. Therefore, some of these events may have been single events, interrupted somehow by the presence of clouds. From further analysis, we propose that the first nucleation and growth event of the day was often associated with the mixing of a residual air layer rich in SO<sub>2</sub> (oxidized to sulphuric acid) into the shallow surface-coupled layer. The second nucleation and growth event of the day usually started before midday and was sometimes associated with renewed SO<sub>2</sub> emissions from industrial origin. However, it was also evident that vapours other than sulphuric acid were required for the particle growth during both events. This was especially the case when two simultaneously growing particle modes were observed. Based on our analysis, we conclude that the relative contributions of estimated H<sub>2</sub>SO<sub>4</sub> and other vapours on the first and second nucleation and growth events of the day varied from day to day, depending on anthropogenic and natural emissions, as well as atmospheric conditions.
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Atmospheric water vapour tracers (WVTs) are an elegant tool to determine source–sink relations of moisture "online" in atmospheric general circulation models (AGCMs). However, it is sometimes desirable to establish such relations "offline" based on already existing atmospheric data (e.g. reanalysis data). One simple and frequently applied offline method is 2-D moisture tracing. It makes use of the "well-mixed" assumption, which allows for treating the vertical dimension integratively. Here we scrutinise the "well-mixed" assumption and 2-D moisture tracing by means of analytical considerations in combination with AGCM-WVT simulations. <br><br> We find that vertically well-mixed conditions are seldom met. Due to the presence of vertical inhomogeneities, 2-D moisture tracing (i) neglects a significant degree of fast-recycling, and (ii) results in erroneous advection where the direction of the horizontal winds varies vertically. The latter is not so much the case in the extratropics, but in the tropics this can lead to large errors. For example, computed by 2-D moisture tracing, the fraction of precipitation in the western Sahel that originates from beyond the Sahara is ~40%, whereas the fraction that originates from the tropical and Southern Atlantic is only ~4%. According to full (i.e. 3-D) moisture tracing, however, both regions contribute roughly equally, showing that the errors introduced by the 2-D approximation can be substantial.
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Climate models that do not simulate changes in stratospheric ozone concentrations require the prescription of ozone fields to accurately calculate UV fluxes and stratospheric heating rates. In this study, three different global ozone time series that are available for this purpose are compared: the data set of Randel and Wu (2007) (RW07), Cionni et al. (2011) (SPARC), and Bodeker et al. (2013) (BDBP). All three data sets represent multiple-linear regression fits to vertically resolved ozone observations, resulting in a spatially and temporally continuous stratospheric ozone field covering at least the period from 1979 to 2005. The main differences among the data sets result from regression models, which use different observations and include different basis functions. The data sets are compared against ozonesonde and satellite observations to assess how the data sets represent concentrations, trends and interannual variability. In the Southern Hemisphere polar region, RW07 and SPARC underestimate the ozone depletion in spring ozonesonde measurements. A piecewise linear trend regression is performed to estimate the 1979–1996 ozone decrease globally, covering a period of extreme depletion in most regions. BDBP overestimates Arctic and tropical ozone depletion over this period relative to the available measurements, whereas the depletion is underestimated in RW07 and SPARC. While the three data sets yield ozone concentrations that are within a range of different observations, there is a large spread in their respective ozone trends. One consequence of this is differences of almost a factor of four in the calculated stratospheric ozone radiative forcing between the data sets (RW07: −0.038 Wm<sup>−2</sup>, SPARC: −0.033 Wm<sup>−2</sup>, BDBP: −0.119 Wm<sup>−2</sup>), important in assessing the contribution of stratospheric ozone depletion to the total anthropogenic radiative forcing.
