Ozone climatology using interactive chemistry: results from the Canadian Middle Atmosphere Model

The climatology of ozone produced by the Canadian Middle Atmosphere Model (CMAM) is presented. This three-dimensional global model incorporates the radiative feedbacks of ozone and water vapor calculated on-line with a photochemical module. This module includes a comprehensive gas-phase reaction set and a limited set of heterogeneous reactions to account for processes occurring on background sulphate aerosols. While transport is global, photochemistry is solved from about 400 hPa to the top of the model at ∼95 km. This approach provides a complete and comprehensive representation of transport, emission, and photochemistry of various constituents from the surface to the mesopause region. A comparison of model results with observations indicates that the ozone distribution and variability are in agreement with observations throughout most of the model domain. Column ozone annual variation is represented to within 5–10% of the observations except in the Southern Hemisphere for springtime high latitudes. The vertical ozone distribution is generally well represented by the model up to the mesopause region. Nevertheless, in the upper stratosphere, the model generally underestimates the amount of ozone as well as the latitudinal tilting of ozone isopleths at high latitude. Ozone variability is analyzed and compared with measurements. The comparison shows that the phase and amplitude of the seasonal variation as well as shorter timescale variations are well represented by the model at various latitudes and heights. Finally, the impact of incorporating ozone radiative feedback on the model climatology is isolated. It is found that the incorporation of ozone radiative feedback results in a cooling of ∼8 K in the summer stratopause region, which corrects a warm bias that results when climatological ozone is used.

Historical and idealized climate model experiments: an intercomparison of Earth system models of intermediate complexity

Both historical and idealized climate model experiments are performed with a variety of Earth system models of intermediate complexity (EMICs) as part of a community contribution to the Intergovernmental Panel on Climate Change Fifth Assessment Report. Historical simulations start at 850 CE and continue through to 2005. The standard simulations include changes in forcing from solar luminosity, Earth's orbital configuration, CO2, additional greenhouse gases, land use, and sulphate and volcanic aerosols. In spite of very different modelled pre-industrial global surface air temperatures, overall 20th century trends in surface air temperature and carbon uptake are reasonably well simulated when compared to observed trends. Land carbon fluxes show much more variation between models than ocean carbon fluxes, and recent land fluxes appear to be slightly underestimated. It is possible that recent modelled climate trends or climate–carbon feedbacks are overestimated resulting in too much land carbon loss or that carbon uptake due to CO2 and/or nitrogen fertilization is underestimated. Several one thousand year long, idealized, 2 × and 4 × CO2 experiments are used to quantify standard model characteristics, including transient and equilibrium climate sensitivities, and climate–carbon feedbacks. The values from EMICs generally fall within the range given by general circulation models. Seven additional historical simulations, each including a single specified forcing, are used to assess the contributions of different climate forcings to the overall climate and carbon cycle response. The response of surface air temperature is the linear sum of the individual forcings, while the carbon cycle response shows a non-linear interaction between land-use change and CO2 forcings for some models. Finally, the preindustrial portions of the last millennium simulations are used to assess historical model carbon-climate feedbacks. Given the specified forcing, there is a tendency for the EMICs to underestimate the drop in surface air temperature and CO2 between the Medieval Climate Anomaly and the Little Ice Age estimated from palaeoclimate reconstructions. This in turn could be a result of unforced variability within the climate system, uncertainty in the reconstructions of temperature and CO2, errors in the reconstructions of forcing used to drive the models, or the incomplete representation of certain processes within the models. Given the forcing datasets used in this study, the models calculate significant land-use emissions over the pre-industrial period. This implies that land-use emissions might need to be taken into account, when making estimates of climate–carbon feedbacks from palaeoclimate reconstructions.

Impact of the modal aerosol scheme GLOMAP-mode on aerosol forcing in the Hadley Centre Global Environmental Model

The Hadley Centre Global Environmental Model (HadGEM) includes two aerosol schemes: the Coupled Large-scale Aerosol Simulator for Studies in Climate (CLASSIC), and the new Global Model of Aerosol Processes (GLOMAP-mode). GLOMAP-mode is a modal aerosol microphysics scheme that simulates not only aerosol mass but also aerosol number, represents internally-mixed particles, and includes aerosol microphysical processes such as nucleation. In this study, both schemes provide hindcast simulations of natural and anthropogenic aerosol species for the period 2000–2006. HadGEM simulations of the aerosol optical depth using GLOMAP-mode compare better than CLASSIC against a data-assimilated aerosol re-analysis and aerosol ground-based observations. Because of differences in wet deposition rates, GLOMAP-mode sulphate aerosol residence time is two days longer than CLASSIC sulphate aerosols, whereas black carbon residence time is much shorter. As a result, CLASSIC underestimates aerosol optical depths in continental regions of the Northern Hemisphere and likely overestimates absorption in remote regions. Aerosol direct and first indirect radiative forcings are computed from simulations of aerosols with emissions for the year 1850 and 2000. In 1850, GLOMAP-mode predicts lower aerosol optical depths and higher cloud droplet number concentrations than CLASSIC. Consequently, simulated clouds are much less susceptible to natural and anthropogenic aerosol changes when the microphysical scheme is used. In particular, the response of cloud condensation nuclei to an increase in dimethyl sulphide emissions becomes a factor of four smaller. The combined effect of different 1850 baselines, residence times, and abilities to affect cloud droplet number, leads to substantial differences in the aerosol forcings simulated by the two schemes. GLOMAP-mode finds a presentday direct aerosol forcing of −0.49Wm−2 on a global average, 72% stronger than the corresponding forcing from CLASSIC. This difference is compensated by changes in first indirect aerosol forcing: the forcing of −1.17Wm−2 obtained with GLOMAP-mode is 20% weaker than with CLASSIC. Results suggest that mass-based schemes such as CLASSIC lack the necessary sophistication to provide realistic input to aerosol-cloud interaction schemes. Furthermore, the importance of the 1850 baseline highlights how model skill in predicting present-day aerosol does not guarantee reliable forcing estimates. Those findings suggest that the more complex representation of aerosol processes in microphysical schemes improves the fidelity of simulated aerosol forcings.

Highly contrasting effects of different climate forcing agents on terrestrial ecosystem services

Many atmospheric constituents besides carbon dioxide (CO2) contribute to global warming, and it is common to compare their influence on climate in terms of radiative forcing, which measures their impact on the planetary energy budget. A number of recent studies have shown that many radiatively active constituents also have important impacts on the physiological functioning of ecosystems, and thus the ‘ecosystem services’ that humankind relies upon. CO2 increases have most probably increased river runoff and had generally positive impacts on plant growth where nutrients are non-limiting, whereas increases in near-surface ozone (O3) are very detrimental to plant productivity. Atmospheric aerosols increase the fraction of surface diffuse light, which is beneficial for plant growth. To illustrate these differences, we present the impact on net primary productivity and runoff of higher CO2, higher near-surface O3, and lower sulphate aerosols, and for equivalent changes in radiative forcing.We compare this with the impact of climate change alone, arising, for example, from a physiologically inactive gas such as methane (CH4). For equivalent levels of change in radiative forcing, we show that the combined climate and physiological impacts of these individual agents vary markedly and in some cases actually differ in sign. This study highlights the need to develop more informative metrics of the impact of changing atmospheric constituents that go beyond simple radiative forcing.

Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations

We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from −0.58 to −0.02Wm−2, with a mean of −0.27Wm−2 for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of −0.35Wm−2. Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study.We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results.

Zinc chelatase in human lymphocytes: detection of the enzymatic defect in erythropoietic protoporphyria

We describe a fluorometric assay for heme synthetase, the enzyme that is genetically deficient in erythropoietic protoporphyria. The method, which can readily detect activity in 1 microliter of packed human lymphocytes, is based on the formation of zinc protoheme from protoporphyrin IX. That zinc chelatase and ferrochelatase activities reside in the same enzyme was shown by the competitive action of ferrous ions and the inhibitory effects of N-methyl protoporphyrin (a specific inhibitor of heme synthetase) on zinc chelatase. The Km for zinc was 11 micrograms and that for protoporphyrin IX was 6 microM. The Ki fro ferrous ions was 14 microM. Zinc chelatase was reduced to 15.3% of the mean control activity in lymphocytes obtained from patients with protoporphyria, thus confirming the defect of heme biosynthesis in this disorder. The assay should prove to be useful for determining heme synthetase in tissues with low specific activity and to investigate further the enzymatic defect in protoporphyria.

The impacts of European and Asian anthropogenic sulphur dioxide emissions on Sahel rainfall

In this study, the atmospheric component of a state-of-the-art climate model (HadGEM2-ES) has been used to investigate the impacts of regional anthropogenic sulphur dioxide emissions on boreal summer Sahel rainfall. The study focuses on the transient response of the West African monsoon (WAM) to a sudden change in regional anthropogenic sulphur dioxide emissions, including land surface feedbacks, but without sea surface temperature (SST) feedbacks. The response occurs in two distinct phases: 1) fast adjustment of the atmosphere on a time scale of days to weeks (up to 3 weeks) through aerosol-radiation and aerosol-cloud interactions with weak hydrological cycle changes and surface feedbacks. 2) adjustment of the atmosphere and land surface with significant local hydrological cycle changes and changes in atmospheric circulation (beyond 3 weeks). European emissions lead to an increase in shortwave (SW) scattering by increased sulphate burden, leading to a decrease in surface downward SW radiation which causes surface cooling over North Africa, a weakening of the Saharan heat low and WAM, and a decrease in Sahel precipitation. In contrast, Asian emissions lead to very little change in sulphate burden over North Africa, but they induce an adjustment of the Walker Circulation which leads again to a weakening of the WAM and a decrease in Sahel precipitation. The responses to European and Asian emissions during the second phase exhibit similar large scale patterns of anomalous atmospheric circulation and hydrological variables, suggesting a preferred response. The results support the idea that sulphate aerosol emissions contributed to the observed decline in Sahel precipitation in the second half of the twentieth century.

A risk-based framework for assessing the effectiveness of stratospheric aerosol geoengineering

Geoengineering by stratospheric aerosol injection has been proposed as a policy response to warming from human emissions of greenhouse gases, but it may produce unequal regional impacts. We present a simple, intuitive risk-based framework for classifying these impacts according to whether geoengineering increases or decreases the risk of substantial climate change, with further classification by the level of existing risk from climate change from increasing carbon dioxide concentrations. This framework is applied to two climate model simulations of geoengineering counterbalancing the surface warming produced by a quadrupling of carbon dioxide concentrations, with one using a layer of sulphate aerosol in the lower stratosphere, and the other a reduction in total solar irradiance. The solar dimming model simulation shows less regional inequality of impacts compared with the aerosol geoengineering simulation. In the solar dimming simulation, 10% of the Earth’s surface area, containing 10% of its population and 11% of its gross domestic product, experiences greater risk of substantial precipitation changes under geoengineering than under enhanced carbon dioxide concentrations. In the aerosol geoengineering simulation the increased risk of substantial precipitation change is experienced by 42% of Earth’s surface area, containing 36% of its population and 60% of its gross domestic product.

A study on the sensitivities of simulated aerosol optical properties to composition and size distribution using airborne measurements

We present a flexible framework to calculate the optical properties of atmospheric aerosols at a given relative humidity based on their composition and size distribution. The similarity of this framework to climate model parameterisations allows rapid and extensive sensitivity tests of the impact of uncertainties in data or of new measurements on climate relevant aerosol properties. The data collected by the FAAM BAe-146 aircraft during the EUCAARI-LONGREX and VOCALS-REx campaigns have been used in a closure study to analyse the agreement between calculated and measured aerosol optical properties for two very different aerosol types. The agreement achieved for the EUCAARI-LONGREX flights is within the measurement uncertainties for both scattering and absorption. However, there is poor agreement between the calculated and the measured scattering for the VOCALS-REx flights. The high concentration of sulphate, which is a scattering aerosol with no absorption in the visible spectrum, made the absorption measurements during VOCALS-REx unreliable, and thus no closure study was possible for the absorption. The calculated hygroscopic scattering growth factor overestimates the measured values during EUCAARI-LONGREX and VOCALS-REx by ∼30% and ∼20%, respectively. We have also tested the sensitivity of the calculated aerosol optical properties to the uncertainties in the refractive indices, the hygroscopic growth factors and the aerosol size distribution. The largest source of uncertainty in the calculated scattering is the aerosol size distribution (∼35%), followed by the assumed hygroscopic growth factor for organic aerosol (∼15%), while the predominant source of uncertainty in the calculated absorption is the refractive index of organic aerosol (28–60%), although we would expect the refractive index of black carbon to be important for aerosol with a higher black carbon fraction.

Aerosol scattering and absorption during the EUCAARI-LONGREX flights of the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146: can measurements and models agree?

Scattering and absorption by aerosol in anthropogenically perturbed air masses over Europe has been measured using instrumentation flown on the UK’s BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM) on 14 flights during the EUCAARI-LONGREX campaign in May 2008. The geographical and temporal variations of the derived shortwave optical properties of aerosol are presented. Values of single scattering albedo of dry aerosol at 550 nm varied considerably from 0.86 to near unity, with a campaign average of 0.93 ± 0.03. Dry aerosol optical depths ranged from 0.030 ± 0.009 to 0.24 ± 0.07. An optical properties closure study comparing calculations from composition data and Mie scattering code with the measured properties is presented. Agreement to within measurement uncertainties of 30% can be achieved for both scattering and absorption,but the latter is shown to be sensitive to the refractive indices chosen for organic aerosols, and to a lesser extent black carbon, as well as being highly dependent on the accuracy of the absorption measurements. Agreement with the measured absorption can be achieved either if organic carbon is assumed to be weakly absorbing, or if the organic aerosol is purely scattering and the absorption measurement is an overestimate due to the presence of large amounts of organic carbon. Refractive indices could not be inferred conclusively due to this uncertainty, despite the enhancement in methodology compared to previous studies that derived from the use of the black carbon measurements. Hygroscopic growth curves derived from the wet nephelometer indicate moderate water uptake by the aerosol with a campaign mean f (RH) value (ratio in scattering) of 1.5 (range from 1.23 to 1.63) at 80% relative humidity. This value is qualitatively consistent with the major chemical components of the aerosol measured by the aerosol mass spectrometer, which are primarily mixed organics and nitrate and some sulphate.

Atmospheric chemistry and physics in the atmosphere of a developed megacity (London): an overview of the REPARTEE experiment and its conclusions

The REgents PARk and Tower Environmental Experiment (REPARTEE) comprised two campaigns in London in October 2006 and October/November 2007. The experiment design involved measurements at a heavily trafficked roadside site, two urban background sites and an elevated site at 160–190 m above ground on the BT Tower, supplemented in the second campaign by Doppler lidar measurements of atmospheric vertical structure. A wide range of measurements of airborne particle physical metrics and chemical composition were made as well as measurements of a considerable range of gas phase species and the fluxes of both particulate and gas phase substances. Significant findings include (a) demonstration of the evaporation of traffic-generated nanoparticles during both horizontal and vertical atmospheric transport; (b) generation of a large base of information on the fluxes of nanoparticles, accumulation mode particles and specific chemical components of the aerosol and a range of gas phase species, as well as the elucidation of key processes and comparison with emissions inventories; (c) quantification of vertical gradients in selected aerosol and trace gas species which has demonstrated the important role of regional transport in influencing concentrations of sulphate, nitrate and secondary organic compounds within the atmosphere of London; (d) generation of new data on the atmospheric structure and turbulence above London, including the estimation of mixed layer depths; (e) provision of new data on trace gas dispersion in the urban atmosphere through the release of purposeful tracers; (f) the determination of spatial differences in aerosol particle size distributions and their interpretation in terms of sources and physico-chemical transformations; (g) studies of the nocturnal oxidation of nitrogen oxides and of the diurnal behaviour of nitrate aerosol in the urban atmosphere, and (h) new information on the chemical composition and source apportionment of particulate matter size fractions in the atmosphere of London derived both from bulk chemical analysis and aerosol mass spectrometry with two instrument types.

Dietary iron depletion at weaning imprints low microbiome diversity and this is not recovered with oral nano Fe(III)

Alterations in the gut microbiota have been recently linked to oral iron. We conducted two feeding studies including an initial diet-induced iron-depletion period followed by supplementation with nanoparticulate tartrate-modified ferrihydrite (Nano Fe(III): considered bioavailable to host but not bacteria) or soluble ferrous sulfate (FeSO4: considered bioavailable to both host and bacteria). We applied denaturing gradient gel electrophoresis and fluorescence in situ hybridization for study-1 and 454-pyrosequencing of fecal 16S rRNA in study-2. In study-1, the within-community microbial diversity increased with FeSO4 (P = 0.0009) but not with Nano Fe(III) supplementation. This was confirmed in study-2, where we also showed that iron depletion at weaning imprinted significantly lower within- and between-community microbial diversity compared to mice weaned onto the iron-sufficient reference diet (P < 0.0001). Subsequent supplementation with FeSO4 partially restored the within-community diversity (P = 0.006 in relation to the continuously iron-depleted group) but not the between-community diversity, whereas Nano Fe(III) had no effect. We conclude that (1) dietary iron depletion at weaning imprints low diversity in the microbiota that is not, subsequently, easily recovered; (2) in the absence of gastrointestinal disease iron supplementation does not negatively impact the microbiota; and (3) Nano Fe(III) is less available to the gut microbiota.

Comparison of bioactivities, binding properties and intra-follicular levels of bovine follistatins

Five isoforms of follistatin (FST) (Mr 31, 33, 35, 37, 41kDa) were purified from bovine follicular fluid (bFF). Comparison of their activin- and heparan sulphate proteoglycan (HSP)-binding properties and bio-potencies in neutralization of activin-A action in vitro revealed that all five isoforms bound activin-A, but with different affinities. Only the 31kDa isoform (FST-288) bound to HSP. FST-288 also showed the greatest biopotency with 35 and 41kDa isoforms being least potent. To determine whether bovine follicle development is associated with changing intrafollicular FST and activin profiles, we analyzed bFF from dominant (DF) and subordinate (SF) follicles collected at strategic times during a synchronized estrous cycle. Total FST, activin-A and activin-AB were measured by immunoassay while individual FST isoforms were quantified by immunoblotting. Follicle diameter was positively correlated with estrogen:progesterone ratio (r=0.56) in bFF but negatively correlated with activin-A (r=-0.34), activin-AB (r=-0.80) and ‘total’ FST (r=-0.70) levels. Follicle diameter was positively correlated with abundance of the 41 kDa isoform (r=0.59) but negatively correlated with abundance of 33 and 31 kDa isoforms (r=-0.56, -0.41). Both follicle status (DF vs SF) and cycle stage affected total FST, activin-A, activin-B levels while follicle status, but not cycle stage, affected abundance of 41, 37, 33 and 31kDa FST isoforms. Collectively, these findings indicate that intrafollicular FST isoforms that differ in their ability to bind and neutralise activins and associate with cell-surface proteoglycans, show divergent changes during follicle development. Enhanced FST production may have an important negative role, either directly or via inhibition of the positive effects of activins, on follicle growth and function during follicular waves.

Preferred response of the East Asian summer monsoon to local and non-local anthropogenic sulphur dioxide emissions

In this study, the atmospheric component of a state-of-the-art climate model (HadGEM2-ES) that includes earth system components such as interactive chemistry and eight species of tropospheric aerosols considering aerosol direct, indirect, and semi-direct effects, has been used to investigate the impacts of local and non-local emissions of anthropogenic sulphur dioxide on the East Asian summer monsoon (EASM). The study focuses on the fast responses (including land surface feedbacks, but without sea surface temperature feedbacks) to sudden changes in emissions from Asia and Europe. The initial responses, over days 1–40, to Asian and European emissions show large differences. The response to Asian emissions involves a direct impact on the sulphate burden over Asia, with immediate consequences for the shortwave energy budget through aerosol–radiation and aerosol–cloud interactions. These changes lead to cooling of East Asia and a weakening of the EASM. In contrast, European emissions have no significant impact on the sulphate burden over Asia, but they induce mid-tropospheric cooling and drying over the European sector. Subsequently, however, this cold and dry anomaly is advected into Asia, where it induces atmospheric and surface feedbacks over Asia and the Western North Pacific (WNP), which also weaken the EASM. In spite of very different perturbations to the local aerosol burden in response to Asian and European sulphur dioxide emissions, the large scale pattern of changes in land–sea thermal contrast, atmospheric circulation and local precipitation over East Asia from days 40 onward exhibits similar structures, indicating a preferred response, and suggesting that emissions from both regions likely contributed to the observed weakening of the EASM. Cooling and drying of the troposphere over Asia, together with warming and moistening over the WNP, reduces the land–sea thermal contrast between the Asian continent and surrounding oceans. This leads to high sea level pressure (SLP) anomalies over Asia and low SLP anomalies over the WNP, associated with a weakened EASM. In response to emissions from both regions warming and moistening over the WNP plays an important role and determines the time scale of the response.

Airborne measurements of trace gases and aerosols over the London metropolitan region

The Emissions around the M25 motorway (EM25) campaign took place over the megacity of London in the United Kingdom in June 2009 with the aim of characterising trace gas and aerosol composition and properties entering and emitted from the urban region. It featured two mobile platforms, the UK BAe-146 Facility for Airborne Atmospheric Measurements (FAAM) research aircraft and a ground-based mobile lidar van, both travelling in circuits around London, roughly following the path of the M25 motorway circling the city. We present an overview of findings from the project, which took place during typical UK summertime pollution conditions. Emission ratios of volatile organic compounds (VOCs) to acetylene and carbon monoxide emitted from the London region were consistent with measurements in and downwind of other large urban areas and indicated traffic and associated fuel evaporation were major sources. Sub-micron aerosol composition was dominated by secondary species including sulphate (24% of sub-micron mass in the London plume and 29% in the non-plume regional aerosol), nitrate (24% plume; 20% regional) and organic aerosol (29% plume; 31% regional). The primary sub-micron aerosol emissions from London were minor compared to the larger regional background, with only limited increases in aerosol mass in the urban plume compared to the background (~12% mass increase on average). Black carbon mass was the major exception and more than doubled in the urban plume, leading to a decrease in the single scattering albedo from 0.91 in the regional aerosol to 0.86 in the London plume, on average. Our observations indicated that regional aerosol plays a major role on aerosol concentrations around London, at least during typical summertime conditions, meaning future efforts to reduce PM levels in London must account for regional as well as local aerosol sources.