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Biomass burning is one of the largest sources of atmospheric trace gases and aerosols globally. These emissions have a major impact on the radiative balance of the atmosphere and on air quality, and are thus of significant scientific and societal interest. Several datasets have been developed that quantify those emissions on a global grid and offered to the atmospheric modelling community. However, no study has yet attempted to systematically quantify the dependence of the inferred pyrogenic emissions on underlying assumptions and input data. Such a sensitivity study is needed for understanding how well we can currently model those emissions and what the factors are that contribute to uncertainties in those emission estimates. <br><br> Here, we combine various satellite-derived burned area products, a terrestrial ecosystem model to simulate fuel loads and the effect of fire on ecosystem dynamics, a model of fuel combustion, and various emission models that relate combusted biomass to the emission of various trace gases and aerosols. We carry out simulations with varying parameters for combustion completeness and fuel decomposition rates within published estimates, four different emissions models and three different global burned-area products. We find that variations in combustion completeness and simulated fuel loads have the largest impact on simulated global emissions for most species, except for some with highly uncertain emission factors. Variation in burned-area estimates also contribute considerably to emission uncertainties. We conclude that global models urgently need more field-based data for better parameterisation of combustion completeness and validation of simulated fuel loads, and that further validation and improvement of burned area information is necessary for accurately modelling global wildfire emissions. The results are important for chemical transport modelling studies, and for simulations of biomass burning impacts on the atmosphere under future climate change scenarios.
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The in situ boundary layer measurement site in Białystok (Poland) has been upgraded with a fully automated observatory for total greenhouse gas column measurements. The automated Fourier Transform Spectrometer (FTS) complements the on-site in situ facilities and FTS solar absorption measurements have been recorded nearly continuously in clear and partially cloudy conditions since March 2009. Here, the FTS measurements are compared with the collocated tall tower data. Additionally, simulations of the Jena CO<sub>2</sub> inversion model are evaluated with the Białystok measurement facilities. The simulated seasonal CO<sub>2</sub> cycle is slightly overestimated by a mean difference of 1.2 ppm ± 0.9 ppm (1σ) in comparison with the FTS measurements. CO<sub>2</sub> concentrations at the surface, measured at the tall tower (5 m, 90 m, 300 m), are slightly underestimated by −1.5 ppm, −1.6 ppm, and −0.7 ppm respectively during the day and by −9.1 ppm, −5.9 ppm, and −1.3 ppm during the night. The comparison of the simulated CO<sub>2</sub> profiles with low aircraft profiles shows a slight overestimation of the lower troposphere (by up to 1 ppm) and an underestimation in near-surface heights until 800 m (by up to 2.5 ppm). In an appendix the automated FTS observatory, including the hardware components and the automation software, is described in its basics.
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We study the combined effects of land surface conditions, atmospheric boundary layer dynamics and chemistry on the diurnal evolution of biogenic secondary organic aerosol in the atmospheric boundary layer, using a model that contains the essentials of all these components. First, we evaluate the model for a case study in Hyytiälä, Finland, and find that it is able to satisfactorily reproduce the observed dynamics and gas-phase chemistry. We show that the exchange of organic aerosol between the free troposphere and the boundary layer (entrainment) must be taken into account in order to explain the observed diurnal cycle in organic aerosol (OA) concentration. An examination of the budgets of organic aerosol and terpene concentrations show that the former is dominated by entrainment, while the latter is mainly driven by emission and chemical transformation. We systematically investigate the role of the land surface, which governs both the surface energy balance partitioning and terpene emissions, and the large-scale atmospheric process of vertical subsidence. Entrainment is especially important for the dilution of organic aerosol concentrations under conditions of dry soils and low terpene emissions. Subsidence suppresses boundary layer growth while enhancing entrainment. Therefore, it influences the relationship between organic aerosol and terpene concentrations. Our findings indicate that the diurnal evolution of secondary organic aerosols (SOA) in the boundary layer is the result of coupled effects of the land surface, dynamics of the atmospheric boundary layer, chemistry, and free troposphere conditions. This has potentially some consequences for the design of both field campaigns and large-scale modeling studies.
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The atmospheric chemistry general circulation model EMAC has been used to estimate the impact of anthropogenic emission changes on global and regional air quality in recent and future years (2005, 2010, 2025 and 2050). The emission scenario assumes that population and economic growth largely determine energy and food consumption and consequent pollution sources with the current technologies ("business as usual"). This scenario is chosen to show the effects of not implementing legislation to prevent additional climate change and growing air pollution, other than what is in place for the base year 2005, representing a pessimistic (but plausible) future. <br><br> By comparing with recent observations, it is shown that the model reproduces the main features of regional air pollution distributions though with some imprecisions inherent to the coarse horizontal resolution (~100 km) and simplified bottom-up emission input. <br><br> To identify possible future hot spots of poor air quality, a multi pollutant index (MPI), suited for global model output, has been applied. It appears that East and South Asia and the Middle East represent such hotspots due to very high pollutant concentrations, while a general increase of MPIs is observed in all populated regions in the Northern Hemisphere. In East Asia a range of pollutant gases and fine particulate matter (PM<sub>2.5</sub>) is projected to reach very high levels from 2005 onward, while in South Asia air pollution, including ozone, will grow rapidly towards the middle of the century. Around the Persian Gulf, where natural PM<sub>2.5</sub> concentrations are already high (desert dust), ozone levels are expected to increase strongly. <br><br> The population weighted MPI (PW-MPI), which combines demographic and pollutant concentration projections, shows that a rapidly increasing number of people worldwide will experience reduced air quality during the first half of the 21st century. Following this business as usual scenario, it is projected that air quality for the global average citizen in 2050 would be almost comparable to that for the average citizen in East Asia in the year 2005, which underscores the need to pursue emission reductions.
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Measurements of ozone vertical profiles are valuable for the evaluation of atmospheric chemistry models and contribute to the understanding of the processes controlling the distribution of tropospheric ozone. The longest record of ozone vertical profiles is provided by ozone sondes, which have a typical frequency of 4 to 12 profiles a month. Here we quantify the uncertainty introduced by low frequency sampling in the determination of means and trends. To do this, the high frequency MOZAIC (Measurements of OZone, water vapor, carbon monoxide and nitrogen oxides by in-service AIrbus airCraft) profiles over airports, such as Frankfurt, have been subsampled at two typical ozone sonde frequencies of 4 and 12 profiles per month. We found the lowest sampling uncertainty on seasonal means at 700 hPa over Frankfurt, with around 5% for a frequency of 12 profiles per month and 10% for a 4 profile-a-month frequency. However the uncertainty can reach up to 15 and 29% at the lowest altitude levels. As a consequence, the sampling uncertainty at the lowest frequency could be higher than the typical 10% accuracy of the ozone sondes and should be carefully considered for observation comparison and model evaluation. We found that the 95% confidence limit on the seasonal mean derived from the subsample created is similar to the sampling uncertainty and suggest to use it as an estimate of the sampling uncertainty. Similar results are found at six other Northern Hemisphere sites. We show that the sampling substantially impacts on the inter-annual variability and the trend derived over the period 1998–2008 both in magnitude and in sign throughout the troposphere. Also, a tropical case is discussed using the MOZAIC profiles taken over Windhoek, Namibia between 2005 and 2008. For this site, we found that the sampling uncertainty in the free troposphere is around 8 and 12% at 12 and 4 profiles a month respectively.
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A new size-resolved dust scheme based on the numerical method of piecewise log-normal approximation (PLA) was developed and implemented in the fourth generation of the Canadian Atmospheric Global Climate Model with the PLA Aerosol Model (CanAM4-PAM). The total simulated annual global dust emission is 2500 Tg yr<sup>−1</sup>, and the dust mass load is 19.3 Tg for year 2000. Both are consistent with estimates from other models. Results from simulations are compared with multiple surface measurements near and away from dust source regions, validating the generation, transport and deposition of dust in the model. Most discrepancies between model results and surface measurements are due to unresolved aerosol processes. Biases in long-range transport are also contributing. Radiative properties of dust aerosol are derived from approximated parameters in two size modes using Mie theory. The simulated aerosol optical depth (AOD) is compared with satellite and surface remote sensing measurements and shows general agreement in terms of the dust distribution around sources. The model yields a dust AOD of 0.042 and dust aerosol direct radiative forcing (ADRF) of −1.24 W m<sup>−2</sup> respectively, which show good consistency with model estimates from other studies.
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The seasonal cycle in Arctic aerosol is typified by high concentrations of large aged anthropogenic particles transported from lower latitudes in the late Arctic winter and early spring followed by a sharp transition to low concentrations of locally sourced smaller particles in the summer. However, multi-model assessments show that many models fail to simulate a realistic cycle. Here, we use a global aerosol microphysics model (GLOMAP) and surface-level aerosol observations to understand how wet scavenging processes control the seasonal variation in Arctic black carbon (BC) and sulphate aerosol. We show that the transition from high wintertime concentrations to low concentrations in the summer is controlled by the transition from ice-phase cloud scavenging to the much more efficient warm cloud scavenging in the late spring troposphere. This seasonal cycle is amplified further by the appearance of warm drizzling cloud in the late spring and summer boundary layer. Implementing these processes in GLOMAP greatly improves the agreement between the model and observations at the three Arctic ground-stations Alert, Barrow and Zeppelin Mountain on Svalbard. The SO<sub>4</sub> model-observation correlation coefficient (<i>R</i>) increases from: −0.33 to 0.71 at Alert (82.5° N), from −0.16 to 0.70 at Point Barrow (71.0° N) and from −0.42 to 0.40 at Zeppelin Mountain (78° N). The BC model-observation correlation coefficient increases from −0.68 to 0.72 at Alert and from −0.42 to 0.44 at Barrow. Observations at three marginal Arctic sites (Janiskoski, Oulanka and Karasjok) indicate a far weaker aerosol seasonal cycle, which we show is consistent with the much smaller seasonal change in the frequency of ice clouds compared to higher latitude sites. Our results suggest that the seasonal cycle in Arctic aerosol is driven by temperature-dependent scavenging processes that may be susceptible to modification in a future climate.
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We present a new model for the global tropospheric chemistry of inorganic bromine (Br<sub>y</sub>) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Br<sub>y</sub> include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by <1–8 nmol mol<sup>−1</sup> (6.5% globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4%. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40% higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.
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For the first time, carbon monoxide (CO) and formaldehyde (HCHO) satellite retrievals are used together with methane (CH<sub>4</sub>) and methyl choloroform (CH<sub>3</sub>CCl<sub>3</sub> or MCF) surface measurements in an advanced inversion system. The CO and HCHO are respectively from the MOPITT and OMI instruments. The multi-species and multi-satellite dataset inversion is done for the 2005–2010 period. The robustness of our results is evaluated by comparing our posterior-modeled concentrations with several sets of independent measurements of atmospheric mixing ratios. The inversion leads to significant changes from the prior to the posterior, in terms of magnitude and seasonality of the CO and CH<sub>4</sub> surface fluxes and of the HCHO production by non-methane volatile organic compounds (NMVOC). The latter is significantly decreased, indicating an overestimation of the biogenic NMVOC emissions, such as isoprene, in the GEIA inventory. CO and CH<sub>4</sub> surface emissions are increased by the inversion, from 1037 to 1394 TgCO and from 489 to 529 TgCH<sub>4</sub> on average for the 2005–2010 period. CH<sub>4</sub> emissions present significant interannual variability and a joint CO-CH<sub>4</sub> fluxes analysis reveals that tropical biomass burning probably played a role in the recent increase of atmospheric methane.
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The three-hour life-cycle of the isolated thunderstorm on 15 July 2007 during the Convective and Orographically-induced Precipitation Study (COPS) is documented in detail, with a special emphasis on the rapid development and mature phases. Remote sensing techniques as 5-min rapid scans from geostationary satellites, combined velocity retrievals from up to four Doppler-radars, the polarimetric determination of hydrometeors and spatio-temporal occurrences of lightning strokes are employed to arrive at a quantification of the physical parameters of this, during the COPS period, singular event. <br><br> Inner cloud flow fields are available from radar multiple Doppler analyses at four consecutive times separated by 15 min-intervals. They contain horizontal winds of around 15 m s<sup>−1</sup> and updrafts exceeding 5 m s<sup>−1</sup>, the latter collocated with lightning strokes. Reflectivity and polarimetric data indicate the existence of hail at the 2 km level around 14:40. Furthermore, polarimetric and Doppler radar variables indicate intense hydrometeor variability and turbulence corresponding to an enhanced variance of the retrieved 3-D wind fields. Profiles of flow and hydrometeor statistics over the entire cloud volume provide reference data for high-resolution numerical weather prediction runs in research mode. <br><br> The study embarks from two movie-loops of geostationary satellite imagery (as Supplement), which provide an intuitive distinction of six phases making up the entire life-cycle of the thunderstorm. It concludes with a triple-image loop, juxtaposing a close-up of the cloud motion as seen by Meteosat, simulated brightness temperature (as a proxy for clouds seen by the infrared satellite channel), and a perspective view on the model generated system of cloud cells. The simulation suggests that several updrafts fed from a low level convergence line eventually removed the convective inhibition and set deep convection in motion. A shear line in the radial velocity relative to the Feldberg radar site shows good agreement beween observation and simulation, whereas the onset location of deep convection exhibits a horizontal discrepancy of 15 km. A quantitative schematic of the isolated thunderstorm synthesizes all retrieved characteristics.
