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Stohl, A.

Publications and source records attributed to Stohl, A..

Evaluation of Observed and Modelled Aerosol Lifetimes Using Radioactive Tracers of Opportunity and an Ensemble of 19 Global Models

Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (Cs-137) and xenon-133 (Xe-133) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. Cs-137 size distribution measurements taken close to the power plant suggested that accumulation mode (AM) sulfate aerosols were the main carriers of cesium. Hence, Cs-137 can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas Xe-133 behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of Cs-137that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and Xe-133 emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled Cs-137and Xe-133 concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime e, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95% confidence interval 13.1-15.7 days). The equivalent modelled e lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.42.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (Xe-133) concentrations in the Arctic as well but to a smaller extent than for the aerosol (Cs-137) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.

Radioactive isotopes↗

Smoke Dispersion Modeling Over Complex Terrain Using High-Resolution Meteorological Data and Satellite Observations: The FireHub Platform

A total number of 20,212 fire hot spots were recorded by the Moderate Resolution Imaging Spectroradiometer (MODIS) satellite instrument over Greece during the period 2002e2013. The Fire Radiative Power (FRP) of these events ranged from 10 up to 6000 MW at 1 km resolution, and many of these fire episodes resulted in long-range transport of smoke over distances up to several hundred kilometers. Three different smoke episodes over Greece are analyzed here using real time hot-spot observations from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) satellite instrument as well as from MODIS hot-spots. Simulations of smoke dispersion are performed with the FLEXPART-WRF model and particulate matter emissions are calculated directly from the observed FRP. The modeled smoke plumes are compared with smoke stereo-heights from the Multiangle Imaging Spectroradiometer (MISR) instrument and the sensitivities to atmospheric and modeling parameters are examined. Driving the simulations with high resolution meteorology (4 4 km) and using geostationary satellite data to identify the hot spots allows the description of local scale features that govern smoke dispersion. The long-range transport of smoke is found to be favored over the complex coastline environment of Greece due to the abrupt changes between land and marine planetary boundary layers (PBL) and the decoupling of smoke layers from the surface.

fire smoke↗

Simultaneous Retrieval of Aerosol and Cloud Properties During the MILAGRO Field Campaign

Estimation of Direct Climate Forcing (DCF) due to aerosols in cloudy areas has historically been a difficult task, mainly because of a lack of appropriate measurements. Recently, passive remote sensing instruments have been developed that have the potential to retrieve both cloud and aerosol properties using polarimetric, multiple view angle, and multi spectral observations, and therefore determine DCF from aerosols above clouds. One such instrument is the Research Scanning Polarimeter (RSP), an airborne prototype of a sensor on the NASA Glory satellite, which unfortunately failed to reach orbit during its launch in March of 2011. In the spring of 2006, the RSP was deployed on an aircraft based in Veracruz, Mexico, as part of the Megacity Initiative: Local and Global Research Observations (MILAGRO) field campaign. On 13 March, the RSP over flew an aerosol layer lofted above a low altitude marine stratocumulus cloud close to shore in the Gulf of Mexico. We investigate the feasibility of retrieving aerosol properties over clouds using these data. Our approach is to first determine cloud droplet size distribution using the angular location of the cloud bow and other features in the polarized reflectance. The selected cloud was then used in a multiple scattering radiative transfer model optimization to determine the aerosol optical properties and fine tune the cloud size distribution. In this scene, we were able to retrieve aerosol optical depth, the fine mode aerosol size distribution parameters and the cloud droplet size distribution parameters to a degree of accuracy required for climate modeling. This required assumptions about the aerosol vertical distribution and the optical properties of the coarse aerosol size mode. A sensitivity study was also performed to place this study in the context of future systematic scanning polarimeter observations, which found that the aerosol complex refractive index can also be observed accurately if the aerosol optical depth is larger than roughly 0.8 at a wavelength of (0.555 m).

Knobelspiesse, K.↗

Episodes of Cross-Polar Transport in the Arctic Troposphere During July 2008 as Seen from Models, Satellite, and Aircraft Observations

During the POLARCAT summer campaign in 2008, two episodes (2 5 July and 7 10 July 2008) occurred where low-pressure systems traveled from Siberia across the Arctic Ocean towards the North Pole. The two cyclones had extensive smoke plumes from Siberian forest fires and anthropogenic sources in East Asia embedded in their associated air masses, creating an excellent opportunity to use satellite and aircraft observations to validate the performance of atmospheric transport models in the Arctic, which is a challenging model domain due to numerical and other complications. Here we compare transport simulations of carbon monoxide (CO) from the Lagrangian transport model FLEXPART and the Eulerian chemical transport model TOMCAT with retrievals of total column CO from the IASI passive infrared sensor onboard the MetOp-A satellite. The main aspect of the comparison is how realistic horizontal and vertical structures are represented in the model simulations. Analysis of CALIPSO lidar curtains and in situ aircraft measurements provide further independent reference points to assess how reliable the model simulations are and what the main limitations are. The horizontal structure of mid-latitude pollution plumes agrees well between the IASI total column CO and the model simulations. However, finer-scale structures are too quickly diffused in the Eulerian model. Applying the IASI averaging kernels to the model data is essential for a meaningful comparison. Using aircraft data as a reference suggests that the satellite data are biased high, while TOMCAT is biased low. FLEXPART fits the aircraft data rather well, but due to added background concentrations the simulation is not independent from observations. The multi-data, multi-model approach allows separating the influences of meteorological fields, model realisation, and grid type on the plume structure. In addition to the very good agreement between simulated and observed total column CO fields, the results also highlight the difficulty to identify a data set that most realistically represents the actual pollution state of the Arctic atmosphere.

Sodemann, H.↗

Increasing Springtime Ozone Mixing Ratios in the Free Troposphere Over Western North America

In the lowermost layer of the atmosphere - the troposphere - ozone is an important source of the hydroxyl radical, an oxidant that breaks down most pollutants and some greenhouse gases. High concentrations of tropospheric ozone are toxic, however, and have a detrimental effect on human health and ecosystem productivity1. Moreover, tropospheric ozone itself acts as an effective greenhouse gas. Much of the present tropospheric ozone burden is a consequence of anthropogenic emissions of ozone precursors resulting in widespread increases in ozone concentrations since the late 1800s. At present, east Asia has the fastest-growing ozone precursor emissions. Much of the springtime east Asian pollution is exported eastwards towards western North America. Despite evidence that the exported Asian pollution produces ozone, no previous study has found a significant increase in free tropospheric ozone concentrations above the western USA since measurements began in the late 1970s. Here we compile springtime ozone measurements from many different platforms across western North America. We show a strong increase in springtime ozone mixing ratios during 1995-2008 and we have some additional evidence that a similar rate of increase in ozone mixing ratio has occurred since 1984. We find that the rate of increase in ozone mixing ratio is greatest when measurements are more heavily influenced by direct transport from Asia. Our result agrees with previous modelling studies, which indicate that global ozone concentrations should be increasing during the early part of the twenty-first century as a result of increasing precursor emissions, especially at northern mid-latitudes, with western North America being particularly sensitive to rising Asian emissions. We suggest that the observed increase in springtime background ozone mixing ratio may hinder the USA s compliance with its ozone air quality standard.

Cooper, O. R.↗

Establishing Lagrangian Connections between Observations within Air Masses Crossing the Atlantic during the ICARTT Experiment

The International Consortium for Atmospheric Research on Transport and Transformation (ICARTT)-Lagrangian experiment was conceived with an aim to quantify the effects of photochemistry and mixing on the transformation of air masses in the free troposphere away from emissions. To this end attempts were made to intercept and sample air masses several times during their journey across the North Atlantic using four aircraft based in New Hampshire (USA), Faial (Azores) and Creil (France). This article begins by describing forecasts using two Lagrangian models that were used to direct the aircraft into target air masses. A novel technique is then used to identify Lagrangian matches between flight segments. Two independent searches are conducted: for Lagrangian model matches and for pairs of whole air samples with matching hydrocarbon fingerprints. The information is filtered further by searching for matching hydrocarbon samples that are linked by matching trajectories. The quality of these coincident matches is assessed using temperature, humidity and tracer observations. The technique pulls out five clear Lagrangian cases covering a variety of situations and these are examined in detail. The matching trajectories and hydrocarbon fingerprints are shown and the downwind minus upwind differences in tracers are discussed.

Methven, J.↗

Estimating the NO(x) produced by lightning from GOME and NLDN data: A case study in the Gulf of Mexico

Nitrogen oxides (NO(x)=NO+NO2) play an important role in tropospheric chemistry, in particular in catalytic ozone production. Lightning provides a natural source of nitrogen oxides, dominating the production in the tropical upper troposphere, with strong impact on tropospheric ozone and the atmosphere s oxidizing capacity. Recent estimates of lightning produced NO(x) (LNO(x)) are of the order of 5 Tg [N] per year with still high uncertainties in the range of one order of magnitude. The Global Ozone Monitoring Experiment (GOME) on board the ESA-satellite ERS-2 allows the retrieval of tropospheric column densities of NO2 on a global scale. Here we present the GOME NO2 measurement directly over a large convective system over the Gulf of Mexico. Simultaneously, cloud-to-ground (CG) flashes are counted by the U.S. National Lightning Detection Network (NLDN(TradeMark)), and extrapolated to include intracloud (IC)+CG flashes based on a climatological IC:CG ratio derived from NASA s space-based lightning sensors. A series of 14 GOME pixels shows largely enhanced column densities over thick and high clouds, coinciding with strong lightning activity. The enhancements can not be explained by transport of anthropogenic NO(x) and must be due to fresh production of LNO(x). A quantitative analysis, accounting in particular for the visibility of LNO, from satellite, yields a LNO, production of 90 (32-240) moles of NO(x), or 1.3 (0.4-3.4) kg [N], per flash. If simply extrapolated, this corresponds to a global LNO(x) production of 1.7 (0.6-4.7) Tg [N]/yr.

Beirle, S.↗

Processes Influencing Ozone Levels in Alaskan Forest Fires Plumes during Long-Range Transport over the North Atlantic

A case of long-range transport of a biomass burning plume from Alaska to Europe is analyzed using a Lagrangian approach. This plume was sampled several times in the free troposphere over North America, the North Atlantic and Europe by 3 different aircraft during the IGAC Lagrangian 2K4 experiment which was part of the ICARTT/ITOP measurement intensive in summer 2004. Measurements in the plume showed enhanced values of CO, VOCs and NOy, mainly in form of PAN. Observed O3 levels increased by 17 ppbv over 5 days. A photochemical trajectory model, CiTTyCAT, is used to examine processes responsible for the chemical evolution of the plume. The model was initialized with upwind data, and compared with downwind measurements. The influence of high aerosol loading on photolysis rates in the plume is investigated using in-situ aerosol measurements in the plume and lidar retrievals of optical depth as input into a photolysis code (Fast-J), run in the model. Significant impacts on photochemistry are found with a decrease of 18 percent in O3 production and 24 percent in O3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O3 increases attributed primarily to PAN decomposition during descent of the plume towards Europe. The predicted O3 changes are very dependent on temperature changes during transport, and also, on water vapor levels in the lower troposphere which can lead to O3 destruction. Simulation of mixing/dilution was necessary to reproduce observed pollutants level in the plume. Mixing was simulated using background concentrations from measurements in air masses in close proximity to the plume, and mixing timescales (averaging 6.25 days) were derived from CO changes. Observed and simulated O3/CO correlations in the plume are also compared in order to evaluate the photochemistry in the model. Observed slopes changed from negative to positive over 5 days. This change, which can be attributed largely to photochemistry, is well reproduced by multiple model runs even if slope values are slightly underestimated suggesting small underestimation of photochemical processes. The possible impact of this biomass burning plume on O3 levels in the Europe boundary layer is also examined by running the model for a further 5 days, and comparing with data collected at surface sites, such as Jungfraujoch, which showed small O3 increases and elevated CO levels. The model predicts significant changes in O3 over this 10 days due to photochemistry but the signal is largely lost due to the effects of dilution. However, measurement in several others BB plumes over Europe show that O3 impact of Alaskan fires can be punctually significant over Europe.

Real, E.↗