O. Stein

Bio: O. Stein is an academic researcher from Forschungszentrum Jülich. The author has contributed to research in topics: Ozone layer & Stratosphere. The author has an hindex of 9, co-authored 15 publications receiving 445 citations.

Tropospheric chemistry in the integrated forecasting system of ECMWF

Abstract: . A representation of atmospheric chemistry has been included in the Integrated Forecasting System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The new chemistry modules complement the aerosol modules of the IFS for atmospheric composition, which is named C-IFS. C-IFS for chemistry supersedes a coupled system in which chemical transport model (CTM) Model for OZone and Related chemical Tracers 3 was two-way coupled to the IFS (IFS-MOZART). This paper contains a description of the new on-line implementation, an evaluation with observations and a comparison of the performance of C-IFS with MOZART and with a re-analysis of atmospheric composition produced by IFS-MOZART within the Monitoring Atmospheric Composition and Climate (MACC) project. The chemical mechanism of C-IFS is an extended version of the Carbon Bond 2005 (CB05) chemical mechanism as implemented in CTM Transport Model 5 (TM5). CB05 describes tropospheric chemistry with 54 species and 126 reactions. Wet deposition and lightning nitrogen monoxide (NO) emissions are modelled in C-IFS using the detailed input of the IFS physics package. A 1 year simulation by C-IFS, MOZART and the MACC re-analysis is evaluated against ozonesondes, carbon monoxide (CO) aircraft profiles, European surface observations of ozone (O3), CO, sulfur dioxide (SO2) and nitrogen dioxide (NO2) as well as satellite retrievals of CO, tropospheric NO2 and formaldehyde. Anthropogenic emissions from the MACC/CityZen (MACCity) inventory and biomass burning emissions from the Global Fire Assimilation System (GFAS) data set were used in the simulations by both C-IFS and MOZART. C-IFS (CB05) showed an improved performance with respect to MOZART for CO, upper tropospheric O3, and wintertime SO2, and was of a similar accuracy for other evaluated species. C-IFS (CB05) is about 10 times more computationally efficient than IFS-MOZART.

On the wintertime low bias of Northern Hemisphere carbon monoxide found in global model simulations

Abstract: . Despite the developments in the global modelling of chemistry and of the parameterization of the physical processes, carbon monoxide (CO) concentrations remain underestimated during Northern Hemisphere (NH) winter by most state-of-the-art chemistry transport models. The consequential model bias can in principle originate from either an underestimation of CO sources or an overestimation of its sinks. We address both the role of surface sources and sinks with a series of MOZART (Model for Ozone And Related Tracers) model sensitivity studies for the year 2008 and compare our results to observational data from ground-based stations, satellite observations, and vertical profiles from measurements on passenger aircraft. In our base case simulation using MACCity (Monitoring Atmospheric Composition and Climate project) anthropogenic emissions, the near-surface CO mixing ratios are underestimated in the Northern Hemisphere by more than 20 ppb from December to April, with the largest bias of up to 75 ppb over Europe in January. An increase in global biomass burning or biogenic emissions of CO or volatile organic compounds (VOCs) is not able to reduce the annual course of the model bias and yields concentrations over the Southern Hemisphere which are too high. Raising global annual anthropogenic emissions with a simple scaling factor results in overestimations of surface mixing ratios in most regions all year round. Instead, our results indicate that anthropogenic CO and, possibly, VOC emissions in the MACCity inventory are too low for the industrialized countries only during winter and spring. Reasonable agreement with observations can only be achieved if the CO emissions are adjusted seasonally with regionally varying scaling factors. A part of the model bias could also be eliminated by exchanging the original resistance-type dry deposition scheme with a parameterization for CO uptake by oxidation from soil bacteria and microbes, which reduces the boreal winter dry deposition fluxes. The best match to surface observations, satellite retrievals, and aircraft observations was achieved when the modified dry deposition scheme was combined with increased wintertime road traffic emissions over Europe and North America (factors up to 4.5 and 2, respectively). One reason for the apparent underestimation of emissions may be an exaggerated downward trend in the Representative Concentration Pathway (RCP) 8.5 scenario in these regions between 2000 and 2010, as this scenario was used to extrapolate the MACCity emissions from their base year 2000. This factor is potentially amplified by a lack of knowledge about the seasonality of emissions. A methane lifetime of 9.7 yr for our basic model and 9.8 yr for the optimized simulation agrees well with current estimates of global OH, but we cannot fully exclude a potential effect from errors in the geographical and seasonal distribution of OH concentrations on the modelled CO.

3-D evaluation of tropospheric ozone simulations by an ensemble of regional Chemistry Transport Model

Abstract: A detailed 3-D evaluation of an ensemble of five regional Chemistry Transport Models (RCTM) and one global CTM with focus on free tropospheric ozone over Europe is presented. It is performed over a summer period (June to August 2008) in the context of the GEMS-RAQ project. A data set of about 400 vertical ozone profiles from balloon soundings and commercial aircraft at 11 different locations is used for model evaluation, in addition to satellite measurements with the infrared nadir sounder (IASI) showing largest sensitivity to free tropospheric ozone. In the middle troposphere, the four regional models using the same top and boundary conditions from IFS-MOZART exhibit a systematic negative bias with respect to observed profiles of about-20 %. Root Mean Square Error (RMSE) values are constantly growing with altitude, from 22 % to 32 % to 53 %, respectively for 0-2 km, 2-8 km and 8-10 km height ranges. Lowest correlation is found in the middle troposphere, with minimum coefficients (R) between 0.2 to 0.45 near 8 km, as compared to 0.7 near the surface and similar values around10 km. A sensitivity test made with the CHIMERE mode also shows that using hourly instead of monthly chemical boundary conditions generally improves the model skill (i.e. improve RMSE and correlation). Lower tropospheric 0-6 km partial ozone columns derived from IASI show a clear North-South gradient over Europe, which is qualitatively reproduced by the models. Also the temporal variability showing decreasing ozone concentrations in the lower troposphere (0-6 km columns) during summer is well reproduced by models even if systematic bias remains (the value of the bias being also controlled by the type of used boundary conditions). A multi-day case study of a trough with low tropopause was conducted and showed that both IASI and models were able to resolve strong horizontal gradients of middle and upper tropospheric ozone occurring in the vicinity of an upper tropospheric frontal zone.

Current status of the ability of the GEMS/MACC models to reproduce the tropospheric CO vertical distribution as measured by MOZAIC

Abstract: . Vertical profiles of CO taken from the MOZAIC aircraft database are used to globally evaluate the performance of the GEMS/MACC models, including the ECMWF-Integrated Forecasting System (IFS) model coupled to the CTM MOZART-3 with 4DVAR data assimilation for the year 2004. This study provides a unique opportunity to compare the performance of three offline CTMs (MOZART-3, MOCAGE and TM5) driven by the same meteorology as well as one coupled atmosphere/CTM model run with data assimilation, enabling us to assess the potential gain brought by the combination of online transport and the 4DVAR chemical satellite data assimilation. First we present a global analysis of observed CO seasonal averages and interannual variability for the years 2002–2007. Results show that despite the intense boreal forest fires that occurred during the summer in Alaska and Canada, the year 2004 had comparably lower tropospheric CO concentrations. Next we present a validation of CO estimates produced by the MACC models for 2004, including an assessment of their ability to transport pollutants originating from the Alaskan/Canadian wildfires. In general, all the models tend to underestimate CO. The coupled model and the CTMs perform best in Europe and the US where biases range from 0 to -25% in the free troposphere and from 0 to -50% in the surface and boundary layers (BL). Using the 4DVAR technique to assimilate MOPITT V4 CO significantly reduces biases by up to 50% in most regions. However none of the models, even the IFS-MOZART-3 coupled model with assimilation, are able to reproduce well the CO plumes originating from the Alaskan/Canadian wildfires at downwind locations in the eastern US and Europe. Sensitivity tests reveal that deficiencies in the fire emissions inventory and injection height play a role.

Evaluation of near-surface ozone over Europe from the MACC reanalysis

Abstract: . This work is an extended evaluation of near-surface ozone as part of the global reanalysis of atmospheric composition, produced within the European-funded project MACC (Monitoring Atmospheric Composition and Climate). It includes an evaluation over the period 2003–2012 and provides an overall assessment of the modeling system performance with respect to near-surface ozone for specific European subregions. Measurements at rural locations from the European Monitoring and Evaluation Program (EMEP) and the European Air Quality Database (AirBase) were used for the evaluation assessment. The fractional gross error of near-surface ozone reanalysis is on average 24 % over Europe, the highest found over Scandinavia (27 %) and the lowest over the Mediterranean marine stations (21 %). Near-surface ozone shows mostly a negative bias in winter and a positive bias during warm months. Assimilation reduces the bias in near-surface ozone in most of the European subregions – with the exception of Britain and Ireland and the Iberian Peninsula and its impact is mostly notable in winter. With respect to the seasonal cycle, the MACC reanalysis reproduces the photochemically driven broad spring-summer maximum of surface ozone of central and south Europe. However, it does not capture adequately the early spring peak and the shape of the seasonality at northern and north-eastern Europe. The diurnal range of surface ozone, which is as an indication of the local photochemical production processes, is reproduced fairly well, with a tendency for a small overestimation during the warm months for most subregions (especially in central and southern Europe). Possible reasons leading to discrepancies between the MACC reanalysis and observations are discussed.

Tropospheric ozone and its precursors from the urban to the global scale from air quality to short-lived climate forcer

Abstract: Ozone holds a certain fascination in atmospheric science. It is ubiquitous in the atmosphere, central to tropospheric oxidation chemistry, yet harmful to human and ecosystem health as well as being an important greenhouse gas. It is not emitted into the atmosphere but is a by-product of the very oxidation chemistry it largely initiates. Much effort is focussed on the reduction of surface levels of ozone owing to its health impacts but recent efforts to achieve reductions in exposure at a country scale have proved difficult to achieve due to increases in background ozone at the zonal hemispheric scale. There is also a growing realisation that the role of ozone as a short-lived climate pollutant could be important in integrated air quality climate-change mitigation. This review examines current understanding of the processes regulating tropospheric ozone at global to local scales from both measurements and models. It takes the view that knowledge across the scales is important for dealing with air quality and climate change in a synergistic manner.

The Atmospheric Chemistry Experiment (ACE): Mission Overview

Abstract: ACE is a Canadian satellite mission that will provide measurements leading to an improved understanding of the chemical and dynamical processes that control the distribution of ozone in the stratosphere. The ACE instruments are a Fourier transform infrared spectrometer, a UV/visible/near IR spectrograph and a two-channel solar imager, all working in solar occultation mode. ACE was successfully launched on August 12, 2003.

The CAMS reanalysis of atmospheric composition

Abstract: . The Copernicus Atmosphere Monitoring Service (CAMS) reanalysis is the latest global reanalysis dataset of atmospheric composition produced by the European Centre for Medium-Range Weather Forecasts (ECMWF), consisting of three-dimensional time-consistent atmospheric composition fields, including aerosols and chemical species. The dataset currently covers the period 2003–2016 and will be extended in the future by adding 1 year each year. A reanalysis for greenhouse gases is being produced separately. The CAMS reanalysis builds on the experience gained during the production of the earlier Monitoring Atmospheric Composition and Climate (MACC) reanalysis and CAMS interim reanalysis. Satellite retrievals of total column CO; tropospheric column NO2 ; aerosol optical depth (AOD); and total column, partial column and profile ozone retrievals were assimilated for the CAMS reanalysis with ECMWF's Integrated Forecasting System. The new reanalysis has an increased horizontal resolution of about 80 km and provides more chemical species at a better temporal resolution (3-hourly analysis fields, 3-hourly forecast fields and hourly surface forecast fields) than the previously produced CAMS interim reanalysis. The CAMS reanalysis has smaller biases compared with most of the independent ozone, carbon monoxide, nitrogen dioxide and aerosol optical depth observations used for validation in this paper than the previous two reanalyses and is much improved and more consistent in time, especially compared to the MACC reanalysis. The CAMS reanalysis is a dataset that can be used to compute climatologies, study trends, evaluate models, benchmark other reanalyses or serve as boundary conditions for regional models for past periods.

CHIMERE 2013: a model for regional atmospheric composition modelling

Abstract: . Tropospheric trace gas and aerosol pollutants have adverse effects on health, environment and climate. In order to quantify and mitigate such effects, a wide range of processes leading to the formation and transport of pollutants must be considered, understood and represented in numerical models. Regional scale pollution episodes result from the combination of several factors: high emissions (from anthropogenic or natural sources), stagnant meteorological conditions, kinetics and efficiency of the chemistry and the deposition. All these processes are highly variable in time and space, and their relative contribution to the pollutants budgets can be quantified with chemistry-transport models. The CHIMERE chemistry-transport model is dedicated to regional atmospheric pollution event studies. Since it has now reached a certain level a maturity, the new stable version, CHIMERE 2013, is described to provide a reference model paper. The successive developments of the model are reviewed on the basis of published investigations that are referenced in order to discuss the scientific choices and to provide an overview of the main results.

The MACC reanalysis: an 8 yr data set of atmospheric composition

Abstract: . An eight-year long reanalysis of atmospheric composition data covering the period 2003–2010 was constructed as part of the FP7-funded Monitoring Atmospheric Composition and Climate project by assimilating satellite data into a global model and data assimilation system. This reanalysis provides fields of chemically reactive gases, namely carbon monoxide, ozone, nitrogen oxides, and formaldehyde, as well as aerosols and greenhouse gases globally at a horizontal resolution of about 80 km for both the troposphere and the stratosphere. This paper describes the assimilation system for the reactive gases and presents validation results for the reactive gas analysis fields to document the data set and to give a first indication of its quality. Tropospheric CO values from the MACC reanalysis are on average 10–20% lower than routine observations from commercial aircrafts over airports through most of the troposphere, and have larger negative biases in the boundary layer at urban sites affected by air pollution, possibly due to an underestimation of CO or precursor emissions. Stratospheric ozone fields from the MACC reanalysis agree with ozonesondes and ACE-FTS data to within ±10% in most seasons and regions. In the troposphere the reanalysis shows biases of −5% to +10% with respect to ozonesondes and aircraft data in the extratropics, but has larger negative biases in the tropics. Area-averaged total column ozone agrees with ozone fields from a multi-sensor reanalysis data set to within a few percent. NO2 fields from the reanalysis show the right seasonality over polluted urban areas of the NH and over tropical biomass burning areas, but underestimate wintertime NO2 maxima over anthropogenic pollution regions and overestimate NO2 in northern and southern Africa during the tropical biomass burning seasons. Tropospheric HCHO is well simulated in the MACC reanalysis even though no satellite data are assimilated. It shows good agreement with independent SCIAMACHY retrievals over regions dominated by biogenic emissions with some anthropogenic input, such as the eastern US and China, and also over African regions influenced by biogenic sources and biomass burning.