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Estimates of lightning NOx production from GOME satellite observations

Tropospheric NO2 column retrievals from the Global Ozone Monitoring Experiment (GOME) satellite spectrometer are used to quantify the source strength and 3-D distribution of lightning produced nitrogen oxides (NOx=NO+NO2). A sharp increase of NO2 is observed at convective cloud tops with increasing cloud top height, consistent with a power-law behaviour with power 5±2. Convective production of clouds with the same cloud height are found to produce NO2 with a ratio 1.6/1 for continents compared to oceans. This relation between cloud properties and NO2 is used to construct a 10:30 local time global lightning NO2 production map for 1997. An extensive statistical comparison is conducted to investigate the capability of the TM3 chemistry transport model to reproduce observed patterns of lightning NO2 in time and space. This comparison uses the averaging kernel to relate modelled profiles of NO2 to observed NO2 columns. It exploits a masking scheme to minimise the interference of other NOx sources on the observed total columns. Simulations are performed with two lightning parameterizations, one relating convective preciptation (CP scheme) to lightning flash distributions, and the other relating the fifth power of the cloud top height (H5 scheme) to lightning distributions. The satellite-retrieved NO2 fields show significant correlations with the simulated lightning contribution to the NO2 concentrations for both parameterizations. Over tropical continents modelled lightning NO2 shows remarkable quantitative agreement with observations. Over the oceans however, the two model lightning parameterizations overestimate the retrieved NO2 attributed to lightning. Possible explanations for these overestimations are discussed. The ratio between satellite-retrieved NO2 and modelled lightning NO2 is used to rescale the original modelled lightning NOx production. Eight estimates of the lightning NOx production in 1997 are obtained from spatial and temporal correlation methods, from cloud-free and cloud-covered observations, and from two different lightning parameterizations. Accounting for a wide variety of random and possible systematic errors, we estimate the global NOx production from lightning to be in the range 1.1–6.4 Tg N in 1997.
CLABAUTAIR: a new algorithm for retrieving three-dimensional cloud structure from airborne microphysical measurements

A new algorithm is presented to reproduce the three-dimensional structure of clouds from airborne measurements of microphysical parameters. Data from individual flight legs are scanned for characteristic patterns, and the autocorrelation functions for several directions are used to extrapolate the observations along the flight path to a full three-dimensional distribution of the cloud field. Thereby, the mean measured profiles of microphysical parameters are imposed to the cloud field by mapping the measured probability density functions onto the model layers. The algorithm was tested by simulating flight legs through synthetic clouds (by means of Large Eddy Simulations (LES)) and applied to a stratocumulus cloud case measured during the first field experiment of the EC project INSPECTRO (INfluence of clouds on the SPECtral actinic flux in the lower TROposphere) in East Anglia, UK. The number and position of the flight tracks determine the quality of the retrieved cloud field. If they provide a representative sample of the entire field, the derived pattern closely resembles the statistical properties of the real cloud field.
Modelling photochemistry in alpine valleys

Road traffic is a serious problem in the Chamonix Valley, France: traffic, noise and above all air pollution worry the inhabitants. The big fire in the Mont-Blanc tunnel made it possible, in the framework of the POVA project (POllution in Alpine Valleys), to undertake measurement campaigns with and without heavy-vehicle traffic through the Chamonix and Maurienne valleys, towards Italy (before and after the tunnel re-opening). Modelling is one of the aspects of POVA and should make it possible to explain the processes leading to episodes of atmospheric pollution, both in summer and in winter. Atmospheric prediction model ARPS 4.5.2 (Advanced Regional Prediction System), developed at the CAPS (Center for Analysis and Prediction of Storms) of the University of Oklahoma, enables to resolve the dynamics above a complex terrain. This model is coupled to the TAPOM 1.5.2 atmospheric chemistry (Transport and Air POllution Model) code developed at the Air and Soil Pollution Laboratory of the Ecole Polytechnique Fédérale de Lausanne. The numerical codes MM5 and CHIMERE are used to compute large scale boundary forcing. This paper focuses on modelling Chamonix valley using 300-m grid cells to calculate the dynamics and the reactive chemistry which makes possible to accurately represent the dynamics in the Chamonix valley (slope and valley winds) and to process chemistry at fine scale. The summer 2003 intensive campaign was used to validate the model and to study chemistry. NOy according to O3 reduction demonstrates a VOC controlled regime, different from the NOx controlled regime expected and observed in the nearby city of Grenoble.
Global satellite validation of SCIAMACHY O3 columns with GOME WFDOAS

Global stratospheric ozone columns derived from UV nadir spectra measured by SCIAMACHY (Scanning Imaging Spectrometer for Atmospheric Chartography; data ESA Versions 5.01 and 5.04) aboard the recently launched Environmental Satellite (ENVISAT) from January to June 2003 were compared to collocated total ozone data from GOME (Global Ozone Monitoring Experiment on ERS-2) retrieved using the weighting function DOAS algorithm (WFDOAS; Version 1.0) in order to assess the level-2 data (trace gas data) retrieval accuracy from SCIAMACHY. In addition, SCIAMACHY ozone columns retrieved with WFDOAS V1.0 were compared to GOME WFDOAS for some selected days in 2003 in order to separate data quality issues that either come from the optical performance of the instrument or algorithm implementation. Large numbers of collocated total ozone data from the two instruments, which are flying in the same orbit about 30 min apart, were spatially binned into regular 2.5° times 2.5° grids and then compared. Results of these satellite comparisons show that SCIAMACHY O3 vertical columns (ESA Version 5.01/5.04) are on average 1% (±2%) lower than GOME WFDOAS and scatter increases at solar zenith angles above 85° and at very low total ozone values. Results show dependencies on the solar zenith angle, latitudes, and total ozone amounts which are explained by the implementation of an outdated GOME algorithm based on GOME Data Processor (GDP) version 2.4 algorithms for the SCIAMACHY operational product. The reprocessing with an algorithm equivalent to GOME WFDOAS V1.0 shows that the offset and dependencies on solar zenith angle, latitude, and total ozone disappear and that SCIAMACHY WFDOAS data are within 1% of GOME WFDOAS. Since GOME lost its global coverage in July 2003 due to data rate limitation, continuation of the total ozone time series with SCIAMACHY is of highest importance for long-term trend monitoring. Since the beginning of its operation in March 2002 the SCIAMACHY instrument has performed stable. With the application of proper algorithms to retrieve total ozone, SCIAMACHY will be able to contribute to the global long term satellite total ozone record and it has the potential to achieve the high accuracy of GOME total ozone.
The impact of SCIAMACHY near-infrared instrument calibration on CH4 and CO total columns

The near-infrared spectra measured with the SCIAMACHY instrument on board the ENVISAT satellite suffer from several instrument calibration problems. The effects of three important instrument calibration issues on the retrieved methane (CH4) and carbon monoxide (CO) total columns have been investigated: the effects of the growing ice layer on the near-infrared detectors, the effects of the orbital variation of the instrument dark signal, and the effects of the dead/bad detector pixels. Corrections for each of these instrument calibration issues have been defined. The retrieved CH4 and CO total columns including these corrections show good agreement with CO measurements from the MOPITT satellite instrument and with CH4 model calculations by the chemistry transport model TM3. Using a systematic approach, it is shown that all three instrument calibration issues have a significant effect on the retrieved CH4 and CO total columns. However, the impact on the CH4 total columns is more pronounced than for CO, because of its smaller variability. Results for three different wavelength ranges are compared and show good agreement. The growing ice layer and the orbital variation of the dark signal show a systematic, but time-dependent effect on the retrieved CH4 and CO total columns, whereas the effect of the dead/bad pixels is rather unpredictable: some dead pixels show a random effect, some more systematic, and others no effect at all. The importance of accurate corrections for each of these instrument calibration issues is illustrated using examples where inaccurate corrections lead to a wrong interpretation of the results.
SCIAMACHY Absorbing Aerosol Index – calibration issues and global results from 2002–2004

The validity of the Absorbing Aerosol Index (AAI) product from the SCanning Imaging Absorption SpectroMeter for Atmospheric CartograpHY (SCIAMACHY) is discussed. The operational SCIAMACHY AAI product suffers from calibration errors in the reflectance as measured by SCIAMACHY and neglect of polarisation effects in the AAI computational algorithm. Therefore, the AAI product was recalculated, compensating for the errors, with reflectance data from the start of measurements of SCIAMACHY until December 2004. Appropriate correction factors were determined for the UV to correct for the radiometric error in the SCIAMACHY reflectances. The algorithm was provided with LookUp Tables in which a good representation of polarisation effects was incorporated, as opposed to the LookUp Tables of the operational product, in which polarisation effects were not accounted for. The results are presented, their validity discussed, and compared to the operational product and independent AAI data from the Total Ozone Mapping Spectrometer (TOMS). The AAI is very sensitive to calibration errors and can be used to monitor calibration errors and changes. The AAI is sensitive to sunglint and a correction flag used for the AAI is presented. From 2004 onwards, the new SCIAMACHY AAI is suitable to add to the continuation of the long-term AAI record. Important changes in the long-term AAI record due to instrument and algorithm changes are highlighted. Recommendations are given for improvement of the operational AAI product.
New insight into the atmospheric chloromethane budget gained using stable carbon isotope ratios

Atmospheric chloromethane (CH3Cl) plays an important role in stratospheric ozone destruction, but many uncertainties still exist regarding strengths of both sources and sinks and the processes leading to formation of this naturally occurring gas. Recent work has identified a novel chemical origin for CH3Cl, which can explain its production in a variety of terrestrial environments: the widespread structural component of plants, pectin, reacts readily with chloride ion to form CH3Cl at both ambient and elevated temperatures (Hamilton et al., 2003). It has been proposed that this abiotic chloride methylation process in terrestrial environments could be responsible for formation of a large proportion of atmospheric CH3Cl. However, more information is required to determine the global importance of this new source and its contribution to the atmospheric CH3Cl budget. A potentially powerful tool in studying the atmospheric CH3Cl budget is the use of stable carbon isotope ratios. In an accompanying paper it is reported that the reaction of CH3Cl with OH radical, the dominant sink for atmospheric CH3Cl, is accompanied by an unexpectedly large fractionation factor (Gola et al., 2005). Another recently published study shows that CH3Cl formed by the abiotic methylation process at ambient temperatures has a unique stable carbon isotope signature, extremely depleted in 13C, unequivocally distinguishing it from all other known sources (Keppler et al., 2004). Using these findings together with data existing in the literature, we here present three scenarios for an isotopic mass balance for atmospheric CH3Cl. Our calculations provide strong support for the proposal that the largest source of atmospheric CH3Cl (1800 to 2500 Gg yr-1) is the abiotic methylation of chloride in terrestrial ecosytems, primarily located in tropical and subtropical areas where turnover of biomass is highest. Furthermore our calculations also indicate that the microbial soil sink for CH3Cl is likely to be much larger (>1000 Gg yr-1) than that previously assumed.
European surface ozone in the extreme summer 2003

Measurements of ozone and other species from the European EMEP network in 2003 are presented. The European summer of 2003 was exceptionally warm and the surface ozone data for central Europe show the highest values since the end of the 1980s. The concentrations were particularly high in June and August 2003. In this paper we argue that a number of positive feedback effects between the weather conditions and ozone contributed to the elevated surface ozone. Firstly, direct measurements of isoprene as well as the increased temperature and solar radiation indicate that biogenic emissions in Europe were increased during summer 2003 with a potential for enhanced ozone formation. Secondly, we show that the anticyclonic conditions during the ozone episodes were accompanied by an extended residence time of air parcels in the atmospheric boundary layer, a low total ozone column and a reduced cloud cover, all favouring ozone formation. Thirdly, based on the Lagrangian dispersion model FLEXPART, we show that is very likely that extensive forest fires on the Iberian Peninsula, resulting from the drought and heat, contributed to the peak ozone values observed in North Europe in August. Additionally, forest fires in Siberia probably lead to an elevated background level of ozone and CO at northern latitudes during summer 2003 thereby increasing the level the peak ozone episodes sat on. Lastly, and most important, the heat wave presumably lead to less efficient ozone dry deposition due to stomata closure of the plants under drought stress. Due to climate change, situations like this may occur at a higher frequency in the future and may gradually overshadow the effect of reduced emissions from anthropogenic sources of VOC and NOx. This scenario also holds for secondary PM.
Validation of ENVISAT/SCIAMACHY columnar methane by solar FTIR spectrometry at the Ground-Truthing Station Zugspitze

Methane total-vertical column retrievals from ground-based solar FTIR measurements at the Permanent Ground-Truthing Station Zugspitze (47.42° N, 10.98° E, 2964m a.s.l.), Germany are used to validate column averaged methane retrieved from ENVISAT/SCIAMACHY spectra by WFM-DOAS (WFMD) version 0.4 and 0.41 for 153 days in 2003. Smoothing errors are estimated to be below 0.10% for FTIR and 0.14% for SCIAMACHY-WFMD retrievals and can be neglected for the assessment of observed bias and day-to-day-scatter. In order to minimize the altitude-difference effect, dry-air column averaged mixing ratios (XCH4) have been utilized. From the FTIR-time series of XCH4 an atmospheric day-to-day variability of 1% was found, and a sinusoidal annual cycle with a ≈1.6% amplitude. To obtain the WFMD bias, a polynomial fitted to the FTIR series was used as a reference. The result is WFMD v0.4/FTIR=1.008±0.019 and WFMD v0.41/FTIR=1.058±0.008. WFMD v0.41 was significantly improved by a time-dependent bias correction. It can still not capture the natural day-to-day variability, i.e., the standard deviation calculated from the daily-mean values is 2.4% using averages within a 2000-km radius, and 2.7% for a 1000-km radius. These numbers are dominated by a residual time-dependent bias in the order of 3%/month. The latter can be reduced, e.g., from 2.4% to 1.6% as shown by an empirical time-dependent bias correction. Standard deviations of the daily means, calculated from the individual measurements of each day, are excluding time-dependent biases, thus showing the potential precision of WFMD daily means, i.e., 0.3% for a 2000-km selection radius, and 0.6% for a 1000-km selection radius. Therefore, the annual cycle as well as possibly the day-to-day variability could be captured under the prerequisite of further advanced time-dependent bias corrections, or the use of other channels, where the icing issue is less prominent.
Inverse modelling of national and European CH4 emissions using the atmospheric zoom model TM5

A synthesis inversion based on the atmospheric zoom model TM5 is used to derive top-down estimates of CH4 emissions from individual European countries for the year 2001. We employ a model zoom over Europe with 1° × 1° resolution that is two-way nested into the global model domain (with resolution of 6° × 4°. This approach ensures consistent boundary conditions for the zoom domain and thus European top-down estimates consistent with global CH4 observations. The TM5 model, driven by ECMWF analyses, simulates synoptic scale events at most European and global sites fairly well, and the use of high-frequency observations allows exploiting the information content of individual synoptic events. A detailed source attribution is presented for a comprehensive set of 56 monitoring sites, assigning the atmospheric signal to the emissions of individual European countries and larger global regions. The available observational data put significant constraints on emissions from different regions. Within Europe, in particular several Western European countries are well constrained. The inversion results suggest up to 50-90% higher anthropogenic CH4 emissions in 2001 for Germany, France and UK compared to reported UNFCCC values (EEA, 2003). A recent revision of the German inventory, however, resulted in an increase of reported CH4 emissions by 68.5% (EEA, 2004), being now in very good agreement with our top-down estimate. The top-down estimate for Finland is distinctly smaller than the a priori estimate, suggesting much smaller CH4 emissions from Finnish wetlands than derived from the bottom-up inventory. The EU-15 totals are relatively close to UNFCCC values (within 4-30%) and appear very robust for different inversion scenarios.