bluuebunny/crossref_metadata_2025_split huggingface dataset:
Validation of ENVISAT/SCIAMACHY columnar methane by solar FTIR spectrometry at the Ground-Truthing Station Zugspitze
Authors: Sussmann R. , Stremme W. , Buchwitz M. , de Beek R. 
Published: April 2010

Abstract. Methane total-vertical column retrievals from ground-based solar FTIR measurements at the Permanent Ground-Truthing Station Zugspitze (47.42° N, 10.98° E, 2964 m 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 natural 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.
Geophysical validation of SCIAMACHY Limb Ozone Profiles
Authors: Brinksma E. J. , Bracher A. , Lolkema D. E. , Segers A. J. , Boyd I. S. , Bramstedt K. , Claude H. , Godin-Beekmann S. , Hansen G. , Kopp G. , Leblanc T. , McDermid I. S. , Meijer Y. J. , Nakane H. , Parrish A. , von Savigny C. , Stebel K. , Swart D. P. J. , Taha G. , Piters A. J. M. 
Published: April 2010

Abstract. We discuss the quality of the two available SCIAMACHY limb ozone profile products. They were retrieved with the University of Bremen IFE's algorithm version 1.61 (hereafter IFE), and the official ESA offline algorithm (hereafter OL) versions 2.4 and 2.5. The ozone profiles were compared to a suite of correlative measurements from ground-based lidar and microwave, sondes, SAGE II and SAGE III (Stratospheric Aerosol and Gas Experiment). To correct for the expected Envisat pointing errors, which have not been corrected implicitly in either of the algorithms, we applied a constant altitude shift of −1.5 km to the SCIAMACHY ozone profiles. The IFE ozone profile data between 16 and 40 km are biased low by 3–6%. The average difference profiles show a characteristic zigzag shape with a wavelength of approximately 8 km. The standard deviation of the differences is typically 10% between 20 and 35 km. We show that more than 20% of the SCIAMACHY official ESA offline (OL) ozone profiles version 2.4 and 2.5 have unrealistic ozone values, most of these are north of 15° S. The remaining OL profiles compare well to correlative instruments above 24 km. Between 20 and 24 km, they underestimate ozone by 15±5%.
Atmospheric bromoform at Mace Head, Ireland: Evidence for a peatland source
Authors: Carpenter L. J. , Wevill D. J. , O’Doherty S. , Spain G. , Simmonds P. G. 
Published: April 2010

Abstract. In situ atmospheric observations of bromoform (CHBr3) made over a 2.5 year period at Mace Head, Ireland from May 2001–December 2003, including during the NAMBLEX (North Atlantic Marine Boundary Layer Experiment) campaign, show broad maxima from spring until autumn and winter minima, with mixing ratios of 5.3+1.0 pptv (mid March–mid October) and 1.8+0.8 pptv (December–February). This indicates that, unlike CHCl3, which has a summer minimum and winter maximum at Mace Head, local biological sources of CHBr3 have a greater influence on the atmospheric data than photochemical decay during long-range transport. The emission sources are predominantly macroalgal, but we find evidence for a small terrestrial flux from peatland ecosystems, which so far has not been accounted for in the CHBr3 budget. Sharp increases in CHCl3 and CHBr3 concentrations and decreases in O3 concentrations occurred at night when the wind direction switched from an ocean- to a land-based sector (land breeze) and the wind speed dropped to below 5 ms−1. These observations infer a shallow atmospheric boundary layer with increased O3 deposition and concentration of local emissions of both CHCl3 and CHBr3. The ratio of ΔCHCl3/ΔCHBr3 varied strongly according to the prevailing wind direction; from 0.6+0.1 in south-easterly (100–170°) air to 1.9+0.8 in north-easterly (40–70°) air. Of these land-sectors, the south-easterly air masses are likely to be strongly influenced by macroalgal beds along the coast and the emission ratios probably reflect those from seaweeds in addition to land sources. The north-easterly airmasses however have a fetch predominantly over land, which locally is comprised of coastal peatland ecosystems (peat bogs and coastal conifer plantations), previously identified as being strong sources of atmospheric CHCl3 under these conditions. Although we cannot entirely rule out other local land or coastal sources, our observations also suggest peatland ecosystem emissions of CHBr3. We use correlations between CHCl3 and CHBr3 during the land breeze events in conjunction with previous estimates of local wetland CHCl3 release to tentatively deduce a global wetland CHBr3 source of 26.9 (0.5–1247) Gg yr−1, which is approximately 10% of the total global source.
Mobile laboratory measurements of black carbon, polycyclic aromatic hydrocarbons and other vehicle emissions in Mexico City
Authors: Jiang M. , Marr L. C. , Dunlea E. J. , Herndon S. C. , Jayne J. T. , Kolb C. E. , Knighton W. B. , Rogers T. M. , Zavala M. , Molina L. T. , Molina M. J. 
Published: April 2010

Abstract. Black carbon (BC) and polycyclic aromatic hydrocarbons (PAHs) are of concern due to their effects on climate and health. The main goal of this research is to provide the first estimate of emissions of BC and particle-phase PAHs (PPAHs) from motor vehicles in Mexico City. The emissions of other pollutants including carbon monoxide (CO), oxides of nitrogen (NOx), volatile organic compounds (VOCs), and particulate matter of diameter 2.5 µm and less (PM2.5) are also estimated. As a part of the Mexico City Metropolitan Area field campaign in April 2003 (MCMA-2003), a mobile laboratory was driven throughout the city. The laboratory was equipped with a comprehensive suite of gas and particle analyzers, including an aethalometer that measured BC and a photoionization aerosol sensor that measured PPAHs. While driving through traffic, the mobile lab is continuously sampling exhaust plumes from the vehicles around it. We have developed a method of automatically identifying exhaust plumes, which are then used as the basis for calculation of fleet-average emission factors. In the approximately 75 h of on-road sampling during the field campaign, we have identified ~30 000 exhaust measurement points that represent a variety of vehicle types and driving conditions. The large sample provides a basis for estimating fleet-average emission factors and thus the emission inventory. Motor vehicles in the Mexico City area are estimated to emit 1700±200 metric tons BC, 57±6 tons PPAHs, 1 190 000±40 000 tons CO, 120 000±3000 tons NOx, 202 000±4000 tons VOCs, and 4400±400 tons PM2.5 per year, not including cold start emissions. The estimates for CO, NOx, and PPAHs may be low by up to 10% due to the slower response time of analyzers used to measure these species. Compared to the government's official motor vehicle emission inventory for the year 2002, the estimates for CO, NOx, VOCs, and PM2.5 are 38% lower, 23% lower, 7% higher, and 26% higher, respectively. The distributions of emission factors of BC, PPAHs, and PM2.5 are highly skewed, i.e. asymmetric, while those for benzene, measured as a surrogate for total VOCs, and NOx are less skewed. As a result, the total emissions of BC, PPAHs, and PM2.5 could be reduced by approximately 50% if the highest 20% of data points were removed, but ''super polluters'' are less influential on overall NOx and VOC emissions.
Overview of SCIAMACHY validation: 2002–2004
Authors: Piters A. J. M. , Bramstedt K. , Lambert J.-C. , Kirchhoff B. 
Published: April 2010

Abstract. SCIAMACHY, on board Envisat, is now in operation for almost three years. This UV/visible/NIR spectrometer measures the solar irradiance, the earthshine radiance scattered at nadir and from the limb, and the attenuation of solar radiation by the atmosphere during sunrise and sunset, from 240 to 2380 nm and at moderate spectral resolution. Vertical columns and profiles of a variety of atmospheric constituents are inferred from the SCIAMACHY radiometric measurements by dedicated retrieval algorithms. With the support of ESA and several international partners, a methodical SCIAMACHY validation programme has been developed jointly by Germany, the Netherlands and Belgium (the three instrument providing countries) to face complex requirements in terms of measured species, altitude range, spatial and temporal scales, geophysical states and intended scientific applications. This summary paper describes the approach adopted to address those requirements. The actual validation of the operational SCIAMACHY processors established at DLR on behalf of ESA has been hampered by data distribution and processor problems. Since first data releases in summer 2002, operational processors were upgraded regularly and some data products – level-1b spectra, level-2 O3, NO2, BrO and clouds data – have improved significantly. Validation results summarised in this paper conclude that for limited periods and geographical domains they can already be used for atmospheric research. Nevertheless, remaining processor problems cause major errors preventing from scientific usability in other periods and domains. Untied to the constraints of operational processing, seven scientific institutes (BIRA-IASB, IFE, IUP-Heidelberg, KNMI, MPI, SAO and SRON) have developed their own retrieval algorithms and generated SCIAMACHY data products, together addressing nearly all targeted constituents. Most of the UV-visible data products (both columns and profiles) already have acceptable, if not excellent, quality. Several near-infrared column products are still in development but they have already demonstrated their potential for a variety of applications. In any case, scientific users are advised to read carefully validation reports before using the data. It is required and anticipated that SCIAMACHY validation will continue throughout instrument lifetime and beyond. The actual amount of work will obviously depend on funding considerations.
Simulating regional scale secondary organic aerosol formation during the TORCH 2003 campaign in the southern UK
Authors: Johnson D. , Utembe S. R. , Jenkin M. E. , Derwent R. G. , Hayman G. D. , Alfarra M. R. , Coe H. , McFiggans G. 
Published: April 2010

Abstract. A photochemical trajectory model has been used to simulate the chemical evolution of air masses arriving at the TORCH field campaign site in the southern UK during late July and August 2003, a period which included a widespread and prolonged photochemical pollution episode. The model incorporates speciated emissions of 124 non-methane anthropogenic VOC and three representative biogenic VOC, coupled with a comprehensive description of the chemistry of their degradation. A representation of the gas/aerosol absorptive partitioning of ca. 2000 oxygenated organic species generated in the Master Chemical Mechanism (MCM v3.1) has been developed and implemented, allowing simulation of the contribution to organic aerosol (OA) made by semi- and non-volatile products of VOC oxidation; emissions of primary organic aerosol (POA) and elemental carbon (EC) are also represented. Simulations of total OA mass concentrations in nine case study events (optimised by comparison with observed mass loadings derived from aerosol mass spectrometry measurements) imply that the OA can be ascribed to three general sources: (i) POA emissions; (ii) a ubiquitous background concentration of 0.7 µg m−3; and (iii) gas-to-aerosol transfer of lower volatility products of VOC oxidation generated by the regional scale processing of emitted VOC, but with all partitioning coefficients increased by a species-independent factor of 500. The requirement to scale the partitioning coefficients, and the implied background concentration, are both indicative of the occurrence of chemical processes within the aerosol which allow the oxidised organic species to react by association and/or accretion reactions which generate even lower volatility products, leading to a persistent, non-volatile secondary organic aerosol (SOA). The contribution of secondary organic material to the simulated OA results in significant elevations in the simulated ratio of organic carbon (OC) to EC, compared with the ratio of 1.1 assigned to the emitted components. For the selected case study events, [OC]/[EC] is calculated to lie in the range 2.7–9.8, values which are comparable with the high end of the range reported in the literature.
Interannual variation patterns of total ozone and temperature in observations and model simulations
Authors: Steinbrecht W. , Haßler B. , Brühl C. , Dameris M. , Giorgetta M. A. , Grewe V. , Manzini E. , Matthes S. , Schnadt C. , Steil B. , Winkler P. 
Published: April 2010

Abstract. We report results from a multiple linear regression analysis of long-term total ozone observations (1979 to 2002, by TOMS/SBUV), of temperature reanalyses (1958 to 2002, NCEP), and of two chemistry-climate model simulations (1960 to 1999, by ECHAM4.L39(DLR)/CHEM (=E39/C), and MAECHAM4-CHEM). The model runs are transient experiments, where observed sea surface temperatures, increasing source gas concentrations (CO2, CFCs, CH4, N2O, NOx), 11-year solar cycle, volcanic aerosols and the quasi-biennial oscillation (QBO) are all accounted for. MAECHAM4-CHEM covers the atmosphere from the surface up to 0.01 hPa (≈80 km). For a proper representation of middle atmosphere (MA) dynamics, it includes a parametrization for momentum deposition by dissipating gravity wave spectra. E39/C, on the other hand, has its top layer centered at 10 hPa (≈30 km). It is targeted on processes near the tropopause, and has more levels in this region. Both models reproduce the observed amplitudes and much of the observed low-latitude patterns of the various modes of interannual variability, MAECHAM4-CHEM somewhat better than E39/C. Total ozone and lower stratospheric temperature show similar patterns. Main contributions to the interannual variations of total ozone and lower stratospheric temperature at 50 hPa come from a linear trend (up to −30 Dobson Units (DU) per decade, or −1.5 K/decade), the QBO (up to 25 DU, or 2.5 K peak to peak), the intensity of the polar vortices (up to 50 DU, or 5 K peak to peak), and from tropospheric weather (up to 30 DU, or 3 K peak to peak). Smaller variations are related to the 11-year solar cycle (generally less than 25 DU, or 2.5 K), and to ENSO (up to 15 DU, or 1.5 K). Volcanic eruptions have resulted in sporadic changes (up to −40 DU, or +3 K). Most stratospheric variations are connected to the troposphere, both in observations and simulations. At low latitudes, patterns are zonally symmetric. At higher latitudes, however, strong, zonally non-symmetric signals are found close to the Aleutian Islands or south of Australia. Such asymmetric features appear in the model runs as well, but often at different longitudes than in the observations. The results point to a key role of the zonally asymmetric Aleutian (or Australian) stratospheric anti-cyclones for interannual variations at high- latitudes, and for coupling between polar vortex strength, QBO, 11-year solar cycle and ENSO.
Boundary layer concentrations and landscape scale emissions of volatile organic compounds in early spring
Authors: Haapanala S. , Rinne J. , Hakola H. , Hellén H. , Laakso L. , Lihavainen H. , Janson R. , Kulmala M. 
Published: April 2010

Abstract. Boundary layer concenrations of several volatile organic compounds (VOC) were measured during two campaigns in springs of 2003 and 2006. Measurements were conducted over boreal forests near SMEAR II measurement station in Hyytiälä, Southern Finland. In 2003 the measuremens were performed using light aircraft and in 2006 using hot air ballon. Isoprene concentrarions were low, usually below detection limit. This is explained by low biogenic production due to cold weather. Monoterpenes were observed frequently. Average total monoterpene concentration in the boundary layer was 33 pptv. Many anthropogenic compounds e.g. benzene, xylene and toluene, were observed in high amounts. Ecosystem scale surface emissions were estimated using simple mixed box budget methodology. Total monoterpene fluxes varied up to 80 μg m−2 h−1, α-pinene contributing typically more than two thirds of that. Highest fluxes of anthropogenic compounds were those of p/m xylene.
Connections between atmospheric sulphuric acid and new particle formation during QUEST III–IV campaigns in Heidelberg and Hyytiälä
Authors: Riipinen I. , Sihto S.-L. , Kulmala M. , Arnold F. , Dal Maso M. , Birmili W. , Saarnio K. , Teinilä K. , Kerminen V.-M. , Laaksonen A. , Lehtinen K. E. J. 
Published: April 2010

Abstract. This study investigates the connections between atmospheric sulphuric acid and new particle formation during QUEST III and BACCI/QUEST IV campaigns. The campaigns have been conducted in Heidelberg (2004) and Hyytiälä (2005), the first representing a polluted site surrounded by deciduous forest, and the second a rural site in a boreal forest environment. We have studied the role of sulphuric acid in particle formation and growth by determining 1) the power-law dependencies between sulphuric acid ([H2SO4]), and particle concentrations (N3–6) or formation rates at 1 nm and 3 nm (J1 and J3; 2) the time delays between [H2SO4] and N3–6 or J3, and the growth rates for 1–3 nm particles; 3) the empirical nucleation coefficients A and K in relations J1=A[H2SO4] and J1=K[H2SO4]2, respectively; 4) theoretical predictions for J1 and J3 for the days when no significant particle formation is observed, based on the observed sulphuric acid concentrations and condensation sinks. In both environments, N3–6 or J3 and [H2SO4] were linked via a power-law relation with exponents typically ranging from 1 to 2. The result suggests that the cluster activation theory and kinetic nucleation have the potential to explain the observed particle formation. However, some differences between the sites existed: The 1–3 nm growth rates were slightly higher and the nucleation coefficients about an order of magnitude greater in Heidelberg than in Hyytiälä conditions. The time lags between J3 and [H2SO4] were consistently lower than the corresponding delays between N3–6 and [H2SO4]. The exponents in the J3∝[H2SO4]nJ3-connection were consistently higher than or equal to the exponents in the relation N3–6∝[H2SO4]nN36. In the J1 values, no significant differences were found between the observed rates on particle formation event days and the predictions on non-event days. The J3 values predicted by the cluster activation or kinetic nucleation hypotheses, on the other hand, were considerably lower on non-event days than the rates observed on particle formation event days. This study provides clear evidence implying that the main process limiting the observable particle formation is the competition between the growth of the freshly formed particles and their loss by scavenging, rather than the initial particle production by nucleation of sulphuric acid. In general, it can be concluded that the simple models based on sulphuric acid concentrations and particle formation by cluster activation or kinetic nucleation can predict the occurence of atmospheric particle formation and growth well, if the particle scavenging is accurately accounted for.
Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone
Authors: Sauvage B. , Martin R. V. , van Donkelaar A. , Liu X. , Chance K. , Jaeglé L. , Palmer P. I. , Wu S. , Fu T.-M. 
Published: April 2010

Abstract. We use a global chemical transport model (GEOS-Chem) to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flash counts improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 5±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils) and VOCs (biomass burning). The top-down biomass burning inventory is larger by a factor of 2 for HCHO and alkenes, and by 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4) is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv due to enhanced convective detrainment in the upper troposphere. Heterogeneous uptake of HNO3 on aerosols reduces simulated O3 by 5–7 ppbv, reducing a model bias versus in situ observations over and downwind of deserts. Exclusion of HO2 uptake on aerosols improves O3 by 5 ppbv in biomass burning regions.