ALBERT

Description: Reactive nitrogen (N r ) is an essential nutrient to plants and a limiting element for growth in many ecosystems, but it can have harmful effects on ecosystems when in excess. Satellite-derived surface observations are used together with a dry deposition model to estimate the dry deposition flux of the most abundant short-lived nitrogen species, NH 3 and NO 2 , over North America during the 2013 warm season. These fluxes demonstrate that the NH 3 contribution dominates over NO 2 for most regions (comprising ~85% of their sum in Canada and ~65% in the U.S.), with some regional exceptions (e.g. Alberta and northeastern U.S.). Nationwide, ~51 t of N from these species were dry deposited in the U.S., approximately double the ~28 t in Canada over this period. Forest fires are shown to be the major contributor of dry deposition of N r from NH 3 in northern latitudes, leading to deposition fluxes 2–3 times greater than from expected amounts without fires. ©2017. Her Majesty the Queen in Right of Canada. Reproduced with the permission of the Minister of the Environment.

Description: The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Water vapour (H2O), one of the most important molecules for climate and atmospheric chemistry, is one of the key species provided by the two principal instruments, the infrared Fourier Transform Spectrometer (ACE-FTS) and the MAESTRO UV-Visible spectrometer (ACE-MAESTRO). The first instrument performs measurements on several lines in the 1362–2137 cm−1 range, from which vertically resolved H2O concentration profiles are retrieved, from 7 to 90 km altitude. ACE-MAESTRO measures profiles using the water absorption band in the near infrared part of the spectrum at 926.0–969.7 nm. This paper presents a comprehensive validation of the ACE-FTS profiles. We have compared the H2O volume mixing ratio profiles with space-borne (SAGE II, HALOE, POAM III, MIPAS, SMR) observations and measurements from balloon-borne frostpoint hygrometers and a ground based lidar. We show that the ACE-FTS measurements provide H2O profiles with small retrieval uncertainties in the stratosphere (better than 5% from 15 to 70 km, gradually increasing above). The situation is unclear in the upper troposphere, due mainly to the high variability of the water vapour volume mixing ratio in this region. A new water vapour data product from the ACE-MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) is also presented and initial comparisons with ACE-FTS are discussed.

Description: We investigate the effect of using three different cross section data sets on ozone profile retrievals from Global Ozone Monitoring Experiment (GOME) ultraviolet measurements (289–307 nm, 326–337 nm). These include Bass-Paur, Brion, and GOME flight model cross sections (references below). Using different cross sections can significantly affect the retrievals, by up to 12 Dobson Units (DU, 1 DU=2.69×1016 molecules cm−2) in total column ozone, up to 10 DU in tropospheric column ozone, and up to 100% in retrieved ozone values for individual atmospheric layers. Compared to using the Bass-Paur and GOME flight model cross sections, using the Brion cross sections not only reduces fitting residuals by 15–60% in the Huggins bands, but also improves retrievals, especially in the troposphere, as seen from validation against ozonesonde measurements. Therefore, we recommend using the Brion cross section for ozone profile retrievals from ultraviolet measurements. The total column ozone retrieved using the GOME flight model cross sections is systematically lower, by 7–10 DU, than that retrieved using the Brion and Bass-Paur cross sections and is also systematically lower than Total Ozone Mapping Spectrometer (TOMS) observations. This study demonstrates the need for improved ozone cross section measurements in the ultraviolet to improve profile retrievals of this key atmospheric constituent.

Description: The purpose of this study is to perform a global search of the upper troposphere (z≥10 km) for enhancements of nitrogen dioxide and determine their sources. This is the first application of satellite-based limb scattering to study upper tropospheric NO2. We have searched two years (May 2003–May 2005) of OSIRIS (Optical Spectrograph and Infrared Imager System) operational NO2 concentrations (version 2.3/2.4) to find large enhancements in the observations by comparing with photochemical box model calculations and by identifying local maxima in NO2 volume mixing ratio. We find that lightning is the main production mechanism responsible for the large enhancements in OSIRIS NO2 observations as expected. Similar patterns in the abundances and spatial distribution of the NO2 enhancements are obtained by perturbing the lightning within the GEOS-Chem 3-dimensional chemical transport model. In most cases, the presence of lightning is confirmed with coincident imagery from LIS (Lightning Imaging Sensor) and the spatial extent of the NO2 enhancement is mapped using nadir observations of tropospheric NO2 at high spatial resolution from SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric Chartography) and OMI (Ozone Monitoring Instrument). The combination of the lightning and chemical sensors allows us to investigate globally the role of lightning to the abundance of NO2 in the upper troposphere (UT). Lightning contributes 60% of the tropical upper tropospheric NO2 in GEOS-Chem simulations. The spatial and temporal distribution of NO2 enhancements from lightning (May 2003–May 2005) is investigated. The enhancements generally occur at 12 to 13 km more frequently than at 10 to 11 km. This is consistent with the notion that most of the NO2 is forming and persisting near the cloud top altitude in the tropical upper troposphere. The latitudinal distribution is mostly as expected. In general, the thunderstorms exhibiting weaker vertical development (e.g. 11≤z≤13 km) extend latitudinally as far poleward as 45° but the thunderstorms with stronger vertical development (z≥14 km) tend to be located within 33° of the equator. There is also the expected hemispheric asymmetry in the frequency of the NO2 enhancements, as most were observed in the northern hemisphere for the period analyzed.

Description: A global three-dimensional (i.e. latitude, longitude, altitude) climatology of tropospheric ozone is derived from the ozone sounding record by trajectory mapping. Approximately 52 000 ozonesonde profiles from more than 100 stations worldwide since 1965 are used. The small number of stations results in a sparse geographical distribution. Here, forward and backward trajectory calculations are performed for each sounding to map ozone measurements to a number of other locations, and so to fill in the spatial domain. This is possible because the lifetime of ozone in the troposphere is of the order of weeks. This physically based interpolation method offers obvious advantages over typical statistical interpolation methods. The trajectory-mapped ozone values show reasonable agreement, where they overlap, to the actual soundings, and the patterns produced separately by forward and backward trajectory calculations are similar. Major regional features of the tropospheric ozone distribution are clearly evident in the global maps. An interpolation algorithm based on spherical functions is further used for smoothing and to fill in remaining data gaps. The resulting three-dimensional global tropospheric ozone climatology facilitates visualization and comparison of different years, decades, and seasons, and offers some intriguing insights into the global variation of tropospheric ozone. It will be useful for climate and air quality model initialization and validation, and as an a priori climatology for satellite data retrievals. Further division of the climatology into decadal and annual averages can provide a global view of tropospheric ozone changes, although uncertainties with regard to the performance of older sonde types, as well as more recent variations in operating procedures, need to be taken into account.

Description: For the first time, results of four stratospheric BrO profiling instruments, are presented and compared with reference to the SLIMCAT 3-dimensional chemical transport model (3-D CTM). Model calculations are used to infer a BrO profile validation set, measured by 3 different balloon sensors, for the new Envisat/SCIAMACHY (ENVIronment SATellite/SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) satellite instrument. The balloon observations include (a) balloon-borne in situ resonance fluorescence detection of BrO (Triple), (b) balloon-borne solar occultation DOAS measurements (Differential Optical Absorption Spectroscopy) of BrO in the UV, and (c) BrO profiling from the solar occultation SAOZ (Systeme d'Analyse par Observation Zenithale) balloon instrument. Since stratospheric BrO is subject to considerable diurnal variation and none of the measurements are performed close enough in time and space for a direct comparison, all balloon observations are considered with reference to outputs from the 3-D CTM. The referencing is performed by forward and backward air mass trajectory calculations to match the balloon with the satellite observations. The diurnal variation of BrO is considered by 1-D photochemical model calculation along the trajectories. The 1-D photochemical model is initialised with output data of the 3-D model with additional constraints on the vertical transport, the total amount and photochemistry of stratospheric bromine as given by the various balloon observations. Total [Bry]=(20.1±2.5) pptv obtained from DOAS BrO observations at mid-latitudes in 2003, serves as an upper limit of the comparison. Most of the balloon observations agree with the photochemical model predictions within their given error estimates. First retrieval exercises of BrO limb profiling from the SCIAMACHY satellite instrument on average agree to around 20% with the photochemically-corrected balloon observations of the remote sensing instruments (SAOZ and DOAS). An exception is the in situ Triple profile, in which the balloon and satellite data mostly does not agree within the given errors. In general, the satellite measurements show systematically higher values below 25 km than the balloon data and a change in profile shape above about 25 km.

Description: Stratospheric O3 and NO2 abundances measured by different remote sensing instruments are inter-compared: (1) Line-of-sight absorptions and vertical profiles inferred from solar spectra in the ultra-violet (UV), visible and infrared (IR) wavelength ranges measured by the LPMA/DOAS (Limb Profile Monitor of the Atmosphere/Differential Optical Absorption Spectroscopy) balloon payload during balloon ascent/descent and solar occultation are examined with respect to internal consistency. (2) The balloon borne stratospheric profiles of O3 and NO2 are compared to collocated space-borne skylight limb observations of the Envisat/SCIAMACHY satellite instrument. The trace gas profiles are retrieved from SCIAMACHY spectra using different algorithms developed at the Universities of Bremen and Heidelberg and at the Harvard-Smithsonian Center for Astrophysics. A comparison scheme is used that accounts for the spatial and temporal mismatch as well as differing photochemical conditions between the balloon and satellite borne measurements. It is found that the balloon borne measurements internally agree to within ±10% and ±20% for O3 and NO2, respectively, whereas the agreement with the satellite is ±20% for both gases in the 20 km to 30 km altitude range and in general worse below 20 km.

Description: Episodes of high bromine levels and surface ozone depletion in the springtime Arctic are simulated by an online air-quality model, GEM-AQ, with gas-phase and heterogeneous reactions of inorganic bromine species and a simple scheme of air-snowpack chemical interactions implemented for this study. Snowpack on sea ice is assumed to be the only source of bromine to the atmosphere and to be capable of converting relatively stable bromine species to photolabile Br2 via air-snowpack interactions. A set of sensitivity model runs are performed for April 2001 at a horizontal resolution of approximately 100 km×100 km in the Arctic, to provide insights into the effects of temperature and the age (first-year, FY, versus multi-year, MY) of sea ice on the release of reactive bromine to the atmosphere. The model simulations capture much of the temporal variations in surface ozone mixing ratios as observed at stations in the high Arctic and the synoptic-scale evolution of areas with enhanced BrO column amount ("BrO clouds") as estimated from satellite observations. The simulated "BrO clouds" are in modestly better agreement with the satellite measurements when the FY sea ice is assumed to be more efficient at releasing reactive bromine to the atmosphere than on the MY sea ice. Surface ozone data from coastal stations used in this study are not sufficient to evaluate unambiguously the difference between the FY sea ice and the MY sea ice as a source of bromine. The results strongly suggest that reactive bromine is released ubiquitously from the snow on the sea ice during the Arctic spring while the timing and location of the bromine release are largely controlled by meteorological factors. It appears that a rapid advection and an enhanced turbulent diffusion associated with strong boundary-layer winds drive transport and dispersion of ozone to the near-surface air over the sea ice, increasing the oxidation rate of bromide (Br−) in the surface snow. Also, if indeed the surface snowpack does supply most of the reactive bromine in the Arctic boundary layer, it appears to be capable of releasing reactive bromine at temperatures as high as −10 °C, particularly on the sea ice in the central and eastern Arctic Ocean. Dynamically-induced BrO column variability in the lowermost stratosphere appears to interfere with the use of satellite BrO column measurements for interpreting BrO variability in the lower troposphere but probably not to the extent of totally obscuring "BrO clouds" that originate from the surface snow/ice source of bromine in the high Arctic. A budget analysis of the simulated air-surface exchange of bromine compounds suggests that a "bromine explosion" occurs in the interstitial air of the snowpack and/or is accelerated by heterogeneous reactions on the surface of wind-blown snow in ambient air, both of which are not represented explicitly in our simple model but could have been approximated by a parameter adjustment for the yield of Br2 from the trigger.

Description: The calibration of SCIAMACHY was thoroughly checked since the instrument was launched on-board ENVISAT in February 2002. While SCIAMACHY's functional performance is excellent since launch, a number of technical difficulties have appeared, that required adjustments to the calibration. The problems can be separated into three types: (1) Those caused by the instrument and/or platform environment. Among these are the high water content in the satellite structure and/or MLI layer. This results in the deposition of ice on the detectors in channels 7 and 8 which seriously affects the retrievals in the IR, mostly because of the continuous change of the slit function caused by scattering of the light through the ice layer. Additionally a light leak in channel 7 severely hampers any retrieval from this channel. (2) Problems due to errors in the on-ground calibration and/or data processing affecting for example the radiometric calibration. A new approach based on a mixture of on-ground and in-flight data is shortly described here. (3) Problems caused by principal limitations of the calibration concept, e.g. the possible appearance of spectral structures after the polarisation correction due to unavoidable errors in the determination of atmospheric polarisation. In this paper we give a complete overview of the calibration and problems that still have to be solved. We will also give an indication of the effect of calibration problems on retrievals where possible. Since the operational processing chain is currently being updated and no newly processed data are available at this point in time, for some calibration issues only a rough estimate of the effect on Level 2 products can be given. However, it is the intention of this paper to serve as a future reference for detailed studies into specific calibration issues.

Description: We investigate the effect of using three different cross section data sets on ozone profile retrievals from Global Ozone Monitoring Experiment (GOME) ultraviolet measurements (289–307 nm, 326–337 nm). These include Bass-Paur, Brion, and GOME flight model cross sections (references below). Using different cross sections can significantly affect the retrievals, by up to 12 Dobson Units (DU, 1 DU=2.69×1016 molecules cm−2) in total column ozone, up to 10 DU in tropospheric column ozone, and up to 100% in retrieved ozone values for individual atmospheric layers. Compared to using the Bass-Paur and GOME flight model cross sections, using the Brion cross sections not only reduces fitting residuals by 15–60% in the Huggins bands, but also improves retrievals, especially in the troposphere, as seen from validation against ozonesonde measurements. Therefore, we recommend using the Brion cross section for ozone profile retrievals from ultraviolet measurements. The total column ozone retrieved using the GOME flight model cross sections is systematically lower, by 7–10 DU, than that retrieved using the Brion and Bass-Paur cross sections and is also systematically lower than Total Ozone Mapping Spectrometer (TOMS) observations. This study demonstrates the need for improved ozone cross section measurements in the ultraviolet to improve profile retrievals of this key atmospheric constituent.