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The Orbiting Carbon Observatory (OCO) mission will make the first global, space-based measurements of atmospheric carbon dioxide (CO 2 ) with the precision, resolution, and coverage needed to characterize CO 2 sources and sinks on regional scales. The measurement approach and instrument specifications were determined through an analysis of existing carbon cycle data and a series of observing system simulation experiments. During its 2-year mission, OCO will fly in a 1:15 PM sun-synchronous orbit with a 16-day ground-track repeat time, just ahead of the EOS Aqua platform. It will carry a single instrument that incorporates three bore-sighted high-resolution spectrometers designed to measure reflected sunlight in the 0.76-μm O 2 A-band and in the CO 2 bands at 1.61 and 2.06 μm. Soundings recorded in these three bands will be used to retrieve the column-averaged CO 2 dry air mole fraction (X CO2 ). A comprehensive validation program was included in the mission to ensure that the space-based X CO2 measurements have precisions of ∼0.3% (1 ppm) on regional scales. OCO measurements will be used in global synthesis inversion and data assimilation models to quantify CO 2 sources and sinks. While OCO will have a nominal lifetime of only 2 years, it will serve as a pathfinder for future long-term CO 2 monitoring missions. © 2004 COSPAR. Published by Elsevier Ltd. All rights reserved.

The Mapocho River's upper basin (Chilean Central Andes) was studied as a proxy of a high-mountainous hydrothermally-altered (HMHA) system comprised by three sub-basins developed over very different rocks and submitted to different anthropic pressure: 1) a natural acid rock drainage (i.e., Yerba Loca), 2) a creek with mining activity in its headwaters and hydrochemically classified as non-affected by acid mine drainage (i.e., San Francisco), and 3) a low metal concentration creek (i.e., Molina). In general terms, the geochemical composition of the clastic sediments was consistent with the geochemistry inferred from the mineralogical study. However, sediments with a smaller grain size showed higher concentrations than the bigger grain size counterparts for elements such as Fe, S, Cu and As. This behavior was particularly evident in the Yerba Loca basin and it was attributed to the seasonal appearance of Fe- and Al-rich precipitates as constituents of the finer sediments. Different methodologies for the calculation of geochemical backgrounds (Tukey's inner fence, TIF; Median + 2*Median Absolute Deviation, MAD; and 95th percentile) were tested. Results suggest that the 95th percentile-method was the most appropriate for this type of mountainous systems. Using the selected methodology, three different geochemical backgrounds were calculated: 1) Yerba Loca basin, 2) Molina basin, and 3) Mapocho Upper basin. When the generated background levels were compared with the Consensus-Based (CB) Sediment Quality Guidelines; Fe, Mn, Zn, Pb, Cu, Cr, Ni and As showed background values that were consistently higher than the values set by the CB Threshold Effect Concentration and, even higher than the CB Probable Effect Concentration for Fe (MUB Background : 6.78 wt% vs CB PEC: 4.00 wt%; and Cu (MUB Bacground : 3387 mg kg -1 vs CB PEC: 149 mg kg -1 ). The present study clearly states the paramount importance of having a solid geochemical background before any attempt of a sediment risk assessment is made at HMHA regions., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

After several decades' development of retrieval techniques in aerosol remote sensing, no fast and accurate analytical Radiative Transfer Model (RTM) has been developed and applied to create global aerosol products for non-polarimetric instruments such as Ocean and Land Colour Instrument/Sentinel-3 (OLCI/Sentinel-3) and Meteosat Second Generation/Spinning Enhanced Visible and Infrared Imager (MSG/SEVIRI). Global aerosol retrieval algorithms are typically based on a Look-Up-Table (LUT) technique, requiring high-performance computers. The current eXtensible Bremen Aerosol/cloud and surfacE parameters Retrieval (XBAER) algorithm also utilizes the LUT method. In order to have a near-real time retrieval and achieve a quick and accurate "FIRST-LOOK" aerosol product without high-demand of computing resource, we have developed a Fast and Accurate Semi-analytical Model of Atmosphere-surface Reflectance (FASMAR) for aerosol remote sensing. The FASMAR is developed based on a successive order of scattering technique. In FASMAR, the first three orders of scattering are calculated exactly. The contribution of higher orders of scattering is estimated using an extrapolation technique and an additional correction function. The evaluation of FASMAR has been performed by comparing with radiative transfer model SCIATRAN for all typical observation/illumination geometries, surface/aerosol conditions, and wavelengths 412, 550, 670, 870, 1600, 2100 nm used for aerosol remote sensing. The selected observation/illumination conditions are based on the observations from both geostationary satellite (e.g. MSG/SEVIRI) and polar-orbit satellite (e.g. OLCI/Sentinel-3). The percentage error of the top of atmosphere reflectance calculated by FASMAR is within  ± 3% for typical polar-orbit/geostationary satellites' observation/illumination geometries. The accuracy decreases for solar and viewing zenith angles larger than 70 ∘ . However, even in such cases, the error is within the range  ± 5%. The evaluation of model performance also shows that FASMAR can be used for all typical surfaces with albedo in the interval [ 0 - 1 ] and aerosol with optical thickness in the range [ 0.01 - 1 ] ., Competing Interests: The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (© 2020 Elsevier Ltd. All rights reserved.)

We investigate the distribution of volatile organic compounds (VOCs) over Indian subcontinent during a winter month of January 2011 combining the regional model WRF-Chem (Weather Research and Forecasting model coupled with Chemistry) with ground- and space-based observations and chemical reanalysis. WRF-Chem simulated VOCs are found to be comparable with ground-based observations over contrasting environments of the Indian subcontinent. WRF-Chem results reveal the elevated levels of VOCs (e. g. propane) over the Indo-Gangetic Plain (16 ppbv), followed by the Northeast region (9.1 ppbv) in comparison with other parts of the Indian subcontinent (1.3-8.2 ppbv). Higher relative abundances of propane (27-31%) and ethane (13-17%) are simulated across the Indian subcontinent. WRF-Chem simulated formaldehyde and glyoxal show the western coast, Eastern India and the Indo-Gangetic Plain as the regional hotspots, in a qualitative agreement with the MACC (Monitoring Atmospheric Composition and Climate) reanalysis and satellite-based observations. Lower values of R GF (ratio of glyoxal to formaldehyde <0.04) suggest dominant influences of the anthropogenic emissions on the distribution of VOCs over Indian subcontinent, except the northeastern region where higher R GF (∼0.06) indicates the role of biogenic emissions, in addition to anthropogenic emissions. Analysis of HCHO/NO 2 ratio shows a NO x -limited ozone production over India, with a NO x -to-VOC transition regime over central India and IGP. The study highlights a need to initiate in situ observations of VOCs over regional hotspots (Northeast, Central India, and the western coast) based on WRF-Chem results, where different satellite-based observations differ significantly., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Underwater light field characterization is of importance for understanding biogeochemical processes and heat budget of the global oceans, which are impacting and reacting to climate change. Vibrational Raman Scattering (VRS) was retrieved from backscattered radiances measured by three different hyperspectral satellite sensors, SCIAMACHY, GOME-2, and OMI, using Differential Optical Absorption Spectroscopy (DOAS). Diffuse attenuation coefficient (Kd) in the blue spectral range (390 to 426 nm) was derived from the VRS signal via a look-up-table established through ocean-atmosphere coupled radiative transfer modeling. We processed one year of data, representative of the overlapping period of optimal operation for all three sensors. Resulting data sets were evaluated by comparison with Kd at 490 nm from Ocean Colour Climate Change Initiative (OC-CCI) which was first converted to Kd at 390 to 426 nm. Good agreement with the OC-CCI Kd product was achieved for all three sensors when Kd was limited to below 0.15 m -1 . Differences among the hyperspectral sensors and to OC-CCI were attributed to particular instrumental effects on the DOAS retrieval leading to temporal and spatial biases. This is in addition to the fact that the spatial and temporal resolution of the hyperspectral sensors data differ among themselves and are much lower then for the OC-CCI Kd-product. Further corrections (e.g., empirical) are necessary before these data sets can be merged in order to obtain a long-term Kd product for the blue spectral range.

Currently, modeling studies tend to significantly underestimate observed space-based glyoxal (CHOCHO) vertical column densities (VCDs), implying the existence of missing sources of glyoxal. Several recent studies suggest that the emissions of aromatic compounds and molar yields of glyoxal in the chemical mechanisms may both be underestimated, which can affect the simulated glyoxal concentrations. In this study, the influences of these two factors on glyoxal amounts over China were investigated using the RAMS-CMAQ modeling system for January and July 2014. Four sensitivity simulations were performed, and the results were compared to satellite observations. These results demonstrated significant impacts on glyoxal concentrations from these two factors. In case 1, where the emissions of aromatic compounds were increased three-fold, improvements to glyoxal VCDs were seen in high anthropogenic emissions regions. In case 2, where molar yields of glyoxal from isoprene were increased five-fold, the resulted concentrations in July were 3-5-fold higher, achieving closer agreement between the modeled and measured glyoxal VCDs. The combined changes from both cases 1 and 2 were applied in case 3, and the model succeeded in further reducing the underestimations of glyoxal VCDs. However, the results over most of the regions with pronounced anthropogenic emissions were still underestimated. So the molar yields of glyoxal from anthropogenic precursors were considered in case 4. With these additional mole yield changes (a two-fold increase), the improved concentrations agreed better with the measurements in regions of the lower reaches of the Yangtze River and Yellow River in January but not in July., (Copyright © 2018. Published by Elsevier B.V.)

The MEdium Resolution Imaging Spectrometer (MERIS) instrument on board ESA Envisat made measurements from 2002 to 2012. Although MERIS was limited in spectral coverage, accurate Aerosol Optical Thickness (AOT) from MERIS data are retrieved by using appropriate additional information. We introduce a new AOT retrieval algorithm for MERIS over land surfaces, referred to as eXtensible Bremen AErosol Retrieval (XBAER). XBAER is similar to the "dark-target" (DT) retrieval algorithm used for Moderate-resolution Imaging Spectroradiometer (MODIS), in that it uses a lookup table (LUT) to match to satellite-observed reflectance and derive the AOT. Instead of a global parameterization of surface spectral reflectance, XBAER uses a set of spectral coefficients to prescribe surface properties. In this manner, XBAER is not limited to dark surfaces (vegetation) and retrieves AOT over bright surface (desert, semiarid, and urban areas). Preliminary validation of the MERIS-derived AOT and the ground-based Aerosol Robotic Network (AERONET) measurements yield good agreement, the resulting regression equation is y = (0.92 × ± 0.07) + (0.05 ± 0.01) and Pearson correlation coefficient of R = 0.78. Global monthly means of AOT have been compared from XBAER, MODIS and other satellite-derived datasets.

The SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) aboard the Envisat satellite provided measurements from August 2002 until April 2012. SCIAMACHY measured the scattered or direct sunlight using different observation geometries. The limb viewing geometry allows the retrieval of water vapour at about 10-25 km height from the near-infrared spectral range (1353-1410 nm). These data cover the upper troposphere and lower stratosphere (UTLS), a region in the atmosphere which is of special interest for a variety of dynamical and chemical processes as well as for the radiative forcing. Here, the latest data version of water vapour (V3.01) from SCIAMACHY limb measurements is presented and validated by comparisons with data sets from other satellite and in situ measurements. Considering retrieval tests and the results of these comparisons, the V3.01 data are reliable from about 11 to 23 km and the best results are found in the middle of the profiles between about 14 and 20 km. Above 20 km in the extra tropics V3.01 is drier than all other data sets. Additionally, for altitudes above about 19 km, the vertical resolution of the retrieved profile is not sufficient to resolve signals with a short vertical structure like the tape recorder. Below 14 km, SCIAMACHY water vapour V3.01 is wetter than most collocated data sets, but the high variability of water vapour in the troposphere complicates the comparison. For 14-20 km height, the expected errors from the retrieval and simulations and the mean differences to collocated data sets are usually smaller than 10 % when the resolution of the SCIAMACHY data is taken into account. In general, the temporal changes agree well with collocated data sets except for the Northern Hemisphere extratropical stratosphere, where larger differences are observed. This indicates a possible drift in V3.01 most probably caused by the incomplete treatment of volcanic aerosols in the retrieval. In all other regions a good temporal stability is shown. In the tropical stratosphere an increase in water vapour is found between 2002 and 2012, which is in agreement with other satellite data sets for overlapping time periods.

We report on the evolution of tropospheric nitrogen dioxide (NO2) over Spain, focusing on the densely populated cities of Barcelona, Bilbao, Madrid, Sevilla and Valencia, during 17 years, from 1996 to 2012. This data series combines observations from in-situ air quality monitoring networks and the satellite-based instruments GOME and SCIAMACHY. The results in these five cities show a smooth decrease in the NO2 concentrations of ~2% per year in the period 1996-2008, due to the implementation of emissions control environmental legislation, and a more abrupt descend of ~7% per year from 2008 to 2012 as a consequence of the economic recession. In the whole Spanish territory the NO2 levels have decreased by ~22% from 1996 to 2012. Statistical analysis of several economic indicators is used to investigate the different factors driving the NO2 concentration trends over Spain during the last two decades.

The atmospherically relevant chemistry generated by photolysis of I2/O3 mixtures has been studied at 298 K in the pressure range from 10 to 400 hPa by using a laboratory flash photolysis setup combining atomic resonance and molecular absorption spectroscopy. The temporal behaviors of I, I(2), IO, and OIO have been retrieved. Conventional kinetic methods and numerical modeling have been applied to investigate the IO self-reaction and the secondary chemistry. A pressure independent value of k(IO + IO) = (7.6 +/- 1.1) x 10(-11) cm(3) molecule-1 s(-1) has been determined. The pressure dependence of the branching ratios for the I + OIO and IOIO product channels in the IO + IO reaction have been determined and have values of 0.45 +/- 0.10 and 0.44 +/- 0.13 at 400 hPa, respectively. The branching ratios for the 2I + O(2) and I(2) + O(2) product channels are pressure independent with values of 0.09 +/- 0.06 and 0.05 +/- 0.03, respectively. The sensitivity analysis indicates that the isomer IOIO is more thermally stable than predicted by theoretical calculations. A reaction scheme comprising OIO polymerization steps has been shown to be consistent with the temporal behaviors recorded in this study. For simplicity, the rate coefficient has been assumed to be the same for each reaction (OIO)(n) + IO --> (OIO)(n+1), n = 1, 2, 3, 4. The lower limit obtained for this rate coefficient is (1.2 +/- 0.3) x 10(-10) cm(3) molecule(-1) s(-1) at 400 hPa. Evidence for the participation of IO in the polymerization mechanism also has been found. The rate coefficient for IO attachment to OIO and to small polymers has been determined to be larger than (5 +/- 2) x 10(-11) cm(3) molecule(-1) s(-1) at 400 hPa. These results provide supporting evidence for atmospheric particle formation induced by polymerization of iodine oxides.

The Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) onboard the European Envisat spacecraft performs continuous spectral observations of reflected, scattered and transmitted sunlight in various observation geometries. A unique feature of SCIAMACHY is the capability of probing the atmosphere in three different observation geometries:The nadir, limb, and occultation measurement modes. In nadir mode, column densities of trace gases are retrieved with a spatial resolution of typically 30 x 60 km using the Differential Optical Absorption Spectroscopy (DOAS) technique (Platt and Perner, 1983). Alternating with the nadir measurement, vertical profiles of absorber concentration in the stratosphere are derived in limb and occultation. In this paper we present an overview over some applications of SCIAMACHY data in space-based monitoring of atmospheric pollution. The DOAS algorithms for the retrieval of total column amounts from nadir spectra are briefly described and case studies of pollution events are presented. We also illustrate the technique used to derive stratospheric concentration profiles from limb observations and show comparisons with other remote sensing systems. Special emphasis will be given to techniques, which take advantage of SCIAMACHY's different viewing geometries. In particular, we will discuss the potential and limits of strategies to infer tropospheric abundances of O3 and NO2.

Optical multichannel detectors like photodiode arrays or CCD cameras combined with grating spectrometers are commonly used as detection systems in quantitative absorption spectroscopy. As a trade-off to broad spectral coverage, banded spectral features are sometimes recorded with insufficient spectral resolution and/or insufficiently fine detector binning. This renders the true physical spectrum of recorded intensities changed by instrumental and spectrum specific artefacts thus impeding comparability between results from different set-ups. In this work, it is demonstrated that in the case of a "well-behaved"--i.e. free of ro-vibronic structure--absorption band like the iodine monoxide IO(4<--0) transition, these effects can easily change the apparent peak absorption by up to 50%. Also deviations from the strict linearity (Beer-Lambert's law) between absorber concentration and apparent, i.e. pixelwise optical density occur. This can be critical in studies of chemical kinetics. It is shown that the observed non-linearity can cause errors of up to 50% in the determination of a second order rate coefficient for the IO self reaction. To overcome the problem, a consistent and rigorous integral approach for the treatment of intensity recordings is developed. Linearity between optical density and absorber concentration thereby is re-established. The method is validated using artificial test data as well as experimental data of the IO(4<--0) absorption transition, obtained in the context of I2/O3 photochemistry studies. The agreement is accurate to within +/-2% (test data) and +/-3% (experimental data) supporting the validity of the approach. Possible consequences for other spectroscopic work are indicated.

Emissions from fossil fuel combustion and biomass burning reduce local air quality and affect global tropospheric chemistry. Nitrogen oxides are emitted by all combustion processes and play a key part in the photochemically induced catalytic production of ozone, which results in summer smog and has increased levels of tropospheric ozone globally. Release of nitrogen oxide also results in nitric acid deposition, and--at least locally--increases radiative forcing effects due to the absorption of downward propagating visible light. Nitrogen oxide concentrations in many industrialized countries are expected to decrease, but rapid economic development has the potential to increase significantly the emissions of nitrogen oxides in parts of Asia. Here we present the tropospheric column amounts of nitrogen dioxide retrieved from two satellite instruments GOME and SCIAMACHY over the years 1996-2004. We find substantial reductions in nitrogen dioxide concentrations over some areas of Europe and the USA, but a highly significant increase of about 50 per cent-with an accelerating trend in annual growth rate-over the industrial areas of China, more than recent bottom-up inventories suggest.

By the utilization of a new laboratory method to synthesize OBrO employing an electric discharge, the visible absorption spectrum of gaseous OBrO has been investigated. Absorption spectra of OBrO have been recorded at 298 K, using a continuous-scan Fourier transform spectrometer at a spectral resolution of 0.8 cm(-1). A detailed vibrational and rotational analysis of the observed transitions has been carried out. The FTS measurements provide experimental evidence that the visible absorption spectrum of OBrO results from the electronic transition C(2A2)-X(2B1). Vibrational constants have been determined for the C(2A2) state (omega(1) = 648.3 +/- 1.9 cm(-1) and omega 2 = 212.8 +/- 1.2 cm(-1)) and for the X(2B1) state (omega 1 = 804.1 +/- 0.8 cm(-1) and omega 2 = 312.2 +/- 0.5 cm(-1)). The vibrational bands (1,0,0), (2,0,0), and (1,1,0) show rotational structure, whereas the other observed bands are unstructured because of strong predissociation. Rotational constants have been determined experimentally for the upper electronic state C(2A2). By modeling the band contours, predissociation lifetimes have been estimated. Further, an estimate for the absorption cross-section of OBrO has been made by assessing the bromine budget within the gas mixture, and atmospheric lifetimes of OBrO have been calculated using a photochemical model.

A new lightweight near-infrared tunable diode laser spectrometer CHILD (Compact High-altitude In-situ Laser Diode spectrometer) was developed for flights to the stratosphere as an additional in situ sensor on existing balloonborne payloads. Free-air absorption measurements in the near infrared are made with an open-path Herriott cell with new design features. It offers two individual absorption path lengths optimized for CH4 with 74 m (136 pass) and H2O with 36 m (66 pass). New electronic features include a real-time gain control loop that provides an autocalibration function. In flight-ready configuration the instrument mass is approximately 20 kg, including batteries. It successfully measured stratospheric CH4 and H2O profiles on high-altitude balloons on four balloon campaigns (Environmental Satellite validation) between October 2001 and June 2003. On these first flights, in situ spectra were recorded from ground level to 32,000-m altitude with a sensitivity of 0.1 ppm [(parts per million), ground] to 0.4 ppm (32,000 m) for methane and 0.15-0.5 ppm for water.

Retrievals of trace gas columns from the measurements of backscattered radiation by GOME (Global Ozone Monitoring Experiment) show that enhanced tropospheric columns of ozone (O3), nitrogen dioxide (NO2) and formaldehyde (HCHO), over the African continent occur frequently. This study focuses on the behaviour of trace gases over Africa in September 1997, a period impacted by the strongest known El Niño phase of the ENSO. It investigates our qualitative and quantitative understanding of the retrieved tropospheric trace gas column densities. The emissions of NOx and volatile organic compounds (VOC) from biomass burning, biogenic sources and lightning and their photochemical transformation have been investigated. By performing a trajectory analysis, the transport of air masses from the different emission regions was analysed and the potential atmospheric spatial distribution determined. BRemen's Atmospheric PHOtochemical model (BRAPHO) was applied to compute the chemistry along a large number of trajectories. From these results, tropospheric column amounts of O3, NO2 and HCHO were derived. Tropospheric trace gas columns retrieved from GOME measurements and those calculated are in reasonable agreement. Their general spatial extent was similar in the lower troposphere but the modeled trace gas columns in the upper troposphere were located south of the retrieved columns. We attribute this behaviour to uncertainties in the ERA-40 meteorological data in the upper troposphere. The significance of biomass burning and of biogenic emissions with respect to HCHO columns over Africa was investigated. The analysis reveals that the total amounts of HCHO generated over Africa during September 1997 as a result of biomass burning and biogenic emissions are similar. However the HCHO from biogenic sources has the highest specific columns and these are located close to their source. In comparison the HCHO from biomass burning is predicted to be produced and transported over a much wider area. Overall all the emission processes mix together to produce the plume of O3.

The separation of overlapping absorption spectra in the context of multichannel time-resolved absorption spectroscopy and chemical kinetics is a particular case in the general problem of splitting the observed data into several linear components. Here, principal and independent components analysis are applied to kinetic data of iodine--ozone chemistry, which contains overlapping spectra of different absorbers. The objective of this work is to demonstrate a method which in spite of this overlap is able to extract separated time traces of such absorbers. These time traces are clearly a pre-requisite for any further accurate quantitative analysis. The statistical properties of data recordings obtained from flash photolysis of I(2) and O(3) have been studied to check if the requirements of the model are fulfilled. Results of separation in appropriate spectral windows displaying overlapped vibrational features are presented. Validation is made using prior information and conventional techniques.

A recent development in ground-based remote sensing of atmospheric constituents by UV-visible absorption measurements of scattered light is the simultaneous use of several horizon viewing directions in addition to the traditional zenith-sky pointing. The different light paths through the atmosphere enable the vertical distribution of some atmospheric absorbers, such as NO2, BrO, or O3, to be retrieved. This approach has recently been implemented on an airborne platform. This novel instrument, the airborne multiaxis differential optical absorption spectrometer (AMAXDOAS), has been flown for the first time. In this study, the amount of profile information that can be retrieved from such measurements is investigated for the trace gas NO2. Sensitivity studies on synthetic data are performed for a variety of representative measurement conditions including two wavelengths, one in the UV and one in the visible, two different surface spectral reflectances, various lines of sight (LOSs), and for two different flight altitudes. The results demonstrate that the AMAXDOAS measurements contain useful profile information, mainly at flight altitude and below the aircraft. Depending on wavelength and LOS used, the vertical resolution of the retrieved profiles is as good as 2 km near flight altitude. Above 14 km the profile information content of AMAXDOAS measurements is sparse. Airborne multiaxis measurements are thus a promising tool for atmospheric studies in the troposphere and the upper troposphere and lower stratosphere region.

A novel approach to retrieving total ozone columns from the ERS2 GOME (Global Ozone Monitoring Experiment) spectral data has been developed. With selected GOME wavelength regions, from clear and cloudy pixels alike plus orbital and instrument data as input, a feed-forward neural network was trained to determine total ozone in a one-step inverse retrieval procedure. To achieve this training, ground-based total ozone measurements from the World Ozone and Ultraviolet Data Center (WOUDC) for the years 1996-2000, supplemented with Dobson-corrected Total Ozone Mapping Spectrometer (TOMS) data to provide global coverage, were collocated with GOME ground pixels into a training data set. Validation of the neural-network-retrieved ozone values relative to independent ground stations yielded a rms error of better than 11 Dobson units. Comparisons performed on the basis of operationally available TOMS and GOME level-3 maps exhibit good agreement in general, with a latitude-dependent offset.

Unlike other heavy metals that are inherently associated with atmospheric aerosols, mercury in ambient air exists predominantly in the gaseous elemental form. Because of its prolonged atmospheric residence time, elemental mercury vapor is distributed on a global scale. Recently, Canadian researchers have discovered that total gaseous mercury levels in the lower tropospheric boundary layer in the Canadian Arctic are often significantly depleted during the months after polar sunrise. A possible explanation may involve oxidation of elemental mercury, followed by adsorption and deposition of the oxidized form, leading to an increased input of atmospheric mercury into the Arctic ecosystem. Here we present the first continuous high-time-resolution measurements of total gaseous mercury in the Antarctic covering a 12-month period between January 2000 and January 2001 at the German Antarctic research station Neumayer (70 degrees 39' S, 8 degrees 15' W). We report that mercury depletion events also occur in the Antarctic after polar sunrise and compare our measurements with a data setfrom Alert, Nunavut, Canada. We also present indications that BrO radicals and ozone play a key role in the boundary-layer chemistry during springtime mercury depletion events in the Antarctic troposphere.

New high-resolution Fourier transform absorption spectra of an (15)N(16)O(2) isotopic sample of nitrogen dioxide were recorded at the University of Bremen in the 6.3-µm region. Starting from the results of a previous study [Y. Hamada, J. Mol. Struct. 242, 367-377 (1991)], a new and more extended analysis of the nu(3) band located at 1582.1039 cm(-1) has been performed. The spin-rotation energy levels were satisfactorily reproduced using a theoretical model which takes into account both the Coriolis interactions between the spin-rotation energy levels of the (001) vibrational state with those of the (020) and (100) states and the spin-rotation resonances within each of the NO(2) vibrational states. Precise vibrational energies and rotational, spin-rotation, and coupling constants were obtained in this way for the first triad of (15)N(16)O(2) interacting states {(020), (100), (001)}. Finally, a comprehensive list of line positions and line intensities of the {nu(1), 2nu(2), nu(3)} interacting bands of (15)N(16)O(2) was generated, using for the line intensities the transition moment operators which were obtained previously for the main isotopic species. Copyright 2000 Academic Press.

The Global Ozone Monitoring Experiment (GOME) is a new instrument, which was launched aboard the second European Remoting Sensing satellite ESA-ERS2 in 1995. For its long-term radiometric and spectral calibration the GOME observes the sun and less frequently the moon on a regular basis. These measurements of the lunar radiance and solar irradiance have been used in a study to determine, for the first time to the authors' knowledge, the geometric lunar albedo from 240 to 800 nm at high spectral resolution from space. For a waning moon there is good agreement with ground-based measurements in the visible region and with recent space-based measurements in the ultraviolet region. In addition, the use of these measurements for the characterization of in-orbit degradation of instruments operating in this spectral region has been adequately demonstrated.

Line shift coefficients for five lines of five different isotopomers in the fundamental band of CO in the spectral region near 2058 cm-1 were measured using a three channel lead salt diode laser spectrometer. The study includes the lines P(3) of 13C17O, R(3) of 13C18O, P(9) of 12C18O, P(10) of 13C16O, and P(21) of 12C16O, and covers collisions with N2, O2, H2, D2, He, Ne, Ar, Kr, and Xe. Line shifts of the isotopomers 13C16O, 12C18O, 13C18O, and 13C17O were determined for the first time. Within the experimental uncertainty no significant dependence of the shift effect on the isotopomer was found. The R-branch line under study shows a smaller line shift coefficient than a P-branch line with a similar rotational quantum number. With increasing mass of the noble gas perturber the absolute size of the shift coefficient increases. Moreover self- and nitrogen-broadening coefficients for the isotopomer lines were determined. Compared to previous measurements no significant deviations between different isotopomers were observed. Copyright 1998 Academic Press.

N2 broadening coefficients have been measured for 65 lines of the 13C16O 2-0 band using a Fourier transform spectrometer. These lines are located in the spectral range 4011-4252 cm-1. The spectra were recorded with 99% isotopically pure 13CO in a White-type cell at a resolution of 0.005 cm-1. Voigt profiles convolved with the FTS apparatus function were fitted to the experimental lineshapes using a nonlinear least-squares fit technique. From the fits the Lorentzian HWHM was determined as function of N2 pressure. Pressure broadening coefficients for m between -33 and +34 were obtained with uncertainties of 5.8%. The results are compared to earlier published N2 broadening coefficients and our measurements in the 2-0 band of 12C16O. To our knowledge this is the first investigation of 13CO pressure broadening.

Two-tone frequency modulation spectroscopy has been used in conjunction with InGaAsP lasers in the 1.3-microm region to monitor weak water vapor absorptions in a long path White cell. Detection electronics that reduce the effect of Johnson noise are described. The system was capable of detecting optical densities corresponding to <1.7 x 10(-6) in a 1-Hz bandwidth. Factors limiting the difference between observed and shot noise limited performance for these types of laser and condition are discussed.