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Journal ArticleDOI

Glyoxal vertical columns from GOME-2 backscattered light measurements and comparisons with a global model

17 Dec 2010-Atmospheric Chemistry and Physics (Copernicus GmbH)-Vol. 10, Iss: 24, pp 12059-12072
TL;DR: In this article, a two-step DOAS approach was used to calculate glyoxal vertical column densities from nadir backscattered radiances measured from 2007 to 2009 by the spaceborne GOME-2/METOP-A sensor.
Abstract: . Glyoxal vertical column densities have been retrieved from nadir backscattered radiances measured from 2007 to 2009 by the spaceborne GOME-2/METOP-A sensor. The retrieval algorithm is based on the DOAS technique and optimized settings have been used to determine glyoxal slant columns. The liquid water absorption is accounted for using a two-step DOAS approach, leading to a drastic improvement of the fit quality over remote clear water oceans. Air mass factors are calculated by means of look-up tables of weighting functions pre-calculated with the LIDORT v3.3 radiative transfer model and using a priori glyoxal vertical distributions provided by the IMAGESv2 chemical transport model. The total error estimate comprises random and systematic errors associated to the DOAS fit, the air mass factor calculation and the cloud correction. The highest glyoxal vertical column densities are mainly observed in continental tropical regions, while the mid-latitude columns strongly depend on the season with maximum values during warm months. An anthropogenic signature is also observed in highly populated regions of Asia. Comparisons with glyoxal columns simulated with IMAGESv2 in different regions of the world generally point to a missing glyoxal source, most probably of biogenic origin.

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Citations
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Journal ArticleDOI
TL;DR: In this article, the authors present the new version (v14) of the BIRA-IASB algorithm for the retrieval of formaldehyde (H2CO) columns from spaceborne UV-visible sensors.
Abstract: . We present the new version (v14) of the BIRA-IASB algorithm for the retrieval of formaldehyde (H2CO) columns from spaceborne UV–visible sensors. Applied to OMI measurements from Aura and to GOME-2 measurements from MetOp-A and MetOp-B, this algorithm is used to produce global distributions of H2CO representative of mid-morning and early afternoon conditions. Its main features include (1) a new iterative DOAS scheme involving three fitting intervals to better account for the O2–O2 absorption, (2) the use of earthshine radiances averaged in the equatorial Pacific as reference spectra, and (3) a destriping correction and background normalisation resolved in the across-swath position. For the air mass factor calculation, a priori vertical profiles calculated by the IMAGES chemistry transport model at 09:30 and 13:30 LT are used. Although the resulting GOME-2 and OMI H2CO vertical columns are found to be highly correlated, some systematic differences are observed. Afternoon columns are generally larger than morning ones, especially in mid-latitude regions. In contrast, over tropical rainforests, morning H2CO columns significantly exceed those observed in the afternoon. These differences are discussed in terms of the H2CO column variation between mid-morning and early afternoon, using ground-based MAX-DOAS measurements available from seven stations in Europe, China and Africa. Validation results confirm the capacity of the combined satellite measurements to resolve diurnal variations in H2CO columns. Furthermore, vertical profiles derived from MAX-DOAS measurements in the Beijing area and in Bujumbura are used for a more detailed validation exercise. In both regions, we find an agreement better than 15 % when MAX-DOAS profiles are used as a priori for the satellite retrievals. Finally, regional trends in H2CO columns are estimated for the 2004–2014 period using SCIAMACHY and GOME-2 data for morning conditions, and OMI for early afternoon conditions. Consistent features are observed, such as an increase of the columns in India and central–eastern China, and a decrease in the eastern US and Europe. We find that the higher horizontal resolution of OMI combined with a better sampling and a more favourable illumination at midday allow for more significant trend estimates, especially over Europe and North America. Importantly, in some parts of the Amazonian forest, we observe with both time series a significant downward trend in H2CO columns, spatially correlated with areas affected by deforestation.

161 citations

Journal ArticleDOI
TL;DR: In this paper, an improved GOME-2 NO2 retrieval is described which reduces the scatter of the individual NO2 columns globally but in particular in the region of the Southern Atlantic Anomaly.
Abstract: . Satellite observations of nitrogen dioxide (NO2) provide valuable information on both stratospheric and tropospheric composition. Nadir measurements from GOME, SCIAMACHY, OMI, and GOME-2 have been used in many studies on tropospheric NO2 burdens, the importance of different NOx emissions sources and their change over time. The observations made by the three GOME-2 instruments will extend the existing data set by more than a decade, and a high quality of the data as well as their good consistency with existing time series is of particular importance. In this paper, an improved GOME-2 NO2 retrieval is described which reduces the scatter of the individual NO2 columns globally but in particular in the region of the Southern Atlantic Anomaly. This is achieved by using a larger fitting window including more spectral points, and by applying a two step spike removal algorithm in the fit. The new GOME-2 data set is shown to have good consistency with SCIAMACHY NO2 columns. Remaining small differences are shown to be linked to changes in the daily solar irradiance measurements used in both GOME-2 and SCIAMACHY retrievals. In the large retrieval window, a not previously identified spectral signature was found which is linked to deserts and other regions with bare soil. Inclusion of this empirically derived pseudo cross-section significantly improves the retrievals and potentially provides information on surface properties and desert aerosols. Using the new GOME-2 NO2 data set, a long-term average of tropospheric columns was computed and high-pass filtered. The resulting map shows evidence for pollution from several additional shipping lanes, not previously identified in satellite observations. This illustrates the excellent signal to noise ratio achievable with the improved GOME-2 retrievals.

131 citations

Journal ArticleDOI
TL;DR: The first detection of glyoxal (CHOCHO) over the tropical Pacific Ocean in the Marine Boundary Layer (MBL) was made by means of the University of Colorado Ship Multi-Axis Differential Optical Absorption Spectroscopy (CU SMAX-DOAS) instrument aboard the research vessel Ronald H. Brown as mentioned in this paper.
Abstract: . We present the first detection of glyoxal (CHOCHO) over the remote tropical Pacific Ocean in the Marine Boundary Layer (MBL). The measurements were conducted by means of the University of Colorado Ship Multi-Axis Differential Optical Absorption Spectroscopy (CU SMAX-DOAS) instrument aboard the research vessel Ronald H. Brown. The research vessel was on a cruise in the framework of the VAMOS Ocean-Cloud-Atmosphere-Land Study – Regional Experiment (VOCALS-REx) and the Tropical Atmosphere Ocean (TAO) projects lasting from October 2008 through January 2009 (74 days at sea). The CU SMAX-DOAS instrument features a motion compensation system to characterize the pitch and roll of the ship and to compensate for ship movements in real time. We found elevated mixing ratios of up to 140 ppt CHOCHO located inside the MBL up to 3000 km from the continental coast over biologically active upwelling regions of the tropical Eastern Pacific Ocean. This is surprising since CHOCHO is very short lived (atmospheric life time ~2 h) and highly water soluble (Henry's Law constant H = 4.2 × 105 M/atm). This CHOCHO cannot be explained by transport of it or its precursors from continental sources. Rather, the open ocean must be a source for CHOCHO to the atmosphere. Dissolved Organic Matter (DOM) photochemistry in surface waters is a source for Volatile Organic Compounds (VOCs) to the atmosphere, e.g. acetaldehyde. The extension of this mechanism to very soluble gases, like CHOCHO, is not straightforward since the air-sea flux is directed from the atmosphere into the ocean. For CHOCHO, the dissolved concentrations would need to be extremely high in order to explain our gas-phase observations by this mechanism (40–70 μM CHOCHO, compared to ~0.01 μM acetaldehyde and 60–70 μM DOM). Further, while there is as yet no direct measurement of VOCs in our study area, measurements of the CHOCHO precursors isoprene, and/or acetylene over phytoplankton bloom areas in other parts of the oceans are too low (by a factor of 10–100) to explain the observed CHOCHO amounts. We conclude that our CHOCHO data cannot be explained by currently understood processes. Yet, it supports first global source estimates of 20 Tg/year CHOCHO from the oceans, which likely is a significant source of secondary organic aerosol (SOA). This chemistry is currently not considered by atmospheric models.

121 citations

Journal ArticleDOI
TL;DR: In this article, the authors presented a new dataset of formaldehyde vertical columns retrieved from observations of GOME-2 on board the EUMETSAT MetOp-A platform between 2007 and 2011.
Abstract: . We present a new dataset of formaldehyde vertical columns retrieved from observations of GOME-2 on board the EUMETSAT MetOp-A platform between 2007 and 2011. The new retrieval scheme, which has been optimised for GOME-2, includes a two-step fitting procedure that strongly reduces the impact of spectral interferences between H2CO and BrO, and a modified DOAS approach that better handles ozone absorption effects at moderately low sun elevations. Owing to these new features, the noise in the H2CO slant columns is reduced by up to 40% in comparison to baseline retrieval settings used operationally. Also, the previously reported underestimation of the H2CO columns in tropical and mid-latitude regions has been largely eliminated, improving the agreement with coincident SCIAMACHY observations. To compensate for the drift of the GOME-2 slit function and to mitigate the instrumental degradation effects on H2CO retrievals, an asymmetric Gaussian line-shape is fitted during the irradiance calibration. Additionally, external parameters used in the tropospheric air mass factor computation (surface reflectances, cloud parameters and a priori profile shapes of H2CO) have been updated using most recent databases. Similar updates were also applied to the historical datasets of GOME and SCIAMACHY, leading to the generation of a consistent multi-mission H2CO data record covering the time period from 1997 until 2011. Comparing the resulting time series of monthly averaged H2CO vertical columns in 12 large regions worldwide, the correlation coefficient between SCIAMACHY and GOME-2 columns is generally higher than 0.8 in the overlap period, and linear regression slopes differ by less than 10% from unity in most of the regions. In comparison to SCIAMACHY, the largely improved spatial sampling of GOME-2 allows for a better characterisation of formaldehyde distribution at the regional scale and/or at shorter timescales, leading to a better identification of the emission sources of non-methane volatile organic compounds.

119 citations

Journal ArticleDOI
TL;DR: In this paper, the results of two research flights (RF12, RF17) over the tropical Eastern Pacific Ocean (tEPO) as part of the "Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated hydrocarbons" (TORERO) project are presented.
Abstract: . Tropospheric chemistry of halogens and organic carbon over tropical oceans modifies ozone and atmospheric aerosols, yet atmospheric models remain largely untested for lack of vertically resolved measurements of bromine monoxide (BrO), iodine monoxide (IO) and small oxygenated hydrocarbons like glyoxal (CHOCHO) in the tropical troposphere. BrO, IO, glyoxal, nitrogen dioxide (NO2), water vapor (H2O) and O2–O2 collision complexes (O4) were measured by the University of Colorado Airborne Multi-AXis Differential Optical Absorption Spectroscopy (CU AMAX-DOAS) instrument, aerosol extinction by high spectral resolution lidar (HSRL), in situ aerosol size distributions by an ultra high sensitivity aerosol spectrometer (UHSAS) and in situ H2O by vertical-cavity surface-emitting laser (VCSEL) hygrometer. Data are presented from two research flights (RF12, RF17) aboard the National Science Foundation/National Center for Atmospheric Research Gulfstream V aircraft over the tropical Eastern Pacific Ocean (tEPO) as part of the "Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated hydrocarbons" (TORERO) project (January/February 2012). We assess the accuracy of O4 slant column density (SCD) measurements in the presence and absence of aerosols. Our O4-inferred aerosol extinction profiles at 477 nm agree within 6% with HSRL in the boundary layer and closely resemble the renormalized profile shape of Mie calculations constrained by UHSAS at low (sub-Rayleigh) aerosol extinction in the free troposphere. CU AMAX-DOAS provides a flexible choice of geometry, which we exploit to minimize the SCD in the reference spectrum (SCDREF, maximize signal-to-noise ratio) and to test the robustness of BrO, IO and glyoxal differential SCDs. The RF12 case study was conducted in pristine marine and free tropospheric air. The RF17 case study was conducted above the NOAA RV Ka'imimoana (TORERO cruise, KA-12-01) and provides independent validation data from ship-based in situ cavity-enhanced DOAS and MAX-DOAS. Inside the marine boundary layer (MBL) no BrO was detected (smaller than 0.5 pptv), and 0.2–0.55 pptv IO and 32–36 pptv glyoxal were observed. The near-surface concentrations agree within 30% (IO) and 10% (glyoxal) between ship and aircraft. The BrO concentration strongly increased with altitude to 3.0 pptv at 14.5 km (RF12, 9.1 to 8.6° N; 101.2 to 97.4° W). At 14.5 km, 5–10 pptv NO2 agree with model predictions and demonstrate good control over separating tropospheric from stratospheric absorbers (NO2 and BrO). Our profile retrievals have 12–20 degrees of freedom (DoF) and up to 500 m vertical resolution. The tropospheric BrO vertical column density (VCD) was 1.5 × 1013 molec cm−2 (RF12) and at least 0.5 × 1013 molec cm−2 (RF17, 0–10 km, lower limit). Tropospheric IO VCDs correspond to 2.1 × 1012 molec cm−2 (RF12) and 2.5 × 1012 molec cm−2 (RF17) and glyoxal VCDs of 2.6 × 1014 molec cm−2 (RF12) and 2.7 × 1014 molec cm−2 (RF17). Surprisingly, essentially all BrO as well as the dominant IO and glyoxal VCD fraction was located above 2 km (IO: 58 ± 5%, 0.1–0.2 pptv; glyoxal: 52 ± 5%, 3–20 pptv). To our knowledge there are no previous vertically resolved measurements of BrO and glyoxal from aircraft in the tropical free troposphere. The atmospheric implications are briefly discussed. Future studies are necessary to better understand the sources and impacts of free tropospheric halogens and oxygenated hydrocarbons on tropospheric ozone, aerosols, mercury oxidation and the oxidation capacity of the atmosphere.

91 citations

References
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Journal ArticleDOI
TL;DR: In this article, the authors presented an estimation of the total retrieval uncertainty for vertical tropospheric NO2 columns based on theoretical error source discussions combined with actual Global Ozone Monitoring Experiment (GOME) observations.
Abstract: [1] Retrieval uncertainty estimates for vertical tropospheric NO2 columns based on theoretical error source discussions combined with actual Global Ozone Monitoring Experiment (GOME) observations are presented. Contributions to the total retrieval uncertainty are divided into three categories: (1) errors caused by measurement noise and spectral fitting, affecting the slant column density, (2) errors related to the separation of stratospheric and tropospheric NO2 affecting the estimate of the stratospheric slant column, and (3) errors due to uncertainty in model parameters such as clouds, surface albedo, and a priori profile shape, affecting the tropospheric air mass factor. Furthermore, it is shown that a correction for the effective temperature of the trace gas is essential and that a correction for the presence of aerosols needs to be accompanied by aerosol corrections to the cloud retrieval. A discussion of the error components and total retrieval uncertainty is given for March 1997. Tropospheric NO2 columns can be retrieved with a precision of 35–60% over regions with a large contribution of the troposphere to the total column. This error estimate demonstrates the need for highly accurate albedo maps, cloud retrieval schemes, and realistic a priori NO2 profile shapes.

625 citations


"Glyoxal vertical columns from GOME-..." refers background in this paper

  • ...Although no explicit correction for aerosols is applied, the cloud algorithm implicitly accounts for a possible contribution from reflecting aerosols by retrieving higher effective cloud fractions (Boersma et al. , 2004). In addition,Leitão et al.(2010) found that neglecting aerosols leads to moderate errors in most cases....

    [...]

Journal ArticleDOI
TL;DR: In this paper, a detailed simulation of glyoxal and methylglyoxal in the GEOS-Chem global 3-D chemical transport model including the best knowledge of source and sink processes was conducted.
Abstract: [1] We construct global budgets of atmospheric glyoxal and methylglyoxal with the goal of quantifying their potential for global secondary organic aerosol (SOA) formation via irreversible uptake by aqueous aerosols and clouds. We conduct a detailed simulation of glyoxal and methylglyoxal in the GEOS-Chem global 3-D chemical transport model including our best knowledge of source and sink processes. Our resulting best estimates of the global sources of glyoxal and methylglyoxal are 45 Tg a−1 and 140 Tg a−1, respectively. Oxidation of biogenic isoprene contributes globally 47% of glyoxal and 79% of methylglyoxal. The second most important precursors are acetylene (mostly anthropogenic) for glyoxal and acetone (mostly biogenic) for methylglyoxal. Both acetylene and acetone have long lifetimes and provide a source of dicarbonyls in the free troposphere. Atmospheric lifetimes of glyoxal and methylglyoxal in the model are 2.9 h and 1.6 h, respectively, mostly determined by photolysis. Simulated dicarbonyl concentrations in continental surface air at northern midlatitudes are in the range 10–100 ppt, consistent with in situ measurements. On a global scale, the highest concentrations are over biomass burning regions, in agreement with glyoxal column observations from the SCIAMACHY satellite instrument. SCIAMACHY and a few ship cruises also suggest a large marine source of dicarbonyls missing from our model. The global source of SOA from the irreversible uptake of dicarbonyls in GEOS-Chem is 11 Tg C a−1, including 2.6 Tg C a−1 from glyoxal and 8 Tg C a−1 from methylglyoxal; 90% of this source takes place in clouds. The magnitude of the global SOA source from dicarbonyls is comparable to that computed in GEOS-Chem from the standard mechanism involving reversible partitioning of semivolatile products from the oxidation of monoterpenes, sesquiterpenes, isoprene, and aromatics.

578 citations

Journal ArticleDOI
TL;DR: In this paper, the Global Ozone Monitoring Experiment (GOME) Flight-Model (FM) satellite spectrometer was used to measure the absorption cross sections of O3 in the 231-794nm range.
Abstract: Absorption cross sections of O3 in the 231–794 nm range have been measured at temperatures between 202 and 293 K using the Global Ozone Monitoring Experiment (GOME) Flight-Model (FM) satellite spectrometer. The GOME FM spectra have a spectral resolution of about 0.2 nm below 400 nm and of about 0.3 nm above 400 nm, and were recorded covering simultaneously the Hartley, Huggins, and Chappuis bands centered around 255, 340, and 610 nm, respectively. The variation of the O3 absorption cross sections was investigated over the entire spectral range 231–794 nm. The new cross sections are important as reference data for atmospheric remote-sensing of O3 and other trace gases.

476 citations

Journal ArticleDOI
TL;DR: The absorption spectrum of O2 and O2-O2 collision pairs were measured over the wavelength range from 330 to 1140 nm using pressures of O 2 from 1 to 55 atm at 298 K as mentioned in this paper.
Abstract: The absorption spectrum of O2 and O2-O2 collision pairs were measured over the wavelength range from 330 to 1140 nm using pressures of O2 from 1 to 55 atm at 298 K. Absorption cross sections, pressure dependences, band centers, and full widths at half maximum of the observed absorption bands centered at 343.4, 360.5, 380.2, 446.7, 477.3, 532.2, 577.2, 630.0, 688, 762, and 1065.2 nm are reported. The absorption bands centered at 360.5, 380.2, and 477.3 nm were also measured at 196 K and their temperature dependences were characterized.

474 citations

01 Dec 2007

467 citations


"Glyoxal vertical columns from GOME-..." refers background in this paper

  • ...(2005) O2-O2 collision pair Greenblatt et al. (1990); shifted by 0....

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