scholarly journals The impact of SCIAMACHY near-infrared instrument calibration on CH<sub>4</sub> and CO total columns

2005 ◽  
Vol 5 (2) ◽  
pp. 1733-1770 ◽  
Author(s):  
A. M. S. Gloudemans ◽  
H. Schrijver ◽  
Q. Kleipool ◽  
M. M. P. van den Broek ◽  
A. G. Straume ◽  
...  

Abstract. The effects of three important SCIAMACHY near-infrared instrument calibration issues on the retrieved methane (CH4) and carbon monoxide (CO) total columns have been investigated: the effects of the growing ice layer on the near-infrared detectors, the effects of the orbital variation of the instrument dark signal, and the effects of the dead/bad detector pixels. Corrections for each of these instrument calibration issues have been defined. The retrieved CH4 and CO total columns including these corrections show good agreement with CO measurements from the MOPITT satellite instrument and with CH4 model calculations by the chemistry transport model TM3. Using a systematic approach, it is shown that all three instrument calibration issues have a significant effect on the retrieved CH4 and CO total columns, although the impact on the CH4 total columns is more pronounced than for CO. Results for three different wavelength ranges are compared and show good agreement. The growing ice layer and the orbital variation of the dark signal show a systematic, but time-dependent effect on the retrieved CH4 and CO total columns, whereas the dead/bad pixels show a more random effect. The importance of accurate corrections for each of these instrument calibration issues is illustrated using examples where inaccurate corrections lead to a wrong interpretation of the results.

2005 ◽  
Vol 5 (9) ◽  
pp. 2369-2383 ◽  
Author(s):  
A. M. S. Gloudemans ◽  
H. Schrijver ◽  
Q. Kleipool ◽  
M. M. P. van den Broek ◽  
A. G. Straume ◽  
...  

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


2014 ◽  
Vol 7 (11) ◽  
pp. 3783-3799 ◽  
Author(s):  
A. T. J. de Laat ◽  
I. Aben ◽  
M. Deeter ◽  
P. Nédélec ◽  
H. Eskes ◽  
...  

Abstract. Validation results from a comparison between Measurement Of Pollution In The Troposphere (MOPITT) V5 Near InfraRed (NIR) carbon monoxide (CO) total column measurements and Measurement of Ozone and Water Vapour on Airbus in-service Aircraft (MOZAIC)/In-Service Aircraft for a Global Observing System (IAGOS) aircraft measurements are presented. A good agreement is found between MOPITT and MOZAIC/IAGOS measurements, consistent with results from earlier studies using different validation data and despite large variability in MOPITT CO total columns along the spatial footprint of the MOZAIC/IAGOS measurements. Validation results improve when taking the large spatial footprint of the MOZAIC/IAGOS data into account. No statistically significant drift was detected in the validation results over the period 2002–2010 at global, continental and local (airport) scales. Furthermore, for those situations where MOZAIC/IAGOS measurements differed from the MOPITT a priori, the MOPITT measurements clearly outperformed the MOPITT a priori data, indicating that MOPITT NIR retrievals add value to the MOPITT a priori. Results from a high spatial resolution simulation of the chemistry-transport model MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle) showed that the most likely explanation for the large MOPITT variability along the MOZAIC-IAGOS profile flight path is related to spatio-temporal CO variability, which should be kept in mind when using MOZAIC/IAGOS profile measurements for validating satellite nadir observations.


2013 ◽  
Vol 13 (17) ◽  
pp. 9057-9082 ◽  
Author(s):  
T. Stavrakou ◽  
J.-F. Müller ◽  
K. F. Boersma ◽  
R. J. van der A ◽  
J. Kurokawa ◽  
...  

Abstract. Triggered by recent developments from laboratory and field studies regarding major NOx sink pathways in the troposphere, this study evaluates the influence of chemical uncertainties in NOx sinks for global NOx distributions calculated by the IMAGESv2 chemistry-transport model, and quantifies their significance for top-down NOx emission estimates. Our study focuses on five key chemical parameters believed to be of primary importance, more specifically, the rate of the reaction of NO2 with OH radicals, the newly identified HNO3-forming channel in the reaction of NO with HO2, the reactive uptake of N2O5 and HO2 by aerosols, and the regeneration of OH in the oxidation of isoprene. Sensitivity simulations are performed to estimate the impact of each source of uncertainty. The model calculations show that, although the NO2+OH reaction is the largest NOx sink globally accounting for ca. 60% of the total sink, the reactions contributing the most to the overall uncertainty are the formation of HNO3 in NO+HO2, leading to NOx column changes exceeding a factor of two over tropical regions, and the uptake of HO2 by aqueous aerosols, in particular over East and South Asia. Emission inversion experiments are carried out using model settings which either minimise (MINLOSS) or maximise (MAXLOSS) the total NOx sink, both constrained by one year of OMI NO2 column data from the DOMINO v2 KNMI algorithm. The choice of the model setup is found to have a major impact on the top-down flux estimates, with 75% higher emissions for MAXLOSS compared to the MINLOSS inversion globally. Even larger departures are found for soil NO (factor of 2) and lightning (1.8). The global anthropogenic source is better constrained (factor of 1.57) than the natural sources, except over South Asia where the combined uncertainty primarily associated to the NO+HO2 reaction in summer and HO2 uptake by aerosol in winter lead to top-down emission differences exceeding a factor of 2. Evaluation of the emission optimisation is performed against independent satellite observations from the SCIAMACHY sensor, with airborne NO2 measurements of the INTEX-A and INTEX-B campaigns, as well as with two new bottom-up inventories of anthropogenic emissions in Asia (REASv2) and China (MEIC). Neither the MINLOSS nor the MAXLOSS setup succeeds in providing the best possible match with all independent datasets. Whereas the minimum sink assumption leads to better agreement with aircraft NO2 profile measurements, consistent with the results of a previous analysis (Henderson et al., 2012), the same assumption leads to unrealistic features in the inferred distribution of emissions over China. Clearly, although our study addresses an important issue which was largely overlooked in previous inversion exercises, and demonstrates the strong influence of NOx loss uncertainties on top-down emission fluxes, additional processes need to be considered which could also influence the inferred source.


2006 ◽  
Vol 6 (3) ◽  
pp. 5387-5425 ◽  
Author(s):  
M. P. Barkley ◽  
P. S. Monks ◽  
U. Frieß ◽  
R. L. Mittermeier ◽  
H. Fast ◽  
...  

Abstract. Atmospheric CO2 concentrations, retrieved from spectral measurements made in the near infrared (NIR) by the SCIAMACHY instrument, using Full Spectral Initiation Weighting Function Modified Differential Optical Absorption Spectroscopy (FSI WFM-DOAS), are compared to ground based Fourier Transform Infrared (FTIR) data and to the output from a global chemistry-transport model. Analysis of the FSI WFM-DOAS retrievals with respect to the ground based FTIR instrument, located at Egbert, Canada, show good agreement with an average negative bias of approximately −4.0% with a standard deviation of ~3.0%. This bias which exhibits an apparent seasonal trend, is of unknown origin, though slight differences between the averaging kernels of the instruments and the limited temporal coverage of the FTIR data may be the cause. The relative scatter of the retrieved vertical column densities is comparable to the spread of the FTIR measurements themselves. Normalizing the CO2 columns using the surface pressure does not affect the magnitude of this bias although it slightly increases the scatter of the FSI data. Comparisons of the FSI retrievals to the TM3 global chemistry-transport model, performed over four selected Northern Hemisphere scenes show good agreement. The correlation, between the time series of the SCIAMACHY and model monthly scene averages, are ~0.7 or greater, demonstrating the ability of SCIAMACHY to detect seasonal changes in the CO2 distribution. The amplitude of the seasonal cycle, peak to peak, observed by SCIAMACHY however, is overestimated by a factor of 2–3, which cannot be explained. The yearly means detected by SCIAMACHY are within 2% of those of the model with the mean difference between the CO2 distributions also approximately 2.0%. Additionally, analysis of the retrieved CO2 distributions reveals structure not evident in the model fields which correlates well with land classification type. From these comparisons, the overall precision and bias of the CO2 columns retrieved by the FSI algorithm are estimated to be close to 1.0% and <4.0% respectively.


2010 ◽  
Vol 10 (20) ◽  
pp. 9915-9930 ◽  
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
F. Goutail

Abstract. The polar stratospheric ozone loss during the Arctic winters 2004/2005–2009/2010 is investigated by using high resolution simulations from the chemical transport model Mimosa-Chim and observations from Aura Microwave Limb Sounder (MLS), by applying the passive tracer technique. The winter 2004/2005 shows the coldest temperatures, highest area of polar stratospheric clouds and strongest chlorine activation in 2004/2005–2009/2010. The ozone loss diagnosed from both simulations and measurements inside the polar vortex at 475 K ranges from 0.7 ppmv in the warm winter 2005/2006 to 1.5–1.7 ppmv in the cold winter 2004/2005. Halogenated (chlorine and bromine) catalytic cycles contribute to 75–90% of the ozone loss at this level. At 675 K the lowest loss of 0.3–0.5 ppmv is computed in 2008/2009, and the highest loss of 1.3 ppmv is estimated in 2006/2007 by the model and in 2004/2005 by MLS. Most of the ozone loss (60–75%) at this level results from nitrogen catalytic cycles rather than halogen cycles. At both 475 and 675 K levels the simulated ozone and ozone loss evolution inside the vortex is in reasonably good agreement with the MLS observations. The ozone partial column loss in 350–850 K deduced from the model calculations at the MLS sampling locations inside the polar vortex ranges between 43 DU in 2005/2006 and 109 DU in 2004/2005, while those derived from the MLS observations range between 26 DU and 115 DU for the same winters. The partial column ozone depletion derived in that vertical range is larger than that estimated in 350–550 K by 19±7 DU on average, mainly due to NOx chemistry. The column ozone loss estimates from both Mimosa-Chim and MLS in 350–850 K are generally in good agreement with those derived from ground-based ultraviolet-visible spectrometer total ozone observations for the respective winters, except in 2010.


2014 ◽  
Vol 14 (9) ◽  
pp. 4827-4841 ◽  
Author(s):  
M. Rex ◽  
I. Wohltmann ◽  
T. Ridder ◽  
R. Lehmann ◽  
K. Rosenlof ◽  
...  

Abstract. Most of the short-lived biogenic and anthropogenic chemical species that are emitted into the atmosphere break down efficiently by reaction with OH and do not reach the stratosphere. Here we show the existence of a pronounced minimum in the tropospheric column of ozone over the West Pacific, the main source region for stratospheric air, and suggest a corresponding minimum of the tropospheric column of OH. This has the potential to amplify the impact of surface emissions on the stratospheric composition compared to the impact when assuming globally uniform OH conditions. Specifically, the role of emissions of biogenic halogenated species for the stratospheric halogen budget and the role of increasing emissions of SO2 in Southeast Asia or from minor volcanic eruptions for the increasing stratospheric aerosol loading need to be reassessed in light of these findings. This is also important since climate change will further modify OH abundances and emissions of halogenated species. Our study is based on ozone sonde measurements carried out during the TransBrom cruise with the RV Sonne roughly along 140–150° E in October 2009 and corroborating ozone and OH measurements from satellites, aircraft campaigns and FTIR instruments. Model calculations with the GEOS-Chem Chemistry and Transport Model (CTM) and the ATLAS CTM are used to simulate the tropospheric OH distribution over the West Pacific and the transport pathways to the stratosphere. The potential effect of the OH minimum on species transported into the stratosphere is shown via modeling the transport and chemistry of CH2Br2 and SO2.


2013 ◽  
Vol 13 (3) ◽  
pp. 7871-7929 ◽  
Author(s):  
T. Stavrakou ◽  
J.-F. Müller ◽  
K. F. Boersma ◽  
R. J. van der A ◽  
J. Kurokawa ◽  
...  

Abstract. Triggered by recent developments from laboratory and field studies regarding major NOx sink pathways in the troposphere, this study evaluates the influence of chemical uncertainties in NOx sinks for global NOx distributions calculated by the IMAGESv2 chemistry-transport model, and quantifies their significance for top-down NOx emission estimates. Our study focuses on four key chemical parameters believed to be of primary importance, more specifically, the rate of the reaction of NO2 with OH radicals, the newly-identified HNO3-forming channel in the reaction of NO with HO2, the reactive uptake of N2O5 on aerosols, and the regeneration of OH in the oxidation of isoprene. Sensitivity simulations are performed to estimate the impact of each source of uncertainty. The model calculations show that, although the NO2 + OH reaction is the largest NOx sink globally accounting for 50–70% of the total sink, the reaction contributing the most to the overall uncertainty is the formation of HNO3 in NO + HO2, leading to NOx column changes reaching a~factor of two over tropical regions, and to a 35% decrease in the global tropospheric NOx lifetime. Emission inversion experiments are carried out using model settings which either miminize (MINLOSS) or maximize (MAXLOSS) the total NOx sink, both constrained by one year of OMI NO2 column data from the DOMINO v2 KNMI algorithm. The choice of the model setup is found to have a major impact on the top-down flux estimates, with 50% higher emissions for MAXLOSS compared to the MINLOSS inversion globally. Even larger departures are found for soil NO (factor of 2) and lightning (70%), whereas the global anthropogenic source is comparatively better constrained, especially in China. Evaluation of the emission optimization is performed against independent satellite observations from the SCIAMACHY sensor, airborne NO2 measurements, observed NOx lifetimes at megacities, as well as with two new bottom-up inventories of anthropogenic emissions in Asia (REASv2) and China (MEIC). Neither the MINLOSS nor the MAXLOSS setup succeeds in providing the best possible match with all independent datasets. Whereas the minimum sink assumption leads to better agreement with aircraft NO2 profile measurements, comforting the results of a previous analysis (Henderson et al., 2012), the same assumption leads to unrealistic features in the inferred distribution of emissions over China. Clearly, although our study addresses an important issue which was largely overlooked in previous inversion exercises, and demonstrates the strong influence of NOx loss uncertainties on top-down emission fluxes, additional processes need to be considered which could also influence the inferred source.


2017 ◽  
Vol 17 (18) ◽  
pp. 11065-11073 ◽  
Author(s):  
Franz Conen ◽  
Sabine Eckhardt ◽  
Hans Gundersen ◽  
Andreas Stohl ◽  
Karl Espen Yttri

Abstract. Ice-nucleating particles (INPs) active at modest supercooling (e.g. −8 °C; INP−8) can transform clouds from liquid to mixed phase, even at very small number concentrations (< 10 m−3). Over the course of 15 months, we found very similar patterns in weekly concentrations of INP−8 in PM10 (median  =  1.7 m−3, maximum  =  10.1 m−3) and weekly amounts of rainfall (median  =  28 mm, maximum  =  153 mm) at Birkenes, southern Norway. Most INP−8 were probably aerosolised locally by the impact of raindrops on plant, litter and soil surfaces. Major snowfall and heavy rain onto snow-covered ground were not mirrored by enhanced numbers of INP−8. Further, transport model calculations for large (> 4 m−3) and small (< 4 m−3) numbers of INP−8 revealed that potential source regions likely to provide precipitation to southern Norway were associated with large numbers of INP−8. The proportion of land cover and land use type in potential source regions was similar for large and small numbers of INP−8. In PM2. 5 we found consistently about half as many INP−8 as in PM10. From mid-May to mid-September, INP−8 correlated positively with the fungal spore markers arabitol and mannitol, suggesting that some fraction of INP−8 during that period may consist of fungal spores. In the future, warmer winters with more rain instead of snow may enhance airborne concentrations of INP−8 during the cold season in southern Norway and in other regions with a similar climate.


2010 ◽  
Vol 10 (6) ◽  
pp. 14675-14711
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
F. Goutail

Abstract. The stratospheric ozone loss during the Arctic winters 2004/05–2009/10 is investigated by using high resolution simulations from the chemical transport model Mimosa-Chim and observations from Microwave Limb Sounder (MLS) on Aura by the passive tracer technique. The winter 2004/05 was the coldest of the series with strongest chlorine activation. The ozone loss diagnosed from both model and measurements inside the polar vortex at 475 K ranges from ~1–0.7 ppmv in the warm winter 2005/06 to 1.7 ppmv in the cold winter 2004/05. Halogenated (chlorine and bromine) catalytic cycles contribute to 75–90% of the accumulated ozone loss at this level. At 675 K the lowest loss of ~0.4 ppmv is computed in 2008/09 from both simulations and observations and, the highest loss is estimated in 2006/07 by the model (1.3 ppmv) and in 2004/05 by MLS (1.5 ppmv). Most of the ozone loss (60–75%) at this level results from cycles catalysed by nitrogen oxides (NO and NO2) rather than halogens. At both 475 and 675 K levels the simulated ozone evolution inside the polar vortex is in reasonably good agreement with the observations. The ozone total column loss deduced from the model calculations at the MLS sampling locations inside the vortex ranges between 40 DU in 2005/06 and 94 DU in 2004/05, while that derived from observations ranges between 37 DU and 111 DU in the same winters. These estimates from both Mimosa-Chim and MLS are in general good agreement with those from the ground-based UV-VIS (ultra violet–visible) ozone loss analyses for the respective winters.


2014 ◽  
Vol 7 (6) ◽  
pp. 5251-5291
Author(s):  
A. T. J. de Laat ◽  
I. Aben ◽  
M. Deeter ◽  
P. Nédélec ◽  
H. Eskes ◽  
...  

Abstract. Validation results from a comparison between Measurement Of Pollution In The Troposphere (MOPITT) V5 Near InfraRed (NIR) Carbon Monoxide (CO) total column measurements and Measurement of Ozone and Water Vapour on Airbus in-service Aircraft (MOZAIC)/In-Service Aircraft for a Global Observing System (IAGOS) aircraft measurements are presented. A good agreement is found between MOPITT and MOZAIC/IAGOS measurements, consistent with results from earlier studies using different validation data and despite large variability in MOPITT CO total columns along the spatial footprint of the MOZAIC/IAGOS measurements. Validation results improve when taking the large spatial footprint of the MOZAIC/IAGOS data into account. No statistically significant drift was detected in the validation results over the period 2002–2010 at global, continental and local (airport) scales. Furthermore, for those situations where MOZAIC/IAGOS measurements differed from the MOPITT a priori, the MOPITT measurements clearly outperformed the MOPITT a priori data, indicating that MOPITT NIR retrievals add value to the MOPITT a priori. Results from a high spatial resolution simulation of the chemistry-transport model MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle) showed that the most likely explanation for the large MOPITT variability along the MOZAIC-IAGOS profile flight path is related to spatio-temporal CO variability, which should be kept in mind when using MOZAIC/IAGOS profile measurements for validating satellite nadir observations.


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