scholarly journals The continental source of glyoxal estimated by the synergistic use of spaceborne measurements and inverse modelling

2009 ◽  
Vol 9 (3) ◽  
pp. 13593-13628 ◽  
Author(s):  
T. Stavrakou ◽  
J.-F. Müller ◽  
I. De Smedt ◽  
M. Van Roozendael ◽  
M. Kanakidou ◽  
...  

Abstract. Tropospheric glyoxal and formaldehyde columns retrieved from the SCIAMACHY satellite instrument in 2005 are used with the IMAGESv2 global chemistry-transport model and its adjoint in a two-compound inversion scheme designed to estimate the continental source of glyoxal. The formaldehyde observations provide an important constraint on the production of glyoxal from isoprene in the model, since the degradation of isoprene constitutes an important source of both glyoxal and formaldehyde. Current modelling studies underestimate largely the observed glyoxal satellite columns, pointing to the existence of an additional land glyoxal source of biogenic origin. We include an extra glyoxal source in the model and we explore its possible distribution and magnitude through two inversion experiments. In the first case, the additional source is represented as a direct glyoxal emission, and in the second, as a secondary formation through the oxidation of an unspecified glyoxal precursor. Besides this extra source, the inversion scheme optimizes the primary glyoxal and formaldehyde emissions, as well as their secondary production from other identified non-methane volatile organic precursors of anthropogenic, pyrogenic and biogenic origin. In the first inversion experiment, the additional direct source, estimated at 36 Tg/yr, represents 38% of the global continental source, whereas the contribution of isoprene is equally important (30%), the remainder being accounted for by anthropogenic (20%) and pyrogenic fluxes. The inversion succeeds in reducing the underestimation of the glyoxal columns by the model, but it leads to a severe overestimation of glyoxal surface concentrations in comparison with in situ measurements. In the second scenario, the inferred total global continental glyoxal source is estimated at 108 Tg/yr, almost two times higher than the global a priori source. The extra secondary source is the largest contribution to the global glyoxal budget (50%), followed by the production from isoprene (26%) and from anthropogenic NMVOC precursors (14%). A better performance is achieved in this case, as the updated emissions allow for a satisfactory agreement of the model with both satellite and in situ glyoxal observations.

2009 ◽  
Vol 9 (21) ◽  
pp. 8431-8446 ◽  
Author(s):  
T. Stavrakou ◽  
J.-F. Müller ◽  
I. De Smedt ◽  
M. Van Roozendael ◽  
M. Kanakidou ◽  
...  

Abstract. Tropospheric glyoxal and formaldehyde columns retrieved from the SCIAMACHY satellite instrument in 2005 are used with the IMAGESv2 global chemistry-transport model and its adjoint in a two-compound inversion scheme designed to estimate the continental source of glyoxal. The formaldehyde observations provide an important constraint on the production of glyoxal from isoprene in the model, since the degradation of isoprene constitutes an important source of both glyoxal and formaldehyde. Current modelling studies underestimate largely the observed glyoxal satellite columns, pointing to the existence of an additional land glyoxal source of biogenic origin. We include an extra glyoxal source in the model and we explore its possible distribution and magnitude through two inversion experiments. In the first case, the additional source is represented as a direct glyoxal emission, and in the second, as a secondary formation through the oxidation of an unspecified glyoxal precursor. Besides this extra source, the inversion scheme optimizes the primary glyoxal and formaldehyde emissions, as well as their secondary production from other identified non-methane volatile organic precursors of anthropogenic, pyrogenic and biogenic origin. In the first inversion experiment, the additional direct source, estimated at 36 Tg/yr, represents 38% of the global continental source, whereas the contribution of isoprene is equally important (30%), the remainder being accounted for by anthropogenic (20%) and pyrogenic fluxes. The inversion succeeds in reducing the underestimation of the glyoxal columns by the model, but it leads to a severe overestimation of glyoxal surface concentrations in comparison with in situ measurements. In the second scenario, the inferred total global continental glyoxal source is estimated at 108 Tg/yr, almost two times higher than the global a priori source. The extra secondary source is the largest contribution to the global glyoxal budget (50%), followed by the production from isoprene (26%) and from anthropogenic NMVOC precursors (14%). A better performance is achieved in this case, as the updated emissions allow for a satisfactory agreement of the model with both satellite and in situ glyoxal observations.


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.


2015 ◽  
Vol 8 (4) ◽  
pp. 3593-3651 ◽  
Author(s):  
J. Guth ◽  
B. Josse ◽  
V. Marécal ◽  
M. Joly

Abstract. In this study we develop a Secondary Inorganic Aerosol (SIA) module for the chemistry transport model MOCAGE developed at CNRM. Based on the thermodynamic equilibrium module ISORROPIA II, the new version of the model is evaluated both at the global scale and at the regional scale. The results show high concentrations of secondary inorganic aerosols in the most polluted regions being Europe, Asia and the eastern part of North America. Asia shows higher sulfate concentrations than other regions thanks to emissions reduction in Europe and North America. Using two simulations, one with and the other without secondary inorganic aerosol formation, the model global outputs are compared to previous studies, to MODIS AOD retrievals, and also to in situ measurements from the HTAP database. The model shows a better agreement in all geographical regions with MODIS AOD retrievals when introducing SIA. It also provides a good statistical agreement with in situ measurements of secondary inorganic aerosol composition: sulfate, nitrate and ammonium. In addition, the simulation with SIA gives generally a better agreement for secondary inorganic aerosols precursors (nitric acid, sulfur dioxide, ammonia) in particular with a reduction of the Modified Normalised Mean Bias (MNMB). At the regional scale, over Europe, the model simulation with SIA are compared to the in situ measurements from the EMEP database and shows a good agreement with secondary inorganic aerosol composition. The results at the regional scale are consistent with those obtained with the global simulations. The AIRBASE database was used to compare the model to regulated air quality pollutants being particulate matter, ozone and nitrogen dioxide concentrations. The introduction of the SIA in MOCAGE provides a reduction of the PM2.5 MNMB of 0.44 on a yearly basis and even 0.52 on a three spring months period (March, April, May) when SIA are maximum.


2021 ◽  
Author(s):  
Juan Cuesta ◽  
Lorenzo Costantino ◽  
Matthias Beekmann ◽  
Guillaume Siour ◽  
Laurent Menut ◽  
...  

Abstract. We present a comprehensive study integrating satellite observations of ozone pollution, in situ measurements and chemistry transport model simulations for quantifying the role of anthropogenic emission reductions during the COVID-19 lockdown in spring 2020 over Europe. Satellite observations are derived from the IASI+GOME2 multispectral synergism, which provides particularly enhanced sensitivity to near-surface ozone pollution. These observations are first analysed in terms of differences between the average on 1–15 April 2020, when the strictest lockdown restrictions took place, and the same period in 2019. They show clear enhancements of near-surface ozone in Central Europe and Northern Italy, and some other hotspots, which are typically characterized by VOC-limited chemical regimes. An overall reduction of ozone is observed elsewhere, where ozone chemistry is limited by the abundance of NOx. The spatial distribution of positive and negative ozone concentration anomalies observed from space is in relatively good quantitative agreement with surface in situ measurements over the continent (a correlation coefficient of 0.55, a root-mean-squared difference of 11 ppb and the same standard deviation and range of variability). An average bias of ∼8 ppb between the two observational datasets is remarked, which can partly be explained by the fact the satellite approach retrieves partial columns of ozone with a peak sensitivity above the surface (near 2 km of altitude). For assessing the impact of the reduction of anthropogenic emissions during the lockdown, we adjust the satellite and in situ surface observations for withdrawing the influence of meteorological conditions in 2020 and 2019. This adjustment is derived from the chemistry transport model simulations using the meteorological fields of each year and identical emission inventories. This observational estimate of the influence of lockdown emission reduction is consistent for both datasets. They both show lockdown-associated ozone enhancements in hotspots over Central Europe and Northern Italy, with a reduced amplitude with respect to the total changes observed between the two years, and an overall reduction elsewhere over Europe and the ocean. Satellite observations additionally highlight the ozone anomalies in the regions remote from in situ sensors, an enhancement over the Mediterranean likely associated with maritime traffic emissions and a marked large-scale reduction of ozone elsewhere over ocean (particularly over the North Sea), in consistency with previous assessments done with ozonesondes measurements in the free troposphere. These observational assessments are compared with model-only estimations, using the CHIMERE chemistry transport model. For analysing the uncertainty of the model estimates, we perform two sets of simulations with different setups, differing in the emission inventories, their modifications to account for changes in anthropogenic activities during the lockdown and the meteorological fields. Whereas a general qualitative consistency of positive and negative ozone anomalies is remarked between all model and observational estimates, significant changes are seen in their amplitudes. Models underestimate the range of variability of the ozone changes by at least a factor 2 with respect to the two observational data sets, both for enhancements and decreases of ozone, while the large-scale ozone decrease is not simulated. With one of the setups, the model simulates ozone enhancements a factor 3 to 6 smaller than with the other configuration. This is partly linked to the emission inventories of ozone precursors (at least a 30 % difference), but mainly to differences in vertical mixing of atmospheric constituents depending on the choice of the meteorological model.


2012 ◽  
Vol 12 (10) ◽  
pp. 4493-4512 ◽  
Author(s):  
A. Klonecki ◽  
M. Pommier ◽  
C. Clerbaux ◽  
G. Ancellet ◽  
J.-P. Cammas ◽  
...  

Abstract. This work evaluates the IASI CO product against independent in-situ aircraft data from the MOZAIC program and the POLARCAT aircraft campaign. The validation is carried out by analysing the impact of assimilation of eight months of IASI CO columns retrieved for the period of May to December 2008 into the global chemistry transport model LMDz-INCA. A modelling system based on a sub-optimal Kalman filter was developed and a specific treatment that takes into account the representativeness of observations at the scale of the model grid is applied to the IASI CO columns and associated errors before their assimilation in the model. Comparisons of the assimilated CO profiles with in situ CO measurements indicate that the assimilation leads to a considerable improvement of the model simulations in the middle troposphere as compared with a control run with no assimilation. Model biases in the simulation of background values are reduced and improvement in the simulation of very high concentrations is observed. The improvement is due to the transport by the model of the information present in the IASI CO retrievals. Our analysis also shows the impact of assimilation of CO on the representation of transport into the Arctic region during the POLARCAT summer campaign. A considerable increase in CO mixing ratios over the Asian source region was observed when assimilation was used leading to much higher values of CO during the cross-pole transport episode. These higher values are in good agreement with data from the POLARCAT flights that sampled this plume.


2020 ◽  
Author(s):  
Iolanda Ialongo ◽  
Henrik Virta ◽  
Henk Eskes ◽  
Jari Hovila ◽  
John Douros

<p>We evaluate the satellite-based TROPOMI (TROPOspheric Monitoring Instrument) NO2 products against ground-based observations in Helsinki (Finland). TROPOMI NO2 total (summed) columns are compared with the measurements performed by the Pandora spectrometer during April–September 2018. The mean relative and absolute bias between the TROPOMI and Pandora NO2 total columns is about 10 % and 0.12 × 10<sup>15</sup> molec. cm<sup>-2</sup> respectively.<span> </span></p><p>We find high correlation (r = 0.68) between satellite- and ground-based data, but also that TROPOMI total columns underestimate ground-based observations for relatively large Pandora NO2 total columns, corresponding to episodes of relatively elevated pollution. This is expected because of the relatively large size of the TROPOMI ground pixel (3.5 × 7 km) and the a priori used in the retrieval compared to the relatively small field-of-view of the Pandora instrument. On the other hand, TROPOMI slightly overestimates relatively small NO2 total columns. Replacing the coarse a priori NO2 profiles with high-resolution profiles from the CAMS chemical transport model improves the agreement between TROPOMI and Pandora total columns for episodes of NO2 enhancement.<span> </span></p><p>In order to evaluate the capability of TROPOMI observation for monitoring urban air quality, we also analyse the consistency between satellite-based data and NO2 surface concentrations from the local air quality station. We find similar day-to-day variability between TROPOMI and in situ measurements, with NO2 enhancements observed during the same days. Both satellite- and ground-based data show a similar weekly cycle, with lower NO2 levels during the weekend compared to the weekdays as a result of reduced emissions from traffic and industrial activities (as expected in urban sites). The TROPOMI NO2 maps reveal also spatial features, such as the main traffic ways, the airport and other industrial areas, as well as the effect of the prevailing south-west wind patterns.<span> </span></p><p>These first results confirm that TROPOMI NO2 products are valuable to complement the traditional ground-based in situ data for monitoring urban air quality and are already tested by local and national authorities as well as private companies to monitor pollution sources in the Helsinki region (e.g., emissions from traffic, energy production or oil refineries). For example, TROPOMI NO2 products are already used by the oil refinery company NESTE in their sustainability report and by the Finnish Ministry of Environment to map the air pollution levels in Finland.</p><p>Ialongo, I., Virta, H., Eskes, H., Hovila, J., and Douros, J.: Comparison of TROPOMI/Sentinel 5 Precursor NO2 observations with ground-based measurements in Helsinki, Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2019-329, accepted for publication, 2020.</p>


2014 ◽  
Vol 14 (5) ◽  
pp. 2555-2570 ◽  
Author(s):  
K. C. Wells ◽  
D. B. Millet ◽  
K. E. Cady-Pereira ◽  
M. W. Shephard ◽  
D. K. Henze ◽  
...  

Abstract. We employ new global space-based measurements of atmospheric methanol from the Tropospheric Emission Spectrometer (TES) with the adjoint of the GEOS-Chem chemical transport model to quantify terrestrial emissions of methanol to the atmosphere. Biogenic methanol emissions in the model are based on version 2.1 of the Model of Emissions of Gases and Aerosols from Nature (MEGANv2.1), using leaf area data from NASA's Moderate Resolution Imaging Spectroradiometer (MODIS) and GEOS-5 assimilated meteorological fields. We first carry out a pseudo observation test to validate the overall approach, and find that the TES sampling density is sufficient to accurately quantify regional- to continental-scale methanol emissions using this method. A global inversion of two years of TES data yields an optimized annual global surface flux of 122 Tg yr−1 (including biogenic, pyrogenic, and anthropogenic sources), an increase of 60% from the a priori global flux of 76 Tg yr−1. Global terrestrial methanol emissions are thus nearly 25% those of isoprene (~540 Tg yr−1), and are comparable to the combined emissions of all anthropogenic volatile organic compounds (~100–200 Tg yr−1). Our a posteriori terrestrial methanol source leads to a strong improvement of the simulation relative to an ensemble of airborne observations, and corroborates two other recent top-down estimates (114–120 Tg yr−1) derived using in situ and space-based measurements. Inversions testing the sensitivity of optimized fluxes to model errors in OH, dry deposition, and oceanic uptake of methanol, as well as to the assumed a priori constraint, lead to global fluxes ranging from 118 to 126 Tg yr−1. The TES data imply a relatively modest revision of model emissions over most of the tropics, but a significant upward revision in midlatitudes, particularly over Europe and North America. We interpret the inversion results in terms of specific source types using the methanol : CO correlations measured by TES, and find that biogenic emissions are overestimated relative to biomass burning and anthropogenic emissions in central Africa and southeastern China, while they are underestimated in regions such as Brazil and the US. Based on our optimized emissions, methanol accounts for > 25% of the photochemical source of CO and HCHO over many parts of the northern extratropics during springtime, and contributes ~6% of the global secondary source of those compounds annually.


2015 ◽  
Vol 8 (1) ◽  
pp. 385-398 ◽  
Author(s):  
G. M. Miles ◽  
R. Siddans ◽  
B. J. Kerridge ◽  
B. G. Latter ◽  
N. A. D. Richards

Abstract. This paper describes and assesses the performance of the RAL (Rutherford Appleton Laboratory) ozone profile retrieval scheme for the Global Ozone Monitoring Experiment 2 (GOME-2) with a focus on tropospheric ozone. Developments to the scheme since its application to GOME-1 measurements are outlined. These include the approaches developed to account sufficiently for UV radiometric degradation in the Hartley band and for inadequacies in knowledge of instrumental parameters in the Huggins bands to achieve the high-precision spectral fit required to extract information on tropospheric ozone. The assessment includes a validation against ozonesondes (sondes) sampled worldwide over 2 years (2007–2008). Standard deviations of the ensemble with respect to the sondes are considerably lower for the retrieved profiles than for the a priori, with the exception of the lowest subcolumn. Once retrieval vertical smoothing (averaging kernels) has been applied to the sonde profiles there is a retrieval bias of 6% (1.5 DU) in the lower troposphere, with smaller biases in the subcolumns above. The bias in the troposphere varies with latitude. The retrieval underestimates lower tropospheric ozone in the Southern Hemisphere (SH) (15–20% or ~ 1–3 DU) and overestimates it in the Northern Hemisphere (NH) (10% or 2 DU). The ability of the retrieval to reflect the geographical distribution of lower tropospheric ozone, globally (rather than just ozonesonde launch sites) is demonstrated by comparison with the chemistry transport model TOMCAT. For a monthly mean of cloud-cleared GOME-2 pixels, a correlation of 0.66 is found between the retrieval and TOMCAT sampled accordingly, with a bias of 0.7 Dobson Units. GOME-2 estimates higher concentrations in NH pollution centres but lower ozone in the Southern Ocean and South Pacific, which is consistent with the comparison to ozonesondes.


2009 ◽  
Vol 9 (14) ◽  
pp. 4621-4638 ◽  
Author(s):  
X. Tie ◽  
S. Madronich ◽  
G. Li ◽  
Z. Ying ◽  
A. Weinheimer ◽  
...  

Abstract. The quantification of tropospheric O3 production in the downwind of the Mexico City plume is a major objective of the MIRAGE-Mex field campaign. We used a regional chemistry-transport model (WRF-Chem) to predict the distribution of O3 and its precursors in Mexico City and the surrounding region during March 2006, and compared the model with in-situ aircraft measurements of O3, CO, VOCs, NOx, and NOy concentrations. The comparison shows that the model is capable of capturing the timing and location of the measured city plumes, and the calculated variability along the flights is generally consistent with the measured results, showing a rapid increase in O3 and its precursors when city plumes are detected. However, there are some notable differences between the calculated and measured values, suggesting that, during transport from the surface of the city to the outflow plume, ozone mixing ratios are underestimated by about 0–25% during different flights. The calculated O3-NOx, O3-CO, and O3-NOz correlations generally agree with the measured values, and the analyses of these correlations suggest that photochemical O3 production continues in the plume downwind of the city (aged plume), adding to the O3 already produced in the city and exported with the plume. The model is also used to quantify the contributions to OH reactivity from various compounds in the aged plume. This analysis suggests that oxygenated organics (OVOCs) have the highest OH reactivity and play important roles for the O3 production in the aging plume. Furthermore, O3 production per NOx molecule consumed (O3 production efficiency) is more efficient in the aged plume than in the young plume near the city. The major contributor to the high O3 production efficiency in the aged plume is the reaction RO2+NO. By contrast, the reaction of HO2+NO is rather uniformly distributed in the plume.


2003 ◽  
Vol 3 (4) ◽  
pp. 1051-1062 ◽  
Author(s):  
P. K. Patra ◽  
S. Lal ◽  
S. Venkataramani ◽  
D. Chand

Abstract. Measurements of methane have been made from various observational platforms in the atmosphere. In this article, we have compared four high precision balloon-borne measurements from Hyderabad (17.5°N), India in the period of 1987 and 1998 with a part of HALOE/UARS global observations available since 1991. All the balloon measurements correspond to boreal spring (March and April) but belong to different years. A comparison shows fairly good agreement with each other. The gradient in CH4 profiles in the troposphere is controlled by the variation in vertical transport. The strongest effect of dynamical influence on methane vertical profiles is shown to be resulting from the dynamical quasi-biennial oscillation in the stratosphere, and that has been consistently derived from both the measurement techniques and chemistry-transport model simulations. It is observed that the QBO signal in CH4 anomaly exhibits interhemispheric asymmetry caused by the tropics to midlatitude circulation in the stratosphere. A mechanism is suggested to explain how and to what extent the methane vertical profiles over Hyderabad and higher latitudes could be modulated by the prevailing QBO winds in the tropics. We have also discussed how the same mechanism would affect ozone distribution in the stratosphere quite differently.


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