scholarly journals Validation of satellite formaldehyde (HCHO) retrievals using observations from 12 aircraft campaigns

2020 ◽  
Vol 20 (20) ◽  
pp. 12329-12345 ◽  
Author(s):  
Lei Zhu ◽  
Gonzalo González Abad ◽  
Caroline R. Nowlan ◽  
Christopher Chan Miller ◽  
Kelly Chance ◽  
...  

Abstract. Formaldehyde (HCHO) has been measured from space for more than 2 decades. Owing to its short atmospheric lifetime, satellite HCHO data are used widely as a proxy of volatile organic compounds (VOCs; please refer to Appendix A for abbreviations and acronyms), providing constraints on underlying emissions and chemistry. However, satellite HCHO products from different satellite sensors using different algorithms have received little validation so far. The accuracy and consistency of HCHO retrievals remain largely unclear. Here we develop a validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns with a chemical transport model (GEOS-Chem) as the intercomparison method. Application to the NASA operational OMI HCHO product indicates negative biases (−44.5 % to −21.7 %) under high-HCHO conditions, while it indicates high biases (+66.1 % to +112.1 %) under low-HCHO conditions. Under both conditions, HCHO a priori vertical profiles are likely not the main driver of the biases. By providing quick assessment of systematic biases in satellite products over large domains, the platform facilitates, in an iterative process, optimization of retrieval settings and the minimization of retrieval biases. It is also complementary to localized validation efforts based on ground observations and aircraft spirals.

2020 ◽  
Author(s):  
Lei Zhu ◽  
Gonzalo González Abad ◽  
Caroline R. Nowlan ◽  
Christopher Chan Miller ◽  
Kelly Chance ◽  
...  

Abstract. Formaldehyde (HCHO) has been measured from space for more than two decades. Owing to its short atmospheric lifetime, satellite HCHO data are used widely as a proxy of volatile organic compounds (VOCs; please refer to Appendix A for abbreviations and acronyms), providing constraints on underlying emissions and chemistry. However, satellite HCHO products from different satellite sensors using different algorithms have received little validation so far. The accuracy and consistency of HCHO retrievals remain largely unclear. Here we develop a global validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns with a chemical transport model (GEOS-Chem) as the intercomparison method. Application to the NASA operational OMI HCHO product indicates slight biases (−30.9 % to +16.0 %) under high-HCHO conditions partially caused by a priori shape factors used in the retrievals, while high biases (+113.9 % to +194.6 %) under low-HCHO conditions due mainly to slant column fitting and radiance reference sector correction. By providing quick assessment to systematic biases in satellite products over large domains, the platform facilitates, in an iterative process, optimization of retrieval settings and the minimization of retrieval biases. It is also complementary to localized validation efforts based on ground observations and aircraft spirals.


2013 ◽  
Vol 13 (12) ◽  
pp. 5887-5905 ◽  
Author(s):  
M. R. Koohkan ◽  
M. Bocquet ◽  
Y. Roustan ◽  
Y. Kim ◽  
C. Seigneur

Abstract. The emissions of non-methane volatile organic compounds (VOCs) over western Europe for the year 2005 are estimated via inverse modelling by assimilation of in situ observations of concentration and then subsequently compared to a standard emission inventory. The study focuses on 15 VOC species: five aromatics, six alkanes, two alkenes, one alkyne and one biogenic diene. The inversion relies on a validated fast adjoint of the chemical transport model used to simulate the fate and transport of these VOCs. The assimilated ground-based measurements over Europe are provided by the European Monitoring and Evaluation Programme (EMEP) network. The background emission errors and the prior observational errors are estimated by maximum-likelihood approaches. The positivity assumption on the VOC emission fluxes is pivotal for a successful inversion, and this maximum-likelihood approach consistently accounts for the positivity of the fluxes. For most species, the retrieved emissions lead to a significant reduction of the bias, which underlines the misfit between the standard inventories and the observed concentrations. The results are validated through a forecast test and a cross-validation test. An estimation of the posterior uncertainty is also provided. It is shown that the statistically consistent non-Gaussian approach based on a reliable estimation of the errors offers the best performance. The efficiency in correcting the inventory depends on the lifetime of the VOCs and the accuracy of the boundary conditions. In particular, it is shown that the use of in situ observations using a sparse monitoring network to estimate emissions of isoprene is inadequate because its short chemical lifetime significantly limits the spatial radius of influence of the monitoring data. For species with a longer lifetime (a few days), successful, albeit partial, emission corrections can reach regions hundreds of kilometres away from the stations. Domain-wide corrections of the emission inventories of some VOCs are significant, with underestimations of the order of a factor of 2 for propane, ethane, ethylene and acetylene.


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>


2020 ◽  
Vol 13 (1) ◽  
pp. 205-218 ◽  
Author(s):  
Iolanda Ialongo ◽  
Henrik Virta ◽  
Henk Eskes ◽  
Jari Hovila ◽  
John Douros

Abstract. We present a comparison between satellite-based TROPOMI (TROPOspheric Monitoring Instrument) NO2 products and ground-based observations in Helsinki (Finland). TROPOMI NO2 total (summed) columns are compared with the measurements performed by the Pandora spectrometer between April and September 2018. The mean relative and absolute bias between the TROPOMI and Pandora NO2 total columns is about 10 % and 0.12×1015 molec. cm−2 respectively. The dispersion of these differences (estimated as their standard deviation) is 2.2×1015 molec. cm−2. 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 (within the retrieval uncertainties) 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. When only the low values of NO2 total columns or the whole dataset are taken into account, the mean bias slightly increases. The change in bias remains mostly within the uncertainties. We also analyse the consistency between satellite-based data and in situ NO2 surface concentrations measured at the Helsinki–Kumpula air quality station (located a few metres from the Pandora spectrometer). We find similar day-to-day variability between TROPOMI, Pandora 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 and the airport area, as well as the effect of the prevailing south-west wind patterns. This is one of the first works in which TROPOMI NO2 retrievals are validated against ground-based observations and the results provide an early evaluation of their applicability for monitoring pollution levels in urban sites. Overall, TROPOMI retrievals are valuable to complement the ground-based air quality data (available with high temporal resolution) for describing the spatio-temporal variability of NO2, even in a relatively small city like Helsinki.


2012 ◽  
Vol 12 (12) ◽  
pp. 33219-33263 ◽  
Author(s):  
M. R. Koohkan ◽  
M. Bocquet ◽  
Y. Roustan ◽  
Y. Kim ◽  
C. Seigneur

Abstract. The emission of volatile organic compounds (VOCs) over western Europe for the year 2005 are estimated via inverse modelling, by assimilation of in situ observations of concentration and compared to a standard emission inventory. The study focuses on fifteen VOC species: five aromatics, six alkanes, two alkenes, one alkyne and one biogenic diene. The inversion relies on a validated fast adjoint of the chemistry transport model used to simulate the fate and transport of these VOCs. The assimilated ground-based measurements over Europe are provided by the European Monitoring and Evaluation Programme (EMEP) network. The background emissions errors and the prior observational errors are estimated by maximum likelihood approaches. The positivity assumptions on the VOC emission fluxes is pivotal for a successful inversion and this maximum likelihood approach consistently accounts for the positivity of the fluxes. For most species, the retrieval leads to a significant reduction of the bias, which underlines the misfit between the standard inventories and the observed concentrations. The results are validated through a forecast test and a cross-validation test. It is shown that the statistically consistent non-Gaussian approach based on a reliable estimation of the errors offers the best performance. The efficiency in correcting the inventory depends on the lifetime of the VOCs. In particular, it is shown that the use of in-situ observations using a sparse monitoring network to estimate emissions of isoprene is inadequate because its short chemical lifetime significantly limits the spatial radius of influence of the monitoring data. For species with longer lifetime (a few days), successful, albeit partial, emission corrections can reach regions hundreds of kilometres away from the stations. Domainwide corrections of the emissions inventories of some VOCs are significant, with underestimations on order of a factor of two of propane, ethane, ethylene and acetylene.


2014 ◽  
Vol 14 (9) ◽  
pp. 4617-4641 ◽  
Author(s):  
E. Saikawa ◽  
R. G. Prinn ◽  
E. Dlugokencky ◽  
K. Ishijima ◽  
G. S. Dutton ◽  
...  

Abstract. We present a comprehensive estimate of nitrous oxide (N2O) emissions using observations and models from 1995 to 2008. High-frequency records of tropospheric N2O are available from measurements at Cape Grim, Tasmania; Cape Matatula, American Samoa; Ragged Point, Barbados; Mace Head, Ireland; and at Trinidad Head, California using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. The Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also collected discrete air samples in flasks and in situ measurements from remote sites across the globe and analyzed them for a suite of species including N2O. In addition to these major networks, we include in situ and aircraft measurements from the National Institute of Environmental Studies (NIES) and flask measurements from the Tohoku University and Commonwealth Scientific and Industrial Research Organization (CSIRO) networks. All measurements show increasing atmospheric mole fractions of N2O, with a varying growth rate of 0.1–0.7% per year, resulting in a 7.4% increase in the background atmospheric mole fraction between 1979 and 2011. Using existing emission inventories as well as bottom-up process modeling results, we first create globally gridded a priori N2O emissions over the 37 years since 1975. We then use the three-dimensional chemical transport model, Model for Ozone and Related Chemical Tracers version 4 (MOZART v4), and a Bayesian inverse method to estimate global as well as regional annual emissions for five source sectors from 13 regions in the world. This is the first time that all of these measurements from multiple networks have been combined to determine emissions. Our inversion indicates that global and regional N2O emissions have an increasing trend between 1995 and 2008. Despite large uncertainties, a significant increase is seen from the Asian agricultural sector in recent years, most likely due to an increase in the use of nitrogenous fertilizers, as has been suggested by previous studies.


2013 ◽  
Vol 13 (7) ◽  
pp. 19471-19525 ◽  
Author(s):  
E. Saikawa ◽  
R. G. Prinn ◽  
E. Dlugokencky ◽  
K. Ishijima ◽  
G. S. Dutton ◽  
...  

Abstract. We present a comprehensive estimate of nitrous oxide ( N2O) emissions using observations and models from 1995 to 2008. High-frequency records of tropospheric N2O are available from measurements at Cape Grim, Tasmania; Cape Matatula, American Samoa; Ragged Point, Barbados; Mace Head, Ireland; and at Trinidad Head, California using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. The Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also discrete air samples collected in flasks and in situ measurements from remote sites across the globe and analyzed them for a suite of species including N2O. In addition to these major networks, we include in situ and aircraft measurements from the National Institute for Environmental Studies (NIES) and flask measurements from the Tohoku University and Commonwealth Scientific and Industrial Research Organization (CSIRO) networks. All measurements show increasing atmospheric mole fractions of N2O, with a varying growth rate of 0.1–0.7 % yr-1, resulting in a 7.4% increase in the background atmospheric mole fraction between 1979 and 2011. Using existing emission inventories as well as bottom-up process modeling results, we first create globally-gridded a priori N2O emissions over the 37 yr since 1975. We then use the three-dimensional chemical transport model, Model for Ozone and Related Chemical Tracers version 4 (MOZART v4), and a Bayesian inverse method to estimate global as well as regional annual emissions for five source sectors from 13 regions in the world. This is the first time that all of these measurements from multiple networks have been combined to determine emissions. Our inversion indicates that global and regional N2O emissions have an increasing trend between 1995 and 2008. Despite large uncertainties, a significant increase is seen from the Asian agricultural sector in the recent years, most likely due to an increase in the use of nitrogenous fertilizers, as has been suggested by previous studies, and also in Asian natural soil.


2009 ◽  
Vol 9 (5) ◽  
pp. 19967-20018 ◽  
Author(s):  
M. Kopacz ◽  
D. J. Jacob ◽  
J. A. Fisher ◽  
J. A. Logan ◽  
L. Zhang ◽  
...  

Abstract. We combine CO column measurements from the MOPITT, AIRS, SCIAMACHY, and TES satellite instruments in a full-year (May 2004–April 2005) global inversion of CO sources at 4°×5° spatial resolution and monthly temporal resolution. The inversion uses the GEOS-Chem chemical transport model (CTM) and its adjoint applied to MOPITT, AIRS, and SCIAMACHY. Observations from TES, surface sites (NOAA/GMD), and aircraft (MOZAIC) are used for evaluation of the a posteriori solution. Global intercomparison of the different satellite datasets using GEOS-Chem as a common intercomparison platform shows consistency between the satellite datasets and with the in situ data. The majority of the differences between the datasets can be explained by different averaging kernels and a priori information. The global CO emission from combustion as constrained in the inversion is 1350 Tg a−1, with an additional 217 Tg a−1 from oxidation of co-emitted VOCs. This is much higher than current bottom-up emission inventories. Consistent with both the satellite and in situ data, a large fraction of the correction results from a seasonal underestimate of CO sources at northern mid-latitudes and suggests a larger-than-expected CO source from vehicle cold starts and residential heating. A posteriori emissions also indicate a general underestimation of biomass burning relative to the GFED2 inventory. However, the tropical biomass burning constraints are not consistent across the different datasets. Although the datasets reveal regional inconsistencies over tropical biomass burning regions, we find the global emission estimates to be a balance of information from all three instruments.


2019 ◽  
Author(s):  
Iolanda Ialongo ◽  
Henrik Virta ◽  
Henk Eskes ◽  
Jari Hovila ◽  
John Douros

Abstract. We present a comparison between satellite-based TROPOMI (TROPOspheric Monitoring Instrument) NO2 products and 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. We find a 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 km x 7 km) and the a-priori used in the retrieval compared to the relatively small field-of-view of the Pandora instrument. 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. We also analyse the consistency between satellite-based data and in situ NO2 surface concentrations measured at the Helsinki-Kumpula air quality station (located a few metres from the Pandora spectrometer). We find similar day-to-day variability between TROPOMI, Pandora 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 and the airport area, as well as the effect of the prevailing south-west wind patterns. This is one of the first works in which TROPOMI NO2 retrievals are validated against ground-based observations and the results provide an early evaluation of their applicability for monitoring pollution levels in urban sites. Overall, TROPOMI retrievals are valuable to complement the ground-based air quality data (available with high temporal resolution) for describing the spatio-temporal variability of NO2, even in a relatively small city like Helsinki.


2011 ◽  
Vol 11 (17) ◽  
pp. 9253-9269 ◽  
Author(s):  
J. Angelbratt ◽  
J. Mellqvist ◽  
D. Simpson ◽  
J. E. Jonson ◽  
T. Blumenstock ◽  
...  

Abstract. Trends in the CO andC2H6 partial columns ~0–15 km) have been estimated from four European ground-based solar FTIR (Fourier Transform InfraRed) stations for the 1996–2006 time period. The CO trends from the four stations Jungfraujoch, Zugspitze, Harestua and Kiruna have been estimated to −0.45 ± 0.16% yr−1, −1.00 ± 0.24% yr−1, −0.62 ± 0.19 % yr−1 and −0.61 ± 0.16% yr−1, respectively. The corresponding trends for C2H6 are −1.51 ± 0.23% yr−1, −2.11 ± 0.30% yr−1, −1.09 ± 0.25% yr−1 and −1.14 ± 0.18% yr−1. All trends are presented with their 2-σ confidence intervals. To find possible reasons for the CO trends, the global-scale EMEP MSC-W chemical transport model has been used in a series of sensitivity scenarios. It is shown that the trends are consistent with the combination of a 20% decrease in the anthropogenic CO emissions seen in Europe and North America during the 1996–2006 period and a 20% increase in the anthropogenic CO emissions in East Asia, during the same time period. The possible impacts of CH4 and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the measured CO and C2H6 partial columns from Jungfraujoch, Zugspitze, Bremen, Harestua, Kiruna and Ny-Ålesund. The European model reproduces, on average the measurements at the different sites fairly well and within 10–22% deviation for CO and 14–31% deviation for C2H6. Their seasonal amplitude is captured within 6–35% and 9–124% for CO and C2H6, respectively. However, 61–98% of the CO and C2H6 partial columns in the European model are shown to arise from the boundary conditions, making the global-scale model a more suitable alternative when modeling these two species. In the evaluation of the global model the average partial columns for 2006 are shown to be within 1–9% and 37–50% of the measurements for CO and C2H6, respectively. The global model sensitivity for assumptions made in this paper is also analyzed.


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