scholarly journals Estimating NOx LOTOS-EUROS CTM Emission Parameters over the Northwest of South America through 4DEnVar TROPOMI NO2 Assimilation

Atmosphere ◽  
2021 ◽  
Vol 12 (12) ◽  
pp. 1633
Author(s):  
Andrés Yarce Botero ◽  
Santiago Lopez-Restrepo ◽  
Nicolás Pinel Peláez ◽  
Olga L. Quintero ◽  
Arjo Segers ◽  
...  

In this work, we present the development of a 4D-Ensemble-Variational (4DEnVar) data assimilation technique to estimate NOx top-down emissions using the regional chemical transport model LOTOS-EUROS with the NO2 observations from the TROPOspheric Monitoring Instrument (TROPOMI). The assimilation was performed for a domain in the northwest of South America centered over Colombia, and includes regions in Panama, Venezuela and Ecuador. In the 4DEnVar approach, the implementation of the linearized and adjoint model are avoided by generating an ensemble of model simulations and by using this ensemble to approximate the nonlinear model and observation operator. Emission correction parameters’ locations were defined for positions where the model simulations showed significant discrepancies with the satellite observations. Using the 4DEnVar data assimilation method, optimal emission parameters for the LOTOS-EUROS model were estimated, allowing for corrections in areas where ground observations are unavailable and the region’s emission inventories do not correctly reflect the current emissions activities. The analyzed 4DEnVar concentrations were compared with the ground measurements of one local air quality monitoring network and the data retrieved by the satellite instrument Ozone Monitoring Instrument (OMI). The assimilation had a low impact on NO2 surface concentrations reducing the Mean Fractional Bias from 0.45 to 0.32, primordially enhancing the spatial and temporal variations in the simulated NO2 fields.

Atmosphere ◽  
2021 ◽  
Vol 12 (1) ◽  
pp. 91
Author(s):  
Santiago Lopez-Restrepo ◽  
Andres Yarce ◽  
Nicolás Pinel ◽  
O.L. Quintero ◽  
Arjo Segers ◽  
...  

The use of low air quality networks has been increasing in recent years to study urban pollution dynamics. Here we show the evaluation of the operational Aburrá Valley’s low-cost network against the official monitoring network. The results show that the PM2.5 low-cost measurements are very close to those observed by the official network. Additionally, the low-cost allows a higher spatial representation of the concentrations across the valley. We integrate low-cost observations with the chemical transport model Long Term Ozone Simulation-European Operational Smog (LOTOS-EUROS) using data assimilation. Two different configurations of the low-cost network were assimilated: using the whole low-cost network (255 sensors), and a high-quality selection using just the sensors with a correlation factor greater than 0.8 with respect to the official network (115 sensors). The official stations were also assimilated to compare the more dense low-cost network’s impact on the model performance. Both simulations assimilating the low-cost model outperform the model without assimilation and assimilating the official network. The capability to issue warnings for pollution events is also improved by assimilating the low-cost network with respect to the other simulations. Finally, the simulation using the high-quality configuration has lower error values than using the complete low-cost network, showing that it is essential to consider the quality and location and not just the total number of sensors. Our results suggest that with the current advance in low-cost sensors, it is possible to improve model performance with low-cost network data assimilation.


2021 ◽  
Author(s):  
Takashi Sekiya ◽  
Kazuyuki Miyazaki ◽  
Henk Eskes ◽  
Kengo Sudo ◽  
Masayuki Takigawa ◽  
...  

Abstract. This study gives a systematic comparison of the Tropospheric Monitoring Instrument (TROPOMI) version 1.2 and Ozone Monitoring Instrument (OMI) QA4ECV tropospheric NO2 column through global chemical data assimilation (DA) integration for the period April−May 2018. DA performance is controlled by measurement sensitivities, retrieval errors, and coverage. The smaller mean relative observation errors by 16 % in TROPOMI than OMI over 60° N−60° S during April−May 2018 led to larger reductions in the global root mean square error (RMSE) against the assimilated NO2 measurements in TROPOMI DA (by 54 %) than in OMI DA (by 38 %). Agreements against the independent surface, aircraft-campaign, and ozonesonde observation data were also improved by TROPOMI DA compared to the control model simulation (by 12−84 % for NO2 and by 7−40 % for ozone), which were more obvious than those by OMI DA for many cases (by 2−70 % for NO2 and by 1−22 % for ozone). The estimated global total NOx emissions were 15 % lower in TROPOMI DA, with 2−23 % smaller regional total emissions, in line with the observed negative bias of the TROPOMI version 1.2 product compared to the OMI QA4ECV product. TROPOMI DA can provide city scale emission estimates, which were within 10 % differences with other high-resolution analyses for several limited areas, while providing a globally consistent analysis. These results demonstrate that TROPOMI DA improves global analyses of NO2 and ozone, which would also benefit studies on detailed spatial and temporal variations in ozone and nitrate aerosols and the evaluation of bottom-up NOx emission inventories.


2021 ◽  
Vol 14 (1) ◽  
pp. 27-42
Author(s):  
Jianglong Zhang ◽  
Robert J. D. Spurr ◽  
Jeffrey S. Reid ◽  
Peng Xian ◽  
Peter R. Colarco ◽  
...  

Abstract. Using the Vector LInearized Discrete Ordinate Radiative Transfer (VLIDORT) code as the main driver for forward model simulations, a first-of-its-kind data assimilation scheme has been developed for assimilating Ozone Monitoring Instrument (OMI) aerosol index (AI) measurements into the Naval Aerosol Analysis and Predictive System (NAAPS). This study suggests that both root mean square error (RMSE) and absolute errors can be significantly reduced in NAAPS analyses with the use of OMI AI data assimilation when compared to values from NAAPS natural runs. Improvements in model simulations demonstrate the utility of OMI AI data assimilation for aerosol model analysis over cloudy regions and bright surfaces. However, the OMI AI data assimilation alone does not outperform aerosol data assimilation that uses passive-based aerosol optical depth (AOD) products over cloud-free skies and dark surfaces. Further, as AI assimilation requires the deployment of a fully multiple-scatter-aware radiative transfer model in the forward simulations, computational burden is an issue. Nevertheless, the newly developed modeling system contains the necessary ingredients for assimilation of radiances in the ultraviolet (UV) spectrum, and our study shows the potential of direct radiance assimilation at both UV and visible spectrums, possibly coupled with AOD assimilation, for aerosol applications in the future. Additional data streams can be added, including data from the TROPOspheric Monitoring Instrument (TROPOMI), the Ozone Mapping and Profiler Suite (OMPS), and eventually the Plankton, Aerosol, Cloud and ocean Ecosystem (PACE) mission.


2012 ◽  
Vol 12 (20) ◽  
pp. 9545-9579 ◽  
Author(s):  
K. Miyazaki ◽  
H. J. Eskes ◽  
K. Sudo ◽  
M. Takigawa ◽  
M. van Weele ◽  
...  

Abstract. We have developed an advanced chemical data assimilation system to combine observations of chemical compounds from multiple satellites. NO2, O3, CO, and HNO3 measurements from the Ozone Monitoring Instrument (OMI), Tropospheric Emission Spectrometer (TES), Measurement of Pollution in the Troposphere (MOPITT), and Microwave Limb Sounder (MLS) satellite instruments are assimilated into the global chemical transport model CHASER for the years 2006–2007. The CHASER data assimilation system (CHASER-DAS), based on the local ensemble transform Kalman filter technique, simultaneously optimizes the chemical species, as well as the emissions of O3 precursors, while taking their chemical feedbacks into account. With the available datasets, an improved description of the chemical feedbacks can be obtained, especially related to the NOx-CO-OH-O3 set of chemical reactions. Comparisons against independent satellite, aircraft, and ozonesonde data show that the data assimilation results in substantial improvements for various chemical compounds. These improvements include a reduced negative tropospheric NO2 column bias (by 40–85%), a reduced negative CO bias in the Northern Hemisphere (by 40–90%), and a reduced positive O3 bias in the middle and upper troposphere (from 30–40% to within 10%). These changes are related to increased tropospheric OH concentrations by 5–15% in the tropics and the Southern Hemisphere in July. Observing System Experiments (OSEs) have been conducted to quantify the relative importance of each data set on constraining the emissions and concentrations. The OSEs confirm that the assimilation of individual data sets results in a strong influence on both assimilated and non-assimilated species through the inter-species error correlation and the chemical coupling described by the model. The simultaneous adjustment of the emissions and concentrations is a powerful approach to correcting the tropospheric ozone budget and profile analyses.


2021 ◽  
Vol 21 (3) ◽  
pp. 1759-1774
Author(s):  
Maria-Elissavet Koukouli ◽  
Ioanna Skoulidou ◽  
Andreas Karavias ◽  
Isaak Parcharidis ◽  
Dimitris Balis ◽  
...  

Abstract. The unprecedented order, in modern peaceful times, for a near-total lockdown of the Greek population as a means of protection against severe acute respiratory syndrome coronavirus 2, commonly known as COVID-19, has generated unintentional positive side-effects with respect to the country's air quality levels. Sentinel-5 Precursor/Tropospheric Monitoring Instrument (S5P/TROPOMI) monthly mean tropospheric nitrogen dioxide (NO2) observations show an average change of −34 % to +20 % and −39 % to −5 % with an average decrease of −15 % and −11 % for March and April 2020 respectively, compared with the previous year, over the six larger Greek metropolitan areas; this is mostly attributable to vehicular emission reductions. For the capital city of Athens, weekly analysis was statistically possible for the S5P/TROPOMI observations and revealed a marked decline in the NO2 load of between −8 % and −43 % for 7 of the 8 weeks studied; this is in agreement with the equivalent Ozone Monitoring Instrument (OMI)/Aura observations as well as the ground-based estimates of a multi-axis differential optical absorption spectroscopy ground-based instrument. Chemical transport modelling of the NO2 columns, provided by the Long Term Ozone Simulation European Operational Smog (LOTOS-EUROS) chemical transport model, shows that the magnitude of these reductions cannot solely be attributed to the difference in meteorological factors affecting NO2 levels during March and April 2020 and the equivalent time periods of the previous year. Taking this factor into account, the resulting decline was estimated to range between ∼ −25 % and −65 % for 5 of the 8 weeks studied, with the remaining 3 weeks showing a positive average of ∼ 10 %; this positive average was postulated to be due to the uncertainty of the methodology, which is based on differences. As a result this analysis, we conclude that the effect of the COVID-19 lockdown and the restriction of transport emissions over Greece is ∼ −10 %. As transport is the second largest sector (after industry) affecting Greece's air quality, this occasion may well help policymakers to enforce more targeted measures to aid Greece in further reducing emissions according to international air quality standards.


Atmosphere ◽  
2021 ◽  
Vol 12 (7) ◽  
pp. 900
Author(s):  
Ioanna Skoulidou ◽  
Maria-Elissavet Koukouli ◽  
Arjo Segers ◽  
Astrid Manders ◽  
Dimitris Balis ◽  
...  

In this work, we investigate the ability of a data assimilation technique and space-borne observations to quantify and monitor changes in nitrogen oxides (NOx) emissions over Northwestern Greece for the summers of 2018 and 2019. In this region, four lignite-burning power plants are located. The data assimilation technique, based on the Ensemble Kalman Filter method, is employed to combine space-borne atmospheric observations from the high spatial resolution Sentinel-5 Precursor (S5P) Tropospheric Monitoring Instrument (TROPOMI) and simulations using the LOTOS-EUROS Chemical Transport model. The Copernicus Atmosphere Monitoring Service-Regional European emissions (CAMS-REG, version 4.2) inventory based on the year 2015 is used as the a priori emissions in the simulations. Surface measurements of nitrogen dioxide (NO2) from air quality stations operating in the region are compared with the model surface NO2 output using either the a priori (base run) or the a posteriori (assimilated run) NOx emissions. Relative to the a priori emissions, the assimilation suggests a strong decrease in concentrations for the station located near the largest power plant, by 80% in 2019 and by 67% in 2018. Concerning the estimated annual a posteriori NOx emissions, it was found that, for the pixels hosting the two largest power plants, the assimilated run results in emissions decreased by ~40–50% for 2018 compared to 2015, whereas a larger decrease, of ~70% for both power plants, was found for 2019, after assimilating the space-born observations. For the same power plants, the European Pollutant Release and Transfer Register (E-PRTR) reports decreased emissions in 2018 and 2019 compared to 2015 (−35% and −38% in 2018, −62% and −72% in 2019), in good agreement with the estimated emissions. We further compare the a posteriori emissions to the reported energy production of the power plants during the summer of 2018 and 2019. Mean decreases of about −35% and−63% in NOx emissions are estimated for the two larger power plants in summer of 2018 and 2019, respectively, which are supported by similar decreases in the reported energy production of the power plants (~−30% and −70%, respectively).


2012 ◽  
Vol 12 (15) ◽  
pp. 7073-7085 ◽  
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
G. Nikulin ◽  
M. L. Santee ◽  
...  

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.


2011 ◽  
Vol 11 (24) ◽  
pp. 12773-12786 ◽  
Author(s):  
S. Dhomse ◽  
M. P. Chipperfield ◽  
W. Feng ◽  
J. D. Haigh

Abstract. We have used an off-line 3-D chemical transport model (CTM) to investigate the 11-yr solar cycle response in tropical stratospheric ozone. The model is forced with European Centre for Medium-Range Weather Forecasts (ECMWF) (re)analysis (ERA-40/operational and ERA-Interim) data for the 1979–2005 time period. We have compared the modelled solar response in ozone to observation-based data sets that are constructed using satellite instruments such as Total Ozone Mapping Spectrometer (TOMS), Solar Backscatter UltraViolet instrument (SBUV), Stratospheric Aerosol and Gas Experiment (SAGE) and Halogen Occultation Experiment (HALOE). A significant difference is seen between simulated and observed ozone during the 1980s, which is probably due to inhomogeneities in the ERA-40 reanalyses. In general, the model with ERA-Interim dynamics shows better agreement with the observations from 1990 onwards than with ERA-40. Overall both standard model simulations are partially able to simulate a "double peak"-structured ozone solar response with a minimum around 30 km, and these are in better agreement with HALOE than SAGE-corrected SBUV (SBUV/SAGE) or SAGE-based data sets. In the tropical lower stratosphere (TLS), the modelled solar response with time-varying aerosols is amplified through aliasing with a volcanic signal, as the model overestimates ozone loss during high aerosol loading years. However, the modelled solar response with fixed dynamics and constant aerosols shows a positive signal which is in better agreement with SBUV/SAGE and SAGE-based data sets in the TLS. Our model simulations suggests that photochemistry contributes to the ozone solar response in this region. The largest model-observation differences occur in the upper stratosphere where SBUV/SAGE and SAGE-based data show a significant (up to 4%) solar response whereas the standard model and HALOE do not. This is partly due to a positive solar response in the ECMWF upper stratospheric temperatures which reduces the modelled ozone signal. The large positive upper stratospheric solar response seen in SBUV/SAGE and SAGE-based data can be reproduced in model runs with fixed dynamical fields (i.e. no inter-annual meteorological changes). As these runs effectively assume no long-term temperature changes (solar-induced or otherwise), it should provide an upper limit of the ozone solar response. Overall, full quantification of the solar response in stratospheric ozone is limited by differences in the observed data sets and by uncertainties in the solar response in stratospheric temperatures.


2009 ◽  
Vol 9 (14) ◽  
pp. 5281-5297 ◽  
Author(s):  
I. Pison ◽  
P. Bousquet ◽  
F. Chevallier ◽  
S. Szopa ◽  
D. Hauglustaine

Abstract. In order to study the spatial and temporal variations of the emissions of greenhouse gases and of their precursors, we developed a data assimilation system and applied it to infer emissions of CH4, CO and H2 for one year. It is based on an atmospheric chemical transport model and on a simplified scheme for the oxidation chain of hydrocarbons, including methane, formaldehyde, carbon monoxide and molecular hydrogen together with methyl chloroform. The methodology is exposed and a first attempt at evaluating the inverted fluxes is made. Inversions of the emission fluxes of CO, CH4 and H2 and concentrations of HCHO and OH were performed for the year 2004, using surface concentration measurements of CO, CH4, H2 and CH3CCl3 as constraints. Independent data from ship and aircraft measurements and satellite retrievals are used to evaluate the results. The total emitted mass of CO is 30% higher after the inversion, due to increased fluxes by up to 35% in the Northern Hemisphere. The spatial distribution of emissions of CH4 is modified by a decrease of fluxes in boreal areas up to 60%. The comparison between mono- and multi-species inversions shows that the results are close at a global scale but may significantly differ at a regional scale because of the interactions between the various tracers during the inversion.


2020 ◽  
Author(s):  
Yuanhong Zhao ◽  
Marielle Saunois ◽  
Philippe Bousquet ◽  
Xin Lin ◽  
Antoine Berchet ◽  
...  

Abstract. The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role to close the global methane budget. Previous research that assessed the impact of OH changes on the CH4 budget mostly relied on box modeling inversions with a very simplified atmospheric transport and no representation of the heterogeneous spatial distribution of OH radicals. Here using a variational Bayesian inversion framework and a 3D chemical transport model, LMDz, combined with 10 different OH fields derived from chemistry-climate models (CCMI experiment), we evaluate the influence of OH burden, spatial distribution, and temporal variations on the global CH4 budget. The global tropospheric mean CH4-reaction-weighted [OH] ([OH]GM-CH4) ranges 10.3–16.3 × 105 molec cm−3 across 10 OH fields during the early 2000s, resulting in inversion-based global CH4 emissions between 518 and 757 Tg yr−1. The uncertainties in CH4 inversions induced by the different OH fields are comparable to, or even larger than the uncertainty typically given by bottom-up and top-down estimates. Based on the LMDz inversions, we estimate that a 1 %-increase in OH burden leads to an increase of 4 Tg yr−1 in the estimate of global methane emissions, which is about 25 % smaller than what is estimated by box-models. The uncertainties in emissions induced by OH are largest over South America, corresponding to large inter-model differences of [OH] in this region. From the early to the late 2000s, the optimized CH4 emissions increased by 21.9 ± 5.7 Tg yr−1 (16.6–30.0 Tg yr−1), of which ~ 25 % (on average) is contributed by −0.5 to +1.8 % increase in OH burden. If the CCMI models represent the OH trend properly over the 2000s, our results show that a higher increasing trend of CH4 emissions is needed to match the CH4 observations compared to the CH4 emission trend derived using constant OH. This study strengthens the importance to reach a better representation of OH burden and of OH spatial and temporal distributions to reduce the uncertainties on the global CH4 budget.


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