Intercomparison of NO x emission inventories over East Asia

We compare nine emission inventories of nitrogen oxides including four satellite-derived NOx inventories and the following bottom-up inventories for East Asia: REAS (Regional Emission inventory in ASia), MEIC (Multi-resolution Emission Inventory for China), CAPSS (Clean Air Policy Support System) and EDGAR (Emissions Database for Global Atmospheric Research). Two of the satellite-derived inventories are estimated by using the DECSO (Daily Emission derived Constrained by Satellite Observations) algorithm, which is based on an extended Kalman filter applied to observations from OMI or from GOME-2. The other two are derived with the EnKF algorithm, which is based on an ensemble Kalman filter applied to observations of multiple species using either the chemical transport model CHASER and MIROC-chem. The temporal behaviour and spatial distribution of the inventories are compared on a national and regional scale. A distinction is also made between urban and rural areas. The intercomparison of all inventories shows good agreement in total NOx emissions over mainland China, especially for trends, with an average bias of about 20 % for yearly emissions. All the inventories show the typical emission reduction of 10 % during the Chinese New Year and a peak in December. Satellite-derived approaches using OMI show a summer peak due to strong emissions from soil and biomass burning in this season. Biases in NOx emissions and uncertainties in temporal variability increase quickly when the spatial scale decreases. The analyses of the differences show the importance of using observations from multiple instruments and a high spatial resolution model for the satellite-derived inventories, while for bottom-up inventories, accurate emission factors and activity information are required. The advantage of the satellite-derived approach is that the emissions are soon available after observation, while the strength of the bottom-up inventories is that they include detailed information of emissions for each source category.

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abstract: ERA-Interim is the latest global atmospheric reanalysis produced by the European Centre for Medium-Range Weather Forecasts (ECMWF). The ERA-Interim project was conducted in part to prepare for a new atmospheric reanalysis to replace ERA-40, which will extend back to the early part of the twentieth century. This article describes the forecast model, data assimilation method, and input datasets used to produce ERA-Interim, and discusses the performance of the system. Special emphasis is placed on various difficulties encountered in the production of ERA-40, including the representation of the hydrological cycle, the quality of the stratospheric circulation, and the consistency in time of the reanalysed fields. We provide evidence for substantial improvements in each of these aspects. We also identify areas where further work is needed and describe opportunities and objectives for future reanalysis projects at ECMWF.

title: NOx emission estimates during the 2014 Youth Olympic Games in Nanjing (discussion paper)
abstract: The Nanjing Government has taken temporary environmental regulations to guarantee good air quality during the Youth Olympic Games (YOG) in 2014. We study the effect of those regulations by applying the emission estimate algorithm DECSO (Daily Emission estimates Constrained by Satellite Observations) to measurements of the Ozone Monitoring Instrument (OMI). We improved DECSO by updating the chemical transport model CHIMERE from v2006 to v2013 and by adding an Observation minus Forecast (OmF) criterion to filter outlying satellite retrievals due to high aerosol concentrations. The comparison of model results with both ground and satellite observations indicates that CHIMERE v2013 is better performing than CHIMERE v2006. After filtering the satellite observations with high aerosol loads that were leading to large OmF values, unrealistic jumps in the emission estimates are removed. Despite the cloudy conditions during the YOG we could still see a decrease of tropospheric NO2 column concentrations of about 32% in the OMI observations as compared to the average NO2 concentrations from 2005 to 2012. The results of the improved DECSO algorithm for NOx emissions show a reduction of at least 25% during the YOG period. This indicates that air quality regulations taken by the local government were successful. The algorithm is also able to detect an emission reduction of 10% during the Chinese Spring Festival. This study demonstrates the capacity of the DECSO algorithm to capture the change of NOx emissions on a monthly scale. We also show that the observed concentrations and the derived emissions show different patterns that provide complimentary information. For example, the Nanjing smog episode in December 2013 led to a strong increase in NO2 concentrations without an increase in NOx emissions. Furthermore, DECSO gives us important information of the non-trivial seasonal relation between NOx emissions and NO2 concentrations on a local scale.

title: Constraints on surface NOx emissions by assimilating satellite observations of multiple species
abstract: Surface NOx emissions are estimated by a combined assimilation of satellite observations of NO2, CO, O3, and HNO3 with a global chemical transport model. The assimilation of measurements for species other than NO2 provides additional constraints on the NOx emissions by adjusting the concentrations of the species affecting the NOx chemistry and leads to changes in the regional monthly-mean emissions of −58 to +32% and the annual total emissions of −16 to +3%. These large changes highlight that uncertainties in the model chemistry impact the quality of the emission estimates. In the inversion from NO2 observations only, NOx analysis increments occur closer to the surface. Because of the shorter residence time, larger emissions increments are required compared to the multiple species assimilation. Validation against independent observations and comparisons with the recent Regional Emission inventory in Asia version 2.1 emissions shows that the multiple species assimilation improves the chemical consistency including the relation between concentrations and the estimated emissions.

title: Global emission inventories in the Emission Database for Global Atmospheric Research (EDGAR) – Manual (I) I. Gridding: EDGAR emissions distribution on global gridmaps
abstract: The Emissions Database for Global Atmospheric Research EDGAR, version 4 is managed at a JRC-server and documented with an emipedia website. The final resulting datasets of sector-specific emission inventories for all world countries and the resulting gridmaps have been published for all greenhouse gases and air pollutants and PM10 particulate matter on edgar.jrc.ec.europa.eu. These are accompanied so far with a description online, which is then worked out in more detail in the EDGAR Manual series. A first part of the EDGAR Manual series is this report "Gridding: EDGAR emissions distribution on global gridmaps". The report documents all geospatial surrogates that were collected, mainly from publicly available information sources, which were manipulated to arrive to a full set of consistent proxy data with spatial resolution of 0.1degx0.1deg. The set of a hundred proxy datasets are applied to all EDGARv4 emissions yielding the sector-specific global emission gridmaps for all substances. Except for population and the derived urban and rural population proxy datasets, the proxy do not change over time. The population proxy, taken from CIESIN is an important default for the gridding and changes over time, reflecting the migration of people. More in particular the urban population proxy, derived in-house based on a combination of population and urban settlements, the urbanisation process over the past two decades is taken up. All spatial datasets are two-dimensional, covering the globe, except for aviation. The airline distribution occurs with three distinct layers at different heights, in order to cover a minimum third dimension. The other emissions data are upon request split into two height layers, one at stack height, one at ground level, based on the type of activity. The global coverage and geospatial consistency allow to provide a consistent input to the atmospheric chemistry. In particular multipollutant sources are represented as one single point source. The usefulness of these proxy datasets is reflected by the requests for applying it on other emission inventories, such as the UNEP emissions from IIASA or the EMEP emissions at CEIP.

title: Forty years of improvements in European air quality: regional policy-industry interactions with global impacts
abstract: The EDGAR (Emissions Database for Global Atmospheric Research) v4.3 global anthropogenic emissions inventory of several gaseous (SO2, NOx, CO, non-methane volatile organic compounds (NMVOCs) and NH3) and particulate (PM10, PM2.5, black and organic carbon (BC and OC)) air pollutants for the period 1970–2010 is used to develop retrospective air pollution emission scenarios to quantify the roles and contributions of changes in fuels consumption, technology, end-of-pipe emission reduction measures and their resulting impact on health and crop yields. This database presents changes in activity data, fuels and air pollution abatement technology for the past 4 decades, using international statistics and following guidelines for bottom-up emission inventory at the Tier 1 and Tier 2 levels with region-specific default values. 

With two further retrospective scenarios we assess (1) the impact of the technology and end-of-pipe (EOP) reduction measures in the European Union (EU) by considering a stagnation of technology with constant emission factors from 1970 and with no further abatement measures and improvement in European emissions standards, but fuel consumption occurring at historical pace, and (2) the impact of increased fuel consumption by considering unchanged energy use with constant fuel consumption since 1970, but technological development and end-of-pipe reductions. Our scenario analysis focuses on the three most important and most regulated sectors (power generation, the manufacturing industry and road transport), which are subject of multi-pollutant EU Air Quality regulations. 

If technology and European EOP reduction measures had stagnated at 1970 levels, EU air quality in 2010 would have suffered from 129 % higher SO2, 71 % higher NOx and 69 % higher PM2.5 emissions, demonstrating the large role of technology in reducing emissions in 2010. However, if fuel consumption had remained constant starting in 1970, the EU would have benefited from current technology and emission control standards, with reductions in NOx by even 13 % more. Such further savings are not observed for SO2 and PM2.5. If the EU consumed the same amount of fuels as in 1970 but with the current technology and emission control standards, then the emissions of SO2 and PM2.5 would be 42 % respectively 10 % higher. This scenario shows the importance for air quality of abandoning heavy residual fuel oil and shifting fuel types (from, e.g., coal to gas) in the EU. 

A reduced-form TM5-FASST (Fast Screening Scenario Tool based on the global chemical Transport Model 5) is applied to calculate regional and global levels of aerosol and ozone concentrations and to assess the impact of air quality improvements on human health and crop yield loss, showing substantial impacts of export of EU technologies and standards to other world regions.

title: CHIMERE 2013 : a model for regional atmospheric composition modelling
abstract: Tropospheric trace gas and aerosol pollutants have adverse effects on health, environment and climate. In order to quantify and mitigate such effects, a wide range of processes leading to the formation and transport of pollutants must be considered, understood and represented in numerical models. Regional scale pollution episodes result from the combination of several factors: high emissions (from anthropogenic or natural sources), stagnant meteorological conditions, kinetics and efficiency of the chemistry and the deposition. All these processes are highly variable in time and space, and their relative contribution to the pollutants budgets can be quantified with chemistry-transport models. The CHIMERE chemistry-transport model is dedicated to regional atmospheric pollution event studies. Since it has now reached a certain level a maturity, the new stable version, CHIMERE 2013, is described to provide a reference model paper. The successive developments of the model are reviewed on the basis of published investigations that are referenced in order to discuss the scientific choices and to provide an overview of the main results.

title: The ozone monitoring instrument
abstract: The Ozone Monitoring Instrument (OMI) flies on the National Aeronautics and Space Administration's Earth Observing System Aura satellite launched in July 2004. OMI is a ultraviolet/visible (UV/VIS) nadir solar backscatter spectrometer, which provides nearly global coverage in one day with a spatial resolution of 13 km/spl times/24 km. Trace gases measured include O/sub 3/, NO/sub 2/, SO/sub 2/, HCHO, BrO, and OClO. In addition, OMI will measure aerosol characteristics, cloud top heights, and UV irradiance at the surface. OMI's unique capabilities for measuring important trace gases with a small footprint and daily global coverage will be a major contribution to our understanding of stratospheric and tropospheric chemistry and climate change. OMI's high spatial resolution is unprecedented and will enable detection of air pollution on urban scale resolution. In this paper, the instrument and its performance will be discussed.

title: SCIAMACHY: Mission Objectives and Measurement Modes
abstract: (Scanning Imaging Absorption Spectrometer for Atmospheric Chartography) is a spectrometer designed to measure sunlight transmitted, reflected, and scattered by the earth’s atmosphere or surface in the ultraviolet, visible, and near-infrared wavelength region (240–2380 nm) at moderate spectral resolution (0.2–1.5 nm, λ/Δλ ≈ 1000–10 000). SCIAMACHY will measure the earthshine radiance in limb and nadir viewing geometries and solar or lunar light transmitted through the atmosphere observed in occultation. The extraterrestrial solar irradiance and lunar radiance will be determined from observations of the sun and the moon above the atmosphere. The absorption, reflection, and scattering behavior of the atmosphere and the earth’s surface is determined from comparison of earthshine radiance and solar irradiance. Inversion of the ratio of earthshine radiance and solar irradiance yields information about the amounts and distribution of important atmospheric constituents and the spectral reflecta...

title: CHASER: A global chemical model of the troposphere 1. Model description
abstract: We present a new global three-dimensional chemical model for the troposphere, named chemical atmospheric general circulation model (AGCM) for study of atmospheric environment and radiative forcing (CHASER). This model, developed in the framework of the Center for Climate System Research/National Institute for Environment Studies (CCSR/NIES) AGCM, is aimed to study tropospheric photochemistry and its influences on climate. The chemical component of the model simulates the O3-HOx-NOx-CH4-CO photochemical system and oxidation of nonmethane hydrocarbons through 88 chemical and 25 photolytic reactions with 47 chemical species in its present configuration. The model includes emission sources, dry and wet deposition, as well as chemical transformations. Meteorological processes such as transport due to advection, convection, and other subgrid-scale mixing are simulated “on-line” by the dynamical component of the CCSR/NIES AGCM. A detailed evaluation of the model results is presented in a companion paper [Sudo et al., 2002]. An evaluation of the transport scheme adopted in the model suggests that the model is capable of simulating transport associated with convection and boundary layer mixing as well as large-scale advection. The model capability to simulate dry and wet deposition was also evaluated by conducting a simulation of atmospheric lead. The simulated lead distributions are consistent with those observed at the surface, showing the validity of the deposition parameterization adopted in the model.

title: MIROC-ESM 2010: model description and basic results of CMIP5-20c3m experiments
abstract: An earth system model (MIROC-ESM 2010) is fully described in terms of each model component and their interactions. Results for the CMIP5 (Coupled Model Intercomparison Project phase 5) historical simulation are presented to demonstrate the model's performance from several perspectives: atmosphere, ocean, sea-ice, land-surface, ocean and terrestrial biogeochemistry, and atmospheric chemistry and aerosols. An atmospheric chemistry coupled version of MIROC-ESM (MIROC-ESM-CHEM 2010) reasonably reproduces transient variations in surface air temperatures for the period 1850–2005, as well as the present-day climatology for the zonal-mean zonal winds and temperatures from the surface to the mesosphere. The historical evolution and global distribution of column ozone and the amount of tropospheric aerosols are reasonably simulated in the model based on the Representative Concentration Pathways' (RCP) historical emissions of these precursors. The simulated distributions of the terrestrial and marine biogeochemistry parameters agree with recent observations, which is encouraging to use the model for future global change projections.

title: Validation of urban NO 2 concentrations and their diurnal and seasonal variations observed from the SCIAMACHY and OMI sensors using in situ surface measurements in Israeli cities
abstract: We compare a full-year (2006) record of surface air NO2 concentrations measured in Israeli cities to coin- ciding retrievals of tropospheric NO2 columns from satellite sensors (SCIAMACHY aboard ENVISAT and OMI aboard Aura). This provides a large statistical data set for valida- tion of NO2 satellite measurements in urban air, where vali- dation is difficult yet crucial for using these measurements to infer NOx emissions by inverse modeling. Assuming that NO2 is well-mixed throughout the boundary layer (BL), and using observed average seasonal boundary layer heights, near-surface NO2 concentrations are converted into BL NO2 columns. The agreement between OMI and (13:45) BL NO2 columns (slope=0.93, n=542), and the comparable results at 10:00 h for SCIAMACHY, allow a validation of the seasonal, weekly, and diurnal cycles in satellite-derived NO2. OMI and BL NO2 columns show consistent seasonal cycles (win- ter NO2 1.6-2.7◊ higher than summer). BL and coinciding OMI columns both show a strong weekly cycle with 45-50% smaller NO2 columns on Saturday relative to the weekday mean, reflecting the reduced weekend activity, and validating the weekly cycle observed from space. The diurnal differ- ence between SCIAMACHY (10:00) and OMI (13:45) NO 2 is maximum in summer when SCIAMACHY is up to 40% higher than OMI, and minimum in winter when OMI slightly exceeds SCIAMACHY. A similar seasonal variation in the diurnal difference is found in the source region of Cairo. The surface measurements in Israel cities confirm this sea- sonal variation in the diurnal cycle. Using simulations from a global 3-D chemical transport model (GEOS-Chem), we show that this seasonal cycle can be explained by a much stronger photochemical loss of NO2 in summer than in win- ter.

title: Recent reduction in NO x emissions over China: synthesis of satellite observations and emission inventories
abstract: Tropospheric nitrogen dioxide (NO2) column densities detected from space are widely used to infer trends in terrestrial nitrogen oxide (NO x ) emissions. We study changes in NO2 column densities using the Ozone Monitoring Instrument (OMI) over China from 2005 to 2015 and compare them with the bottom-up inventory to examine NO x emission trends and their driving forces. From OMI measurements we detect the peak of NO2 column densities at a national level in the year 2011, with average NO2 column densities deceasing by 32% from 2011 to 2015 and corresponding to a simultaneous decline of 21% in bottom-up emission estimates. A significant variation in the peak year of NO2 column densities over regions is observed. Because of the reasonable agreement between the peak year of NO2 columns and the start of deployment of denitration devices, we conclude that power plants are the primary contributor to the NO2 decline, which is further supported by the emission reduction of 56% from the power sector in the bottom-up emission inventory associated with the penetration of selective catalytic reduction (SCR) increasing from 18% to 86% during 2011–2015. Meanwhile, regulations for vehicles also make a significant contribution to NO x emission reductions, in particular for a few urbanized regions (e.g., Beijing and Shanghai), where they implemented strict regulations for vehicle emissions years before the national schedule for SCR installations and thus reached their NO2 peak 2–3 years ahead of the deployment of denitration devices for power plants.

title: Assimilated inversion of NOx emissions over east Asia using OMI NO2 column measurements
abstract: Assimilated inversion on a daily basis using OMI tropospheric NO2 columns is developed and applied in a regional chemical transport model (REAM) to constrain fossil fuel (FF) NOx emissions over east Asia in 2007. The iterative nature of the assimilated inversion improves upon the widely used monthly-mean inversion by accounting for the chemical feedbacks of changed NOx emissions and reducing the dependence of the a priori emissions. The assimilated a posteriori emissions from FF combustion over east Asia are 9.5 Tg N/yr comparable to 10.9 Tg N/yr of the a priori. Significant changes in the spatial distribution of FF NOx emissions are found in the assimilated inversion from the a priori or monthly-mean inversion. The assimilated inversion shows that the a priori FF NOx emission inventory tends to overestimate the emissions over the economically developed areas and underestimate over the underdeveloped areas in East China, which may reflect in part FF NOx emission reductions resulting from the urban-centric air quality controls in China.

title: Multi-satellite sensor study on precipitation-induced emission pulses of NO x from soils in semi-arid ecosystems
abstract: We present a top-down approach to infer and quantify rain-induced emission pulses of NOx ( ≡  NO + NO2), stemming from biotic emissions of NO from soils, from satellite-borne measurements of NO2. This is achieved by synchronizing time series at single grid pixels according to the first day of rain after a dry spell of prescribed duration. The full track of the temporal evolution several weeks before and after a rain pulse is retained with daily resolution. These are needed for a sophisticated background correction, which accounts for seasonal variations in the time series and allows for improved quantification of rain-induced soil emissions. The method is applied globally and provides constraints on pulsed soil emissions of NOx in regions where the NOx budget is seasonally dominated by soil emissions. We find strong peaks of enhanced NO2 vertical column densities (VCDs) induced by the first intense precipitation after prolonged droughts in many semi-arid regions of the world, in particular in the Sahel. Detailed investigations show that the rain-induced NO2 pulse detected by the OMI (Ozone Monitoring Instrument), GOME-2 and SCIAMACHY satellite instruments could not be explained by other sources, such as biomass burning or lightning, or by retrieval artefacts (e.g. due to clouds). For the Sahel region, absolute enhancements of the NO2 VCDs on the first day of rain based on OMI measurements 2007–2010 are on average 4 × 1014  molec cm−2 and exceed 1 × 1015  molec cm−2 for individual grid cells. Assuming a NOx lifetime of 4 h, this corresponds to soil NOx emissions in the range of 6 up to 65 ng N m−2 s−1, which is in good agreement with literature values. Apart from the clear first-day peak, NO2 VCDs are moderately enhanced (2 × 1014  molec cm−2) compared to the background over the following 2 weeks, suggesting potential further emissions during that period of about 3.3 ng N m−2 s−1. The pulsed emissions contribute about 21–44 % to total soil NOx emissions over the Sahel.

title: Intercomparison of SCIAMACHY and OMI Tropospheric NO2 Columns: Observing the Diurnal Evolution of Chemistry and Emissions from Space
abstract: Concurrent (August 2006) measurements of tropospheric NO2 columns from OMI aboard Aura (1330 local overpass time) and SCIAMACHY aboard Envisat (1000 local overpass time) offer an opportunity to examine the consistency between the two instruments under tropospheric background conditions and the effect of different observing times. For scenes with tropospheric NO2 columns <5.0 × 1015 molecules cm−2, SCIAMACHY and OMI agree within 1.0–2.0 × 1015 molecules cm−2, consistent with the detection limits of both instruments. We find evidence for a low bias of 0.2 × 1015 molecules cm−2 in OMI observations over remote oceans. Over the fossil fuel source regions at northern midlatitudes, we find that SCIAMACHY observes up to 40% higher NO2 at 1000 local time (LT) than OMI at 1330 LT. Over biomass burning regions in the tropics, SCIAMACHY observes up to 40% lower NO2 columns than OMI. These differences are present in the spectral fitting of the data (slant column) and are augmented in the fossil fuel regions and dampened in the tropical biomass burning regions by the expected increase in air mass factor as the mixing depth rises from 1000 to 1330 LT. Using a global 3-D chemical transport model (GEOS-Chem), we show that the 1000–1330 LT decrease in tropospheric NO2 column over fossil fuel source regions can be explained by photochemical loss, dampened by the diurnal cycle of anthropogenic emissions that has a broad daytime maximum. The observed 1000–1330 LT NO2 column increase over tropical biomass burning regions points to a sharp midday peak in emissions and is consistent with a diurnal cycle of emissions derived from geostationary satellite fire counts.

title: Key chemical NOx sink uncertainties and how they influence top-down emissions of nitrogen oxides
abstract: Triggered by recent developments from laboratory and field studies regarding major NO x 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 NO x 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 HO 2, 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 NO x sink globally accounting for ca. 60 % of the total sink, the reactions contributing the most to the overall uncertainty are the formation of HNO 3 in NO+HO2, leading to NOx column changes exceeding a factor of two over tropical regions, and the uptake of HO 2 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 Sou h Asia where the combined uncertainty primarily associated to the NO+HO 2 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.  Impact of NOx sink uncertainties on top-down NOx

title: Structural uncertainty in air mass factor calculation for NO2 and HCHO satellite retrievals
abstract: Air mass factor (AMF) calculation is the largest source of uncertainty in NO2 and HCHO satellite retrievals in situations with enhanced trace gas concentrations in the lower troposphere. Structural uncertainty arises when different retrieval methodologies are applied within the scientific community to the same satellite observations. Here, we address the issue of AMF structural uncertainty via a detailed comparison of AMF calculation methods that are structurally different between seven retrieval groups for measurements from the Ozone Monitoring Instrument (OMI). We estimate the escalation of structural uncertainty in every sub-step of the AMF calculation process. This goes beyond the algorithm uncertainty estimates provided in state-of-the-art retrievals, which address the theoretical propagation of uncertainties for one particular retrieval algorithm only. We find that top-of-atmosphere reflectances simulated by four radiative transfer models (RTMs) (DAK, McArtim, SCIATRAN and VLIDORT) agree within 1.5 %. We find that different retrieval groups agree well in the calculations of altitude resolved AMFs from different RTMs (to within 3 %), and in the tropospheric AMFs (to within 6 %) as long as identical ancillary data (surface albedo, terrain height, cloud parameters and trace gas profile) and cloud and aerosol correction procedures are being used. Structural uncertainty increases sharply when retrieval groups use their preference for ancillary data, cloud and aerosol correction. On average, we estimate the AMF structural uncertainty to be 42 % over polluted regions and 31 % over unpolluted regions, mostly driven by substantial differences in the a priori trace gas profiles, surface albedo and cloud parameters. Sensitivity studies for one particular algorithm indicate that different cloud correction approaches result in substantial AMF differences in polluted conditions (5 to 40 % depending on cloud fraction and cloud pressure, and 11 % on average) even for low cloud fractions (<0.2) and the choice of aerosol correction introduces an average uncertainty of 50 % for situations with high pollution and high aerosol loading. Our work shows that structural uncertainty in AMF calculations is significant and that it is mainly caused by the assumptions and choices made to represent the state of the atmosphere. In order to decide which approach and which ancillary data are best for AMF calculations, we call for well-designed validation exercises focusing on polluted conditions in which AMF structural uncertainty has the highest impact on NO2 and HCHO retrievals.

title: Satellite constraint for emissions of nitrogen oxides from anthropogenic , lightning and soil sources over East China on a high-resolution grid
abstract: Vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) retrieved from space provide valuable information to estimate emissions of nitrogen oxides (NOx) inversely. Accurate emission attribution to individual sources, important both for understanding the global biogeochemical cycling of nitrogen and for emission control, remains difficult. This study presents a regression-based multi-step inversion approach to estimate emissions of NO x from anthropogenic, lightning and soil sources individually for 2006 over East China on a 0.25 ◦ long× 0.25 lat grid, employing the DOMINO product version 2 retrieved from the Ozone Monitoring Instrument. The inversion is done gridbox by gridbox to derive the respective emissions, taking advantage of differences in seasonality between anthropogenic and natural sources. Lightning and soil emissions are combined together for any given gridbox due to their similar seasonality; and their different spatial distributions are used implicitly for source separation to some extent. The nested GEOS-Chem model for East Asia is used to simulate the seasonal variations of different emission sources and impacts on VCDs of NO2 for the inversion purpose. Sensitivity tests are conducted to evaluate key assumptions embedded in the inversion process. The inverse estimate suggests annual budgets of about 7.1 TgN ( ±39 %), 0.21 TgN ( ±61 %), and 0.38 TgN (±65 %) for the a posteriori anthropogenic, lightning and soil emissions, respectively, about 18–23 % higher than the respective a priori values. The enhancements in anthropogenic emissions are largest in cities and areas with extensive use of coal, particularly in the north in winter, as evident on the high-resolution grid. Derived soil emissions are consistent with recent bottom-up estimates. They are less than 6 % of anthropogenic emissions annually, increasing to about 13 % for July. Derived lightning emissions are about 3 % of anthropogenic emissions annually and about 10 % in July. Overall, anthropogenic emissions are found to be the dominant source of NO x over East China with important implications for nitrogen control.