Interannual variation of reactive nitrogen emissions and their impacts on PM2.5 air pollution in China during 2005–2015

Emissions of reactive nitrogen as ammonia (NH3) and nitrogen oxides (NOx), together with sulfur dioxide (SO2), contribute to formation of secondary PM2.5 in the atmosphere. Satellite observations of atmospheric NH3, NO2, and SO2 levels since the 2000s provide valuable information to constrain the spatial and temporal variability of their emissions. Here we present a bottom-up Chinese NH3 emission inventory combined with top-down estimates of Chinese NOx and SO2 emissions using ozone monitoring instrument satellite observations, aiming to quantify the interannual variations of reactive nitrogen emissions in China and their contributions to PM2.5 air pollution over 2005–2015. We find small interannual changes in the total Chinese anthropogenic NH3 emissions during 2005–2016 (12.0–13.3 Tg with over 85% from agricultural sources), but large interannual change in top-down Chinese NOx and SO2 emissions. Chinese NOx emissions peaked around 2011 and declined by 22% during 2011–2015, and Chinese SO2 emissions declined by 55% in 2015 relative to that in 2007. Using the GEOS-Chem chemical transport model simulations, we find that rising atmospheric NH3 levels in eastern China since 2011 as observed by infrared atmospheric sounding interferometer and atmospheric infrared sounder satellites are mainly driven by rapid reductions in SO2 emissions. The 2011–2015 Chinese NOx emission reductions have decreased regional annual mean PM2.5 by 2.3–3.8 μg m−3. Interannual PM2.5 changes due to NH3 emission changes are relatively small, but further control of agricultural NH3 emissions can be effective for PM2.5 pollution mitigation in eastern China

Decadal Variabilities in Tropospheric Nitrogen Oxides Over United States, Europe, and China

Global trends in tropospheric nitrogen dioxide (NO2) have changed dramatically in the past decade. Here, we investigate tropospheric NO2 variabilities over United States, Europe, and E. China in 2005–2018 to explore the mechanisms governing the variation of this critical pollutant. We found large uncertainties in the trends of anthropogenic nitrogen oxides (NOx) emissions, for example, the reductions of NOx emissions, derived with different approaches and data sets, are in the range of 35%–50% over the United States and 15%–45% over Europe in 2005–2018. By contrast, the analysis in this work indicates declines of anthropogenic NOx emissions by about 40% and 25% over the United States and Europe, respectively, in 2005–2018, and about 20% over E. China in 2012–2018. However, the shift of major NOx sources from power generation to industrial and transportation sectors has led to noticeable diminishing effects in emission controls. Furthermore, satellite measurements exhibit the influence of NO2 background levels over the United States and Europe, which offset the impacts of anthropogenic emission declines, resulting in flatter trends of tropospheric NO2 over the United States and Europe. Our analysis further reveals underestimation of background NO2 by chemical transport models, which can lead to inaccurate interpretations of satellite measurements. We use surface in-situ NO2 observations to diagnose the satellite-observed NO2 trends and find top-down NOx emissions over urban grids represent the changes in anthropogenic NOx emissions better. This work highlights the importance of comprehensive applications of different analysis approaches to better characterizing atmospheric composition evolution

Development of the adjoint of GEOS-Chem

We present the adjoint of the global chemical transport model GEOS-Chem, focusing on the chemical and thermodynamic relationships between sulfate - ammonium - nitrate aerosols and their gas-phase precursors. The adjoint model is constructed from a combination of manually and automatically derived discrete adjoint algorithms and numerical solutions to continuous adjoint equations. Explicit inclusion of the processes that govern secondary formation of inorganic aerosol is shown to afford efficient calculation of model sensitivities such as the dependence of sulfate and nitrate aerosol concentrations on emissions of SOX, NOX, and NHs. The accuracy of the adjoint model is extensively verified by comparing adjoint to finite difference sensitivities, which are shown to agree within acceptable tolerances. We explore the robustness of these results, noting how discontinuities in the advection routine hinder, but do not entirely preclude, the use of such comparisons for validation of the adjoint model. The potential for inverse modeling using the adjoint of GEOS-Chem is assessed in a data assimilation framework using simulated observations, demonstrating the feasibility of exploiting gas- and aerosol-phase measurements for optimizing emission inventories of aerosol precursors

ANISORROPIA: The adjoint of the aerosol thermodynamic model ISORROPIA

We present the development of ANISORROPIA, the discrete adjoint of the ISORROPIA thermodynamic equilibrium model that treats the Na +-SO 4 2- HSO 4 -NH 4 +-NO 3 -Cl -H 2O aerosol system, and we demonstrate its sensitivity analysis capabilities. ANISORROPIA calculates sensitivities of an inorganic species in aerosol or gas phase with respect to the total concentrations of each species present with less than a two-fold increase in computational time over the concentration calculations. Due to the highly nonlinear and discontinuous solution surface of ISORROPIA, evaluation of the adjoint required a new, complex-variable version of the model, which determines first-order sensitivities with machine precision and avoids cancellation errors arising from finite difference calculations. The adjoint is verified over an atmospherically relevant range of concentrations, temperature, and relative humidity. We apply ANISORROPIA to recent field campaign results from Atlanta, GA, USA, and Mexico City, Mexico, to characterize the inorganic aerosol sensitivities of these distinct urban air masses. The variability in the relationship between fine mode inorganic aerosol mass and precursor concentrations shown has important implicat

Constraining aerosol health impacts with sensitivity analysis using the CMAQ adjoint

The role of emissions from different sectors and locations on premature mortalities attributed to exposure to black carbon (BC) was studied using CMAQ adjoint model. While a majority of mortalities occur in highly-populated, urban locations, transport from less-populated r

TES ammonia retrieval strategy and global observations of the spatial and seasonal variability of ammonia

Presently only limited sets of tropospheric ammonia (NH3) measurements in the Earth's atmosphere have been reported from satellite and surface station measurements, despite the well-documented negative impact of NH3 on the environment and human health. Presented here is a detailed description of the satellite retrieval strategy and analysis for the Tropospheric Emission Spectrometer (TES) using simulations and measurements. These results show that: (i) the level of detectability for a representative boundary layer TES NH3 mixing ratio value is ∼0.4 ppbv, which typically corresponds to a profile that contains a maximum level value of ∼1 ppbv; (ii) TES NH3 retrievals generally provide at most one degree of freedom for signal (DOFS), with peak sensitivity between 700 and 900 mbar; (iii) TES NH3 retrievals show significant spatial and seasonal variability of NH3 globally; (iv) initial comparisons of TES observations with GEOS-CHEM estimates show TES values being higher overall. Important differences and similarities between modeled and observed seasonal and spatial trends are noted, with discrepancies indicating areas where the timing and magnitude of modeled NH3 emissions from agricultural sources, and to lesser extent biomass burning sources, need further study. © Author(s) 2011. CC Attribution 3.0 License.SCOPUS: ar.jinfo:eu-repo/semantics/publishe

Adjoint inverse modeling of black carbon during the Asian Pacific Regional Aerosol Characterization Experiment

An adjoint model is used for inverse modeling of black carbon during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia). We use the four-dimensional variational data assimilation (4D-Var) approach to optimally recover spatially resolved anthropogenic and bio

The influence of boreal biomass burning emissions on the distribution of tropospheric ozone over North America and the North Atlantic during 2010

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