The 50 most-cited articles in Atmospheric chemistry and physics, 2021

Abstract. Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, the relative contributions of the world’s major dust source regions to the global dust cycle remain poorly constrained. This problem hinders accounting for the potentially large impact of regional differences in dust properties on clouds, the Earth's energy balance, and terrestrial and marine biogeochemical cycles. Here, we constrain the contribution of each of the world’s main dust source regions to the global dust cycle. We use an analytical framework that integrates an ensemble of global model simulations with observationally informed constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth. We obtain a data set that constrains the relative contribution of each of nine major source regions to size-resolved dust emission, atmospheric loading, optical depth, concentration, and deposition flux. We find that the 22–29 Tg (one standard error range) global loading of dust with geometric diameter up to 20 μm is partitioned as follows: North…

Abstract. Southern Africa produces almost a third of the Earth’s biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a five-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three Intensive Observation Periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June-October), aerosol particles reaching 3–5 km in altitude are transported westward over the South-East Atlantic, where they interact with one of the largest subtropical stratocumulus subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, and due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017…

Abstract. Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the present day modelling of aerosol optical properties has been assessed using simulated data representative for the year 2010, from 14 global aerosol models participating in the Phase III Control experiment. The model versions are close or equal to those used for CMIP6 and AerChemMIP and inform also on bias in state of the art ESMs. Modelled column optical depths (total, fine and coarse mode AOD) and Angstrom Exponents (AE) were compared both with ground based observations from the Aerosol Robotic Network (AERONET, version 3) as well as space based observations from AATSR-SU instruments. In addition, the modelled AODs were compared with MODIS (Aqua and Terra) data and a satellite AOD data-set (MERGED-FMI) merged from 12 different individual AOD products. Furthermore, for the first time, the modelled near surface scattering (under dry conditions) and absorption coefficients were evaluated against measurements made at low relative humidity at surface in-situ GAW sites.…

Abstract. The evolution of tropospheric ozone from 1850 to 2100 has been studied using data from Phase 6 of the Coupled Model Intercomparison Project (CMIP6). We evaluate long-term changes using coupled atmosphere-ocean chemistry-climate models, focusing on the CMIP historical and ScenarioMIP ssp370 experiments, for which detailed tropospheric ozone diagnostics were archived. The model ensemble has been evaluated against a suite of surface, sonde, and satellite observations of the past several decades, and found to reproduce well the salient spatial, seasonal and decadal variability and trends. The tropospheric ozone burden increases from 244 ± 30 Tg in 1850 to a mean value of 348 ± 15 Tg for the period 2005–2014, an increase of 40 %. Modelled present day values agree well with previous determinations (ACCENT: 336 ± 27 Tg; ACCMIP: 337 ± 23 Tg and TOAR: 340 ± 34 Tg). In the ssp370 experiments, the ozone burden reaches a maximum of 402 ± 36 Tg in 2090, before declining slightly to 396 ± 32 Tg by 2100. The ozone budget has been examined over the same period using lumped ozone…

Abstract. The Emissions Database for Global Atmospheric Research (EDGAR) estimates the human-induced emission rates on Earth collaborating with atmospheric modelling activities as well as aiding policy in the design of mitigation strategies and in evaluating their effectiveness. In these applications, the uncertainty estimate is an essential component as it quantifies the accuracy and qualifies the level of confidence in the emission. This study complements the EDGAR's emissions inventory with estimation of the structural uncertainty stemming from its base components (activity data statistics (AD) and emission factors (EF)) by i) associating uncertainty to each AD and EF characterizing the emissions of the three main greenhouse gases (GHG) CO2, CH4 and N2O; ii) combining them, and iii) making assumptions for the cross-country uncertainty aggregation of source categories. It was deemed a natural choice to obtain the uncertainties in EFs and AD from the Intergovernmental Panel on Climate Change (IPCC) guidelines issued in 2006 (with a few exceptions), since the EF and AD sources and…

Abstract. The contribution of meteorology and emissions to long-term PM2.5 trends is critical for air quality management but has not yet been fully analyzed. Here, we used a combination of machine learning model, statistical model and chemical transport model to quantify the meteorological impacts on PM2.5 pollution during 2000–2018. Specifically, we first developed a two-stage machine learning PM2.5 prediction model with a synthetic minority oversampling technique to improve the satellite-based PM2.5 estimates over highly polluted days, thus allowing us to better characterize the meteorological effects on haze events. Then we used two methods, a generalized additive model (GAM) driven by the satellite-based full-coverage daily PM2.5 retrievals as well as the Weather Research and Forecasting/Community Multiscale Air Quality (WRF/CMAQ) modelling system, to examine the meteorological contribution to PM2.5. We found good agreements between the GAM model estimations and the CMAQ model estimations of meteorological contribution to PM2.5 on monthly scale (correlation coefficient between…

Abstract. Shallow clouds covering vast areas of the world's mid- and high-latitude oceans play a key role in dampening the global temperature rise associated with CO2. These clouds, which contain both ice and supercooled water, respond to a warming world by transitioning to a state with more liquid water and a greater albedo, resulting in a negative cloud-phase climate feedback component. Here we argue that the magnitude of the negative cloud-phase feedback component depends on the amount and nature of the small fraction of aerosol particles that can nucleate ice crystals. We propose that a concerted research effort is required to reduce substantial and important uncertainties related to the poorly understood sources, concentration, seasonal cycles and nature of these ice-nucleating particles (INPs) and their rudimentary treatment in climate models. The topic is important because many climate models may have overestimated the magnitude of the cloud-phase feedback, and those with better representation of shallow oceanic clouds predict a substantially larger climate warming. We make…

Abstract. Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, atmospheric models struggle to accurately represent its spatial and temporal distribution. These model errors are partially caused by fundamental difficulties in simulating dust emission in coarse-resolution models and in accurately representing dust microphysical properties. Here we mitigate these problems by developing a new methodology that yields an improved representation of the global dust cycle. We present an analytical framework that uses inverse modeling to integrate an ensemble of global model simulations with observational constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth. We then compare the inverse model results against independent measurements of dust surface concentration and deposition flux and find that errors are reduced by approximately a factor of two relative to current model simulations of the Northern Hemisphere dust cycle. The inverse model results show smaller improvements in the less dusty Southern Hemisphere,…

Abstract. The planetary boundary layer height (BLH) governs the vertical transport of mass, momentum and moisture between the surface and the free atmosphere, and thus its characterization is recognized as crucial for air quality, weather and climate. Although reanalysis products can provide important insight into the global view of BLH in a seamless way, the in situ observed BLH on a global scale remains poorly understood due to the lack of high-resolution (1-s or 2-s) radiosonde measurements. The present study attempts to establish a near-global BLH climatology at synoptic times (0000 and 1200 UTC) and in the daytime using high-resolution radiosonde measurements over 300 radiosonde sites worldwide for the period 2012 to 2019, which is then compared against the BLHs obtained from four reanalysis datasets, including ERA-5, MERRA-2, JRA-55, and NCEP-2. The variations of BLH exhibit large spatial and temporal dependence, and as a result the BLH maxima are generally discerned over the regions such as Western United States and Western China, in which the balloon launch times mostly…

Abstract. Ground-level ozone (O3) pollution has been steadily getting worse in most part of eastern China during the past five years. The non-linearity of O3 formation with its precursors like nitrogen oxides (NOx = NO + NO2) and volatile organic compounds (VOCs) are complicating effective O3 abatement plans. The diagnosis from space-based observations, the ratio of formaldehyde (HCHO) columns to tropospheric NO2 columns (HCHO / NO2), has previously been proved to be highly consistent with our current understanding of surface O3 chemistry. HCHO / NO2 ratio thresholds distinguishing O3 formation sensitivity depend on regions and O3 chemistry interactions with aerosol. To shed more light on current the O3 formation sensitivity over China, we have derived HCHO / NO2 ratio thresholds by directly connecting satellite-based HCHO / NO2 observations and ground-based O3 measurements over the major Chinese cities in this study. We find that a VOC-limited regime occurs for HCHO / NO2 4.2. The HCHO / NO2 between 2.3 and 4.2 reflects the transition between the two regimes. Our method shows that…

Abstract. We evaluate the global atmospheric methane column retrievals from the new TROPOMI satellite instrument and apply them to a global inversion of methane sources for 2019 at 2° × 2.5° horizontal resolution. We compare the results to an inversion using the sparser but more mature GOSAT satellite retrievals, as well as a joint inversion using both TROPOMI and GOSAT. Validation of TROPOMI and GOSAT with TCCON ground-based measurements of methane columns, after correcting for retrieval differences in prior vertical profiles and averaging kernels using the GEOS-Chem chemical transport model, shows global biases of −2.7 ppbv for TROPOMI and −1.0 ppbv for GOSAT, and regional biases of 6.7 ppbv for TROPOMI and 2.9 ppbv for GOSAT. Intercomparison of TROPOMI and GOSAT shows larger regional discrepancies exceeding 20 ppbv, mostly over regions with low surface albedo in the shortwave infrared where the TROPOMI retrieval may be biased. Our inversion uses an analytical solution to the Bayesian optimization of methane sources, thus providing an explicit characterization of error statistics…

Abstract. We present an updated mechanism for tropospheric halogen (Cl + Br + I) chemistry in the GEOS-Chem global atmospheric chemical transport model and apply it to investigate halogen radical cycling and implications for tropospheric oxidants. Improved representation of HOBr heterogeneous chemistry and its pH dependence in our simulation leads to less effective recycling and mobilization of bromine radicals, and enables the model to include mechanistic sea salt aerosol debromination without generating excessive BrO. The resulting global mean tropospheric BrO mixing ratio is 0.19 ppt, lower than previous versions of GEOS-Chem. Model BrO shows variable consistency and biases in comparison to surface and aircraft observations in marine air, which are often near or below the detection limit. The model underestimates the daytime measurements of Cl2 and BrCl from the ATom aircraft campaign over the Pacific and Atlantic, which if correct would imply a very large missing primary source of chlorine radicals. Model IO is highest in the marine boundary layer and uniform in the free…

The acidity of aqueous atmospheric solutions is a key parameter driving both the partitioning of semi-volatile acidic and basic trace gases and their aqueous-phase chemistry. In addition, the acidity of atmospheric aqueous phases, e.g., deliquesced aerosol particles, cloud, and fog droplets, is also dictated by aqueous-phase chemistry. These feedbacks between acidity and chemistry have crucial implications for the tropospheric lifetime of air pollutants, atmospheric composition, deposition to terrestrial and oceanic ecosystems, visibility, climate, and human health. Atmospheric research has made substantial progress in understanding feedbacks between acidity and multiphase chemistry during recent decades. This paper reviews the current state of knowledge on these feedbacks with a focus on aerosol and cloud systems, which involve both inorganic and organic aqueous-phase chemistry. Here, we describe the impacts of acidity on the phase partitioning of acidic and basic gases and buffering phenomena. Next, we review feedbacks of different acidity regimes on key chemical reaction…

Abstract. PM2.5 has been used as an important atmospheric environmental parameter primarily due to its impact on human health. PM2.5 is affected by both natural and anthropogenic factors that usually have strong diurnal variations. Monitoring it does not only help understand the causes of air pollution but also our adaptation to it. Most existing PM2.5 products have been derived from polar-orbiting satellites. This study exploits the usage of the next-generation geostationary meteorological satellite Himawari-8/AHI in revealing its diurnal variations. Given the huge volume of the satellite data, a highly efficient tree-based Light Gradient Boosting Machine (LightGBM) learning approach, which is based on the idea of gradient boosting, is applied by involving the spatiotemporal characteristics of air pollution, named the space-time LightGBM (STLG) model. Hourly PM2.5 data set in China (i.e., ChinaHighPM2.5) at a 5 km spatial resolution is derived based on the Himawari-8/AHI aerosol products together with other variables. The hourly PM2.5 estimates (N = 1,415,188) are well correlated…

Abstract. In March 2020, non-pharmaceutical interventions in the form of lockdowns were applied across Europe to urgently reduce the transmission of SARS-CoV-2, the virus which causes the COVID-19 disease. The near-complete shutdown of the European economy had widespread impacts on atmospheric composition, particularly for nitrogen dioxide (NO2) and ozone (O3). To investigate these changes, we analyze data from 246 ambient air pollution monitoring sites in 102 urban areas and 34 countries in Europe between February and July, 2020. Counterfactual, business as usual air quality time series are created using machine learning models to account for natural weather variability. Across Europe, we estimate that NO2 concentrations were 34 and 32 % lower than expected for traffic and urban-background locations while O3 was 30 and 21 % higher (in the same environments) at the point of maximum restriction on mobility. The European urban NO2 experienced in the 2020 lockdown was equivalent to that which might be anticipated in 2028 based on average trends since 2010. Despite NO2 concentrations…

Abstract. Measurements of OH, HO2, complex RO2 (alkene- and aromatic-related RO2) and total RO2 radicals taken during the integrated Study of AIR Pollution PROcesses in Beijing (AIRPRO) campaign in central Beijing in the summer of 2017, alongside observations of OH reactivity, are presented. The concentrations of radicals were elevated, with OH reaching up to 2.8×107moleculecm-3, HO2 peaking at 1×109moleculecm-3 and the total RO2 concentration reaching 5.5×109moleculecm-3. OH reactivity (k(OH)) peaked at 89 s−1 during the night, with a minimum during the afternoon of ≈22s-1 on average. An experimental budget analysis, in which the rates of production and destruction of the radicals are compared, highlighted that although the sources and sinks of OH were balanced under high NO concentrations, the OH sinks exceeded the known sources (by 15 ppbv h−1) under the very low NO conditions (<0.5 ppbv) experienced in the afternoons, demonstrating a missing OH source consistent with previous studies under high volatile organic compound (VOC) emissions and low NO loadings. Under the highest NO…

Abstract. New particle formation (NPF) is one of the major sources of atmospheric ultrafine particles. Due to the high aerosol and trace gas concentrations, the mechanism and governing factors for NPF in the polluted atmospheric boundary layer may be quite different from those in clean environments, which is however less understood. Herein, based on long-term atmospheric measurements from January 2018 to March 2019 in Beijing, the nucleation mechanism and the influences of H2SO4 concentration, amine concentrations, and aerosol concentration on NPF are quantified. The collision of H2SO4-amine clusters is found to be the dominating mechanism to initialize NPF in urban Beijing. The coagulation scavenging due to the high aerosol concentration is a governing factor as it limits the concentration of H2SO4 amine clusters and new particle formation rates. Besides, the effective amine concentration is another limiting factor in Beijing because amine is sometimes insufficient for nucleation at the kinetic limit. Based on the synergistic effects of these factors on H2SO4-amine nucleation,…

Abstract. The TROPOspheric Monitoring Instrument (TROPOMI), launched in October 2017 on board the Sentinel-5 Precursor (S5P) satellite, monitors the composition of the Earth's atmosphere at an unprecedented horizontal resolution as fine as 3.5 × 5.5 km2. This paper assess the performances of the TROPOMI formaldehyde (HCHO) operational product compared to its predecessor, the OMI HCHO QA4ECV product, at different spatial and temporal scales. The parallel development of the two algorithms favored the consistency of the products, which facilitates the production of long-term combined time series. The main difference between the two satellite products is related to the use of different cloud algorithms, leading to a positive bias of OMI compared to TROPOMI of up to 30 % in Tropical regions. We show that after switching off the explicit correction for cloud effects, the two datasets come into an excellent agreement. For medium to large HCHO vertical columns (larger than 5 × 1015 molec.cm−2) the median bias between OMI and TROPOMI HCHO columns is not larger than 10 % (< 0.4 × 1015…

A high-resolution air pollutant emission inventory for the Yangtze River Delta (YRD) region was updated for 2017 using emission factors and chemical speciation based mainly on local measurements in this study. The inventory included 424 non-methane volatile organic compounds (NMVOCs) and 43 fine particulate matter (PM 2.5 ) species from 259 specific sources. The total emissions of SO 2 , NO x , CO, NMVOCs, PM 10 , PM 2.5 , and NH 3 in the YRD region in 2017 were 1552, 3235, 38 507, 4875, 3770, 1597, and 2467 Gg, respectively. SO 2 and CO emissions were mainly from boilers, accounting for 49 % and 73 % of the total. Mobile sources dominated NO x emissions, contributing 57 % of the total. NMVOC emissions, mainly from industrial sources, made up 61 % of the total. Dust sources accounted for 55 % and 28 % of PM 10 and PM 2.5 emissions, respectively. Agricultural sources accounted for 91 % of NH 3 emissions. Major PM 2.5 species were OC, Ca, Si, PSO 4 , and EC, accounting for 9.0 %, 7.0 %, 6.4 %, 4.6 %, and 4.3 % of total PM 2.5 emissions, respectively. The main species of NMVOCs were…

Abstract. In June 2019 a stratospheric moderate eruption occurred at Raikoke (48° N, 153° E). Satellite observations show the injection of ash and SO2 into the lower stratosphere and an early entrainment of the plume into a cyclone. Following the Raikoke eruption stratospheric Aerosol Optical Depth (sAOD) values increased in the whole northern hemisphere and tropics and remained enhanced for more than one year, with peak values at 0.040 (shorter-wavelength visible, higher northern latitudes) to 0.025 (shorter-wavelength visible, average northern hemisphere). Discrepancies between observations and models indicate that ash has played a role on evolution and sAOD values. Top of the atmosphere radiative forcings are estimated at values between −0.3 and −0.4 W/m2 (clear-sky), and of −0.1 to −0.2 W/m2 (all-sky), comparable to what was estimated for the Sarychev eruption in 2009. Almost simultaneously two significantly smaller stratospheric eruptions occurred at Ulawun (5° S, 151° E) in June and August. Aerosol enhancements from the Ulawun eruptions had mainly an impact on the tropics and…

Abstract. This paper quantifies the effective radiative forcing from CMIP6 models of the present-day anthropogenic emissions of NOx, CO, VOCs, SO2, NH3, black carbon and primary organic carbon. Effective radiative forcing from pre-industrial to present-day changes in the concentrations of methane, N2O and halocarbons are quantified and attributed to their anthropogenic emissions. Emissions of reactive species can cause multiple changes in the composition of radiatively active species: tropospheric ozone, stratospheric ozone, secondary inorganic and organic aerosol and methane. We therefore break down the ERFs from each emitted species into the contributions from the composition changes. The 1850 to 2014 mean ERFs are 1.1 ± 0.07 W m−2 for sulfate, −0.24 ± 0.01 W m−2 for organic carbon (OC), and 0.15 ± 0.04 W m−2 for black carbon (BC), and for the aerosols combined it is −0.95 ± 0.03 W m−2. The means for the reactive gases are 0.69 ± 0.04 W m−2 for methane (CH4), 0.06 ± 0.04 W m−2 for NOx, −0.09 ± 0.03 W m−2 for volatile organic carbons (VOC), 0.16 ± 0.03 W m−2 for ozone (O3), 0.27 W…

Abstract. Anthropogenic secondary organic aerosol (ASOA), formed from anthropogenic emissions of organic compounds, constitutes a substantial fraction of the mass of submicron aerosol in populated areas around the world and contributes to poor air quality and premature mortality. However, the precursor sources of ASOA are poorly understood, and there are large uncertainties in the health benefits that might accrue from reducing anthropogenic organic emissions. We show that the production of ASOA in 11 urban areas on three continents is strongly correlated with the anthropogenic reactivity of specific volatile organic compounds. The differences in ASOA production across different cities can be explained by differences in the emissions of aromatics and intermediate- and semi-volatile organic compounds, indicating the importance of controlling these ASOA precursors. With an improved modeling representation of ASOA driven by the observations, we attribute 340,000 PM2.5 premature deaths per year to ASOA, which is over an order of magnitude higher than prior studies. A sensitivity case…

Abstract. We conduct a global inverse analysis of 2010–2018 GOSAT satellite observations to better understand the factors controlling atmospheric methane and its accelerating increase over the 2010–2018 period. The inversion optimizes 2010–2018 anthropogenic methane emissions and their trends on a 4º × 5º grid, monthly regional wetland emissions, and annual hemispheric concentrations of tropospheric OH (the main sink of methane) also for individual years. We use an analytical solution to the Bayesian optimization problem that provides closed-form estimates of error covariances and information content for the solution. Our inversion successfully reduces the errors against the independent methane observations from the TCCON network and reproduces the interannual variability of the methane growth rate inferred from NOAA background sites. We find that prior estimates of fuel-related emissions reported by individual countries to the United Nations are too high for China (coal) and Russia (oil/gas), and too low for Venezuela (oil/gas) and the U.S. (oil/gas). We show that the 2010–2018…

Abstract. We use satellite (GOSAT) and in situ (GLOBALVIEWplus CH4 ObsPack) observations of atmospheric methane in a joint global inversion of methane sources, sinks, and trends for the 2010–2017 period. The inversion is done by analytical solution to the Bayesian optimization problem, yielding closed-form estimates of information content to assess the consistency and complementarity (or redundancy) of the satellite and in situ datasets. We find that GOSAT and in situ observations are to a large extent complementary, with GOSAT providing a stronger overall constraint on the global methane distributions, but in situ observations being more important for northern mid-latitudes and for relaxing global error correlations between methane emissions and the main methane sink (oxidation by OH radicals). The GOSAT observations achieve 212 independent pieces of information (DOFS) for quantifying mean 2010–2017 anthropogenic emissions on 1009 global model grid elements, and a DOFS of 122 for 2010–2017 emission trends. Adding the in situ data increases the DOFS by about 20–30 %, to 262 and 161…

Abstract. Stratospheric ozone and water vapour are key components of the Earth system, and past and future changes to both have important impacts on global and regional climate. Here we evaluate long-term changes in these species from the pre- industrial (1850) to the end of the 21st century in CMIP6 models under a range of future emissions scenarios. There is good agreement between the CMIP multi-model mean and observations, although there is substantial variation between the individual CMIP6 models. For the CMIP6 multi-model mean, global total column ozone (TCO) has increased from ∼300 DU in 1850 to ∼305 DU in 1960, before rapidly declining in the 1970s and 1980s following the use and emission of halogenated ozone depleting substances (ODSs). TCO is projected to return to 1960s values by the middle of the 21st century under the SSP2-4.5, SSP3-7.0, SSP4-3.4, SSP4-6.0 and SSP5-8.5 scenarios, and under the SSP3-7.0 and SSP5-8.5 scenarios TCO values are projected to be ∼10 DU higher than the 1960s values by 2100. However, under the SSP1-1.9 and SSP1-1.6 scenarios, TCO is not projected…

Abstract. The representation of clouds, aerosols and cloud-aerosol-radiation impacts remain some of the largest uncertainties in climate change, limiting our ability to accurately reconstruct and predict future climate. The south-east Atlantic is a region where high atmospheric aerosol loadings and semi-permanent stratocumulus clouds are co-located, providing a natural laboratory for studying the full range of aerosol-radiation and aerosol-cloud interactions and their perturbations of the Earth’s radiation budget. While satellite measurements have provided some useful insights into aerosol-radiation and aerosol cloud interactions over the region, these observations do not have the spatial and temporal resolution, nor the required level of precision to allow for a process level assessment. Detailed measurements from high spatial and temporal resolution airborne atmospheric measurements in the region are very sparse, limiting their use in assessing the performance of aerosol modelling in numerical weather prediction and climate models. CLARIFY-2017 was a major consortium programme…

Abstract. Air pollution, in particular high concentrations of particulate matter smaller than 1 µm in diameter (PM1), continues to be a major health problem, and meteorology is known to substantially contribute to atmospheric PM concentrations. However, the scientific understanding of the complex mechanisms leading to high pollution episodes is inconclusive, as the effects of meteorological variables are not easy to separate and quantify. In this study, a novel, data-driven approach based on empirical relationships is used to characterise the role of meteorology on atmospheric concentrations of PM1. A tree-based machine learning model is set up to reproduce concentrations of speciated PM1 at a suburban site southwest of Paris, France, using meteorological variables as input features. The contributions of each meteorological feature to modeled PM1 concentrations are quantified using SHapley Additive exPlanation (SHAP) regression values. Meteorological contributions to PM1 concentrations are analysed in selected high-resolution case studies, contrasting season-specific processes.…

Abstract. We quantify the reductions in primary emissions due to the COVID-19 lockdowns in Europe. Our estimates are provided in the form of a dataset of reduction factors varying per country and day that will allow modelling and identifying the associated impacts upon air quality. The country- and daily-resolved reduction factors are provided for each of the following source categories: energy industry (power plants), manufacturing industry, road traffic and aviation (landing and take-off cycle). We computed the reduction factors based on open access and near-real time measured activity data from a wide range of information sources. We also trained a machine learning model with meteorological data to derive weather-normalised electricity consumption reductions. The time period covered is from 21 February, when the first European localised lockdown was implemented in the region of Lombardy (Italy), until 26 April 2020. This period includes five weeks (23 March until 26 April) with the most severe and relatively unchanged restrictions upon mobility and socio-economic activities…

Abstract. Feedbacks play a fundamental role in determining the magnitude of the response of the climate system to external forcing, such as from anthropogenic emissions. The latest generation of Earth system models include aerosol and chemistry components that interact with each other and with the biosphere. These interactions introduce a complex web of feedbacks which it is important to understand and quantify. This paper addresses the multiple pathways for aerosol and chemical feedbacks in Earth system models. This is achieved by extending previous formalisms which include CO2 concentrations as a state variable to a formalism which in principle includes the concentrations of all climate-active atmospheric constituents. This framework is demonstrated by applying it to the Earth system models participating in CMIP6 with a focus on the non-CO2 reactive gases and aerosols (methane, ozone, sulphate aerosol, organic aerosol and dust). We find that the overall climate feedback through chemistry and aerosols is negative in the CMIP6 Earth system models due to increased negative forcing…

Abstract. The large uncertainty in mineral dust direct radiative effect (DRE) hinders projections of future climate change due to anthropogenic activity. Resolving modelled dust mineral-speciation allows for spatially and temporally varying refractive indices consistent with dust aerosol composition. Here, for the first time, we quantify the range in dust DRE at the top of the atmosphere (TOA) due to current uncertainties in the surface soil mineralogical content using a dust mineral-resolving climate model. We propagate observed uncertainties in soil mineral abundances from two soil mineralogy atlases along with the optical properties of each mineral into the DRE and compare the resultant range with other sources of uncertainty across six climate models. The shortwave DRE responses region-specifically to the dust burden depending on the mineral speciation and underlying shortwave surface albedo; positively when the regionally averaged annual surface albedo is larger than 0.28, and negatively otherwise. Among all minerals examined, the shortwave TOA DRE and single scattering albedo…

Abstract. We present here results from the Geoengineering Model Intercomparison Project (GeoMIP) simulations for the experiment G6sulfur and G6solar for six Earth System Models participating in the Climate Model Intercomparison Project (CMIP) Phase 6. The aim of the experiments is to reduce the warming from that resulting from a high-tier emission scenario (Shared Socioeconomic Pathways SSP5-8.5) to that resulting from a medium-tier emission scenario (SSP2-4.5). These simulations aim to analyze the response of climate models to a reduction in incoming surface radiation as a means to reduce global surface temperatures, and they do so either by simulating a stratospheric sulfate aerosol layer or, in a more idealized way, through a uniform reduction in the solar constant in the model. We find that, by the end of the century, there is a considerable inter-model spread in the needed injection of sulfate (29 ± 9 Tg-SO2/yr between 2081 and 2100), in how the aerosol cloud is distributed latitudinally, and in how stratospheric temperatures are influenced by the produced aerosol layer. Even…

Abstract. This study provides a comprehensive assessment of NO2 changes across the main European urban areas induced by the COVID-19 lockdown using satellite retrievals from the Tropospheric Monitoring Instrument (TROPOMI), surface site measurements and simulations from the Copernicus Atmospheric Monitoring Service (CAMS) regional ensemble of air quality models. Some recent TROPOMI-based estimates of NO2 changes have neglected the influence of weather variability between the reference and lockdown periods. Here we provide weather-normalized estimates based on a machine learning method (gradient boosting) along with an assessment of the biases that can be expected from methods that omit the influence of weather. We also compare the weather-normalized satellite NO2 column changes with both weather-normalized surface NO2 concentration changes and simulated changes by the CAMS regional ensemble, composed of 11 models, using recently published emission reductions induced by the lockdown. We show that all estimates show the same tendency on NO2 reductions. Locations where the lockdown was…

Abstract. Social-distancing to combat the COVID-19 pandemic has led to widespread reductions in air pollutant emissions. Quantifying these changes requires a business as usual counterfactual that accounts for the synoptic and seasonal variability of air pollutants. We use a machine learning algorithm driven by information from the NASA GEOS-CF model to assess changes in nitrogen dioxide (NO2) and ozone (O3) at 5756 observation sites in 46 countries from January through June 2020. Reductions in NO2 correlate with timing and intensity of COVID-19 restrictions, ranging from 60 % in severely affected cities (e.g., Wuhan, Milan) to little change (e.g., Rio de Janeiro, Taipei). On average, NO2 concentrations were 18 % lower than business as usual from February 2020 onward. China experienced the earliest and steepest decline, but concentrations since April have mostly recovered and remained within 5 % to the business as usual estimate. NO2 reductions in Europe and the US have been more gradual with a halting recovery starting in late March. We estimate that the global NOx (NO + NO2)…

Abstract. We developed incremental reactivity (IR) scales for 116 volatile organic compounds (VOCs) in a Chinese megacity (Guangzhou) and elucidated their application in calculating the ozone (O3) formation potential (OFP) in China. Two sets of model inputs (emission-based and observation-based) were designed to localize the IR scales in Guangzhou using the Master Chemical Mechanism (MCM) box model, and were also compared with those of the U.S. The two inputs differed in how primary pollutant inputs in the model were derived, with one based on emission data and the other based on observed pollutant levels, but the maximum incremental reactivity (MIR) scales derived from them were fairly similar. The IR scales showed a strong dependence on the chemical mechanism (MCM vs. Statewide Air Pollution Research Center), but the discrepancy between China and the U.S. using a similar chemical mechanism was not large. With a given chemical mechanism, the MIR scale for most VOCs showed a relatively small dependence on environmental conditions. However, when the NOx availability decreased, the IR…

Abstract. The characterization of oxygenated organic compounds in urban areas remains a pivotal gap in our understanding of the evolution of organic carbon under polluted environments, as the atmospheric processes involving interactions between organics and inorganics, anthropogenic pollutants and natural emissions lead to formation of various and complex secondary products. Here, we describe measurements of an iodide chemical ionization time-of-flight mass spectrometer installed with a Filter Inlet for Gases and AEROsols (FIGAERO-I-CIMS) in both gas-phase and particle-phase at an urban site in Guangzhou, a typical mega-city in southern China, during the autumn of 2018. Abundant oxygenated organic compounds containing 2~5 oxygen atoms were observed, including organic acids, multi-functional organics typically emitted form biomass burning, oxidation products of biogenic hydrocarbons and aromatics. Photochemistry played dominant roles in the formation of gaseous organic acids and isoprene-derived organic nitrates, while nighttime chemistry contributed significantly to the formation…

Abstract. Photochemical grid models (PGMs) are being applied more frequently to address diverse scientific and regulatory compliance associated with deteriorated air quality in China for the past decade. Solid evaluation of model performances guarantees the robustness and reliability of the baseline modelling results, so subsequent applications are built on top of it; thus, model performance evaluation (MPE) is a critical step of any PGM applications. MPE procedures and associated benchmarks have been proposed for PGM applications in the United States and Europe. However, with numerous input data needed, diverse model configurations, and evolution of the model itself, no two PGM applications are exactly the same. Therefore, those MPE benchmarks proposed based on studies outside China may not be appropriate for evaluation of the increasing number of PGM applications in China. Here we follow an established approach as published in previous literatures, to recommend statistical benchmarks for evaluation of simulated particulate matter (PM) concentrations in China. A total of 128…

Abstract. As a critical precursors of ozone (O3) and secondary organic aerosols, volatile organic compounds (VOCs) play a vital role in air quality, human health, and climate change. In this study, a campaign of comprehensive field observations and VOC grid sampling was conducted in Xi’an, China from June 20 to July 20, 2019 to identify the spatiotemporal concentration levels, sources, and secondary transformation potential of VOCs. During the observation period, the average VOC concentrations at the Chanba (CB), Di Huan Suo (DHS), Qinling (QL), and gridded sampling sites were 27.8 ± 8.9, 33.8 ± 10.5, 15.5 ± 5.8, and 29.1 ± 8.4 ppb, respectively. Vehicle exhaust was the primary source of VOC emissions in Xi’an, and the contributions of vehicle exhaust to VOCs at the CB, DHS, and QL sites were 41.3 %, 30.6 %, and 23.6–41.4 %, respectively. While industrial emissions were the second-largest source of VOCs in urban areas, contributions from ageing sources were high in rural areas. High potential source contribution function values primarily appeared in eastern and southern Xi’an near…

Abstract. We present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, and surface area concentrations in the case of wildfire smoke layers as well as estimates of smoke-related cloud condensation nucleus (CCN) and ice-nucleating particle (INP) concentrations from single-wavelength backscatter lidar measurements at ground and in space. A central role in the data analysis play conversion factors to convert the measured optical into microphysical properties. The set of needed conversion parameters for wildfire smoke are derived from AERONET observations of major smoke events caused by record-breaking wildfires in western Canada in August 2017 and southeastern Australia in January–February 2020. The new smoke analysis scheme is applied to stratospheric CALIPSO observations of fresh smoke plumes over northern Canada in 2017 and New Zealand in January 2020 and to ground-based lidar observation in southern Chile in aged Australian smoke layers in January 2020. These case studies show the potential of spaceborne and ground-based lidars to document…

Abstract. Aeolus is the first satellite mission to directly observe wind profile information on a global scale. After implementing a set of bias corrections, the Aeolus data products has gone public on 12 May 2020. However, Aeolus wind products over China were thus far not evaluated by in-situ comparison. In this study, the Mie-cloudy and Rayleigh-clear wind products from Aeolus measurements are validated against wind observations from the radar wind profiler (RWP) network in China. Based on the position of each RWP site relative to the closest Aeolus ground tracks, three matchup categories are proposed and comparisons between Aeolus wind products and RWP wind observations are performed for each category separately. The performance of Mie-cloudy wind products does not change much between the three matchup categories. On the other hand, for Rayleigh-clear and RWP wind products, Categories 1 and 2 are found to have much smaller differences, compared with category 3. This could be due to the RWP site being sufficiently approximate to Aeolus ground track for categories 1 and 2. In the…

Abstract. Nitro-aromatic compounds (NACs) were measured hourly at a rural site in China during wintertime to monitor the changes due to local and regional impacts of biomass burning (BB). Concurrent and continuous measurements of the concentrations of 16 NACs in the gas and particle phases were performed with a time-of-flight chemical ionization mass spectrometer (CIMS) equipped with a Filter Inlet for Gas and Aerosol (FIGAERO) unit using iodide as the reagent ion. NACs accounted for

Abstract. We present a satellite-derived global dust climatological record over the last two decades, including the monthly mean visible dust optical depth (DAOD) and vertical distribution of dust extinction coefficient at a 2º (latitude) × 5º (longitude) spatial resolution derived from CALIOP and MODIS. Dust is distinguished from non-dust aerosols based on particle shape information (e.g., lidar depolarization ratio) for CALIOP, and on dust size and absorption information (e.g., fine-mode fraction, Angstrom exponent, and single-scattering albedo) for MODIS, respectively. On multi-year average basis, the global (60° S–60° N) and annual mean DAOD is 0.029 and 0.063 derived from CALIOP and MODIS retrievals, respectively. In most dust active regions, CALIOP DAOD generally correlates well with the MODIS DAOD, with CALIOP DAOD being significantly smaller. CALIOP DAOD is 18 %, 34 %, 54 % and 31 % smaller than MODIS DAOD over Sahara Deserts, the tropical Atlantic Ocean, the Caribbean Sea, and the Arabian Sea, respectively. Over East Asia and the northwestern Pacific Ocean (NWP), however,…

Abstract. We use 2010–2015 GOSAT satellite observations of atmospheric methane columns over North America in a high- resolution inversion of methane emissions, including contributions from different sectors and long-term trends. The inversion involves analytical solution to the Bayesian optimization problem for a Gaussian mixture model (GMM) of the emission field with up to 0.5° × 0.625° resolution in concentrated source regions. Analytical solution provides a closed-form characterization of the information content from the inversion and facilitates the construction of a large ensemble of solutions exploring the effect of different uncertainties and assumptions. Prior estimates for the inversion include a gridded version of the EPA Inventory of U.S. Greenhouse Gas Emissions and Sinks (GHGI) and the WetCHARTS model ensemble for wetlands. Our best estimate for mean 2010–2015 US anthropogenic emissions is 30.6 (range: 29.4–31.3) Tg a-1, slightly higher than the gridded EPA inventory (28.7 (26.4–36.2) Tg a-1). The main discrepancy is for the oil and gas production sectors where we find…

Abstract. Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon (ROC) emissions. Among these sources are everyday items, such as personal care products, general cleaners, architectural coatings, pesticides, adhesives, and printing inks. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States, including spatial allocation to regional and local scales. Evaporation of species in the VCPy framework is a function of the compound specific physiochemical properties that govern volatilization and the timescale relevant for product evaporation. We introduce the terms evaporation timescale and use timescale, respectively, to describe these processes. Using this framework, predicted national, per-capita organic emissions from VCPs are 9.7 kg person−1 year−1 (6.5 kgC person−1 year−1) for 2016, which translates to 3.12 Tg (2.10 TgC), making VCPs a dominant source of anthropogenic organic emissions in the United States. Uncertainty associated with this framework and sensitivity to select…

Abstract. China is the largest cement producer and consumer in the world. Cement manufacturing is highly energy-intensive, and is one of the major contributors to carbon dioxide (CO2) and air pollutant emissions, which threatens climate mitigation and air quality improvement. In this study, we investigated the decadal changes of carbon dioxide and air pollutant emissions for the period of 1990–2015, based on intensive unit-based information on activity rates, production capacity, operation status, and control technologies, which improved the accuracy of the cement emissions in China. We found that, from 1990 to 2015, accompanied by a 10.9-fold increase in cement production, CO2, SO2, and NOx emissions from China's cement industry increased by 626 %, 59 %, and 658 %, whereas CO, PM2.5 and PM10 emissions decreased by 9 %, 66 %, and 63 %, respectively. In the 1990s, driven by the rapid growth of cement production, CO2 and air pollutant emissions increased constantly. Then, the production technology innovation of replacing traditional shaft kilns with the new precalciner kilns in the…

Abstract. The acidity of atmospheric aerosols regulates the particulate mass, composition and toxicity, and has important consequences for public health, ecosystems and climate. Despite these broad impacts, the global distribution and evolution of aerosol acidity are unknown. We used the particular, comprehensive atmospheric multiphase chemistry – climate model EMAC to investigate the main factors that control aerosol acidity, and uncovered remarkable variability and unexpected trends during the past 50 years in different parts of the world. We find that alkaline compounds, notably ammonium, and to a lesser extent crustal cations, buffer the aerosol pH on a global scale. Given the importance of aerosols for the atmospheric energy budget, cloud formation, pollutant deposition and public health, alkaline species hold the key to control strategies for air quality and climate change.

Abstract. Volcanic eruptions can cause significant disruption to society and numerical models are crucial for forecasting the dispersion of erupted material. Here we assess the skill and limitations of the Met Office’s Numerical Atmospheric-dispersion Modelling Environment (NAME) in simulating the dispersion of the sulfur dioxide (SO2) cloud from the 21–22 June 2019 eruption of the Raikoke volcano (48.3° N, 153.2° E). The eruption emitted around 1.5 ± 0.2 Tg of SO2, which represents the largest volcanic emission of SO2 into the stratosphere since the 2011 Nabro eruption. We simulate the temporal evolution of the volcanic SO2 cloud across the Northern Hemisphere (NH) and compare our model simulations to high-resolution SO2 measurements from the Tropospheric Monitoring Instrument (TROPOMI) and the Infrared Atmospheric Sounding Interferometer (IASI) satellite SO2 products. We show that NAME accurately simulates the observed location and horizontal extent of the SO2 cloud during the first 2–3 weeks after the eruption, but is unable, in its standard configuration, to capture the extent…

Abstract. During the one-year MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition the German icebreaker Polarstern drifted through the Arctic Ocean ice from October 2019 to May 2020, mainly at latitudes between 85° N and 88.5° N. A multiwavelength polarization Raman lidar was operated aboard the research vessel and continuously monitored aerosol and cloud layers up to 30 km height. The highlight of the lidar measurements was the detection of a persistent, 10 km deep wildfire smoke layer in the upper troposphere and lower stratosphere (UTLS) from about 7–8 km to 17–18 km height. The smoke layer was present throughout the winter half year until the polar vortex, the strongest of the last 40 years, collapsed in late April 2020. The smoke originated from major fire events, especially from extraordinarily intense and long-lasting Siberian fires in July and August 2019. In this article, we summarize the main findings of our seven-month smoke observations and characterize the aerosol properties and decay of the stratospheric perturbation in terms of…

Abstract. Urban aerosol measurements are necessary to establish associations between air pollution and human health outcomes and to evaluate the efficacy of air quality legislation and emissions standards. The measurement of urban aerosol particle size distributions (PSDs) is of particular importance as they enable for characterization of size-dependent processes that govern a particle’s transport, transformation, and fate in the urban atmosphere. PSDs also improve our ability to link air pollution to health effects through evaluation of particle deposition in the respiratory system and inhalation toxicity. To provide guidance for the evolution of urban aerosol observations, this paper reviews and critically analyzes the current state-of-knowledge on urban aerosol PSD measurements by synthesizing n = 793 PSD observations made between 1998 to 2017 in n = 125 cities in n = 51 countries around the globe. Significant variations in the shape and magnitude of urban aerosol number and mass PSDs were identified among different geographical regions. In general, number PSDs in Europe (EU),…

Abstract. Methane emissions associated with the production, transport, and use of oil and natural gas increase the climatic impacts of energy use; however, little is known about how emissions vary temporally and with commodity prices. We present airborne and ground-based data, supported by satellite observations, to measure weekly to monthly changes in total methane emissions in the United States’ Permian Basin during a period of volatile oil prices associated with the COVID-19 pandemic. As oil prices declined from ~$ 60 to $ 20 per barrel, emissions changed concurrently from 3.4 % to 1.5 % of gas production; as prices partially recovered, emissions increased back to near initial values. Concurrently, total oil and natural gas production only declined by a maximum of ~10 % from the peak values seen in the months prior to the crash. Activity data indicate that a rapid decline in well development and subsequent effects on associated gas flaring and midstream infrastructure throughput are the likely drivers of temporary emission reductions. Our results, along with past satellite…

Abstract. Ice-nucleating particles (INPs) trigger the formation of cloud ice crystals in the atmosphere. Therefore, they strongly influence cloud microphysical and optical properties, as well as precipitation and the life cycle of clouds. Improving weather forecasting and climate projection requires an appropriate formulation of atmospheric INP concentrations. This remains challenging, as the global INP distribution and variability depend on a variety of aerosol types and sources, and neither their short-term variability nor their long-term seasonal cycles are well covered by continuous measurements. Here, we provide the first year-long set of observations with a pronounced INP seasonal cycle in a boreal forest environment. Besides the observed seasonal cycle in INP concentrations with a minimum in wintertime and maxima in early and late summer, we also provide indications for a seasonal variation in the prevalent INP type. We show that the seasonal dependency of INP concentrations and prevalent INP types is most likely driven by the abundance of biogenic aerosol. As current…