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The Copernicus Atmosphere Monitoring Service (CAMS) is providing daily analyses and forecasts of the composition of the atmosphere, including the reactive gases such as O3, CO, NO2, HCHO, SO2, aerosol species and greenhouse gases. The global CAMS analysis system (IFS-COMPO) is based on the ECMWF Integrated Forecast System (IFS) for numerical weather prediction (NWP), and assimilates a large number of composition satellite products on top of the meteorological observations ingested in IFS. The CAMS system receives regular upgrades, following the upgrades of IFS. The last upgrade, Cy48R1, operational since 27 June 2023, was major with a large number of code changes, both for COMPO and for NWP. The main COMPO innovations include the introduction of full stratospheric chemistry, a major update of the emissions, of the aerosol model, including the representation of secondary organic aerosol, several updates of the dust life cycle and optics, inorganic chemistry in the troposphere, and the assimilation of VIIRS AOD and TROPOMI CO. The CAMS Cy48R1 upgrade was validated using a large number of independent measurement datasets, including surface in situ, surface remote sensing, routine aircraft and balloon and satellite observations. In this paper we present the validation results for Cy48R1 by comparing with the skill of the previous operational system (Cy47R3), with the independent observations as reference, for the period October 2022 to June 2023 during which daily forecasts from both cycles are available. Major improvements in skill are found for the ozone profile in the lower-middle stratosphere and for stratospheric NO2 due to the inclusion of full stratospheric chemistry. Stratospheric trace gases compare well with ACE-FTS observations between 10–200 hPa, with larger deviations between 1–10 hPa. The impact of the updated emissions is especially visible over East Asia and is beneficial for the trace gases O3, NO2, and SO2. The CO column assimilation is now anchored by IASI instead of MOPITT which is beneficial for most of the CO comparisons, and the assimilation of TROPOMI CO data improves the model CO field in the troposphere. In general the aerosol optical depth has improved globally, but the dust evaluation shows more mixed results. The results of the 47 comparisons are summarised in a score card, which shows that 83 % of the evaluation datasets show a neutral or improved performance of Cy48R1 compared to the previous operational CAMS system, while 17 % indicate a (slight) degradation. This demonstrates the overall success of this upgrade. [ABSTRACT FROM AUTHOR]

Cold extremes have large impacts on human society. Understanding the physical processes dominating the changes in cold extremes is crucial for a reliable projection of future climate change. The observed cold extremes have decreased during the last several decades, and this trend will continue under future global warming. Here, we quantitatively identify the contributions of dynamic (changes in large-scale atmospheric circulation) and thermodynamic (rising temperatures resulting from global warming) effects to East Asian cold extremes in the past several decades and in a future warm climate by using two sets of large-ensemble simulations of climate models. We show that the dynamic component accounts for over 80 % of the cold-month (coldest 5 % boreal winter months) surface air temperature (SAT) anomaly over the past 5 decades. However, in a future warm climate, the thermodynamic change is the main contributor to the decreases in the intensity and occurrence probability of East Asian cold extremes, while the dynamic change is also contributive. The intensity of East Asian cold extremes will decrease by around 5 °C at the end of the 21st century, in which the thermodynamic (dynamic) change contributes approximately 75 % (25 %). The present-day (1986–2005) East Asian cold extremes will almost never occur after around 2035, and this will happen 10 years later due solely to thermodynamic change. The upward trend of a positive Arctic Oscillation-like sea level pressure pattern dominates the changes in the dynamic component. The finding provides a useful reference for policymakers in climate change adaptation activities. [ABSTRACT FROM AUTHOR]

Reliable attribution of Asian summer monsoon variations to aerosol forcing is critical to reducing uncertainties in future projections of regional water availability, which is of utmost importance for risk management and adaptation planning in this densely populated region. Yet, simulating the monsoon remains a challenge for climate models that suffer from long-standing biases, undermining their reliability in attributing anthropogenically forced changes. We analyze a suite of climate model experiments to identify a link between model biases and monsoon responses to Asian aerosols and associated physical mechanisms, including the role of large-scale circulation changes. The aerosol impact on monsoon precipitation and circulation is strongly influenced by a model's ability to simulate the spatio-temporal variability in the climatological monsoon winds, clouds, and precipitation across Asia, which modulates the magnitude and efficacy of aerosol–cloud–precipitation interactions, an important component of the total aerosol response. There is a strong interplay between South Asia and East Asia monsoon precipitation biases and their relative predominance in driving the overall monsoon response. We found a striking contrast between the early- and late-summer aerosol-driven changes ascribable to opposite signs and seasonal evolution of the biases in the two regions. A realistic simulation of the evolution of the large-scale atmospheric circulation is crucial to realize the full extent of the aerosol impact over Asia. These findings provide important implications for better understanding and constraining the diversity and inconsistencies of model responses to aerosol changes over Asia in historical simulations and future projections. [ABSTRACT FROM AUTHOR]

Nitrogen oxide radicals (NOx≡NO+NO2) emitted by fuel combustion are important precursors of ozone and particulate matter pollution, and NO 2 itself is harmful to public health. The Geostationary Environment Monitoring Spectrometer (GEMS), launched in space in 2020, now provides hourly daytime observations of NO 2 columns over East Asia. This diurnal variation offers unique information on the emission and chemistry of NOx , but it needs to be carefully interpreted. Here we investigate the drivers of the diurnal variation in NO 2 observed by GEMS during winter and summer over Beijing and Seoul. We place the GEMS observations in the context of ground-based column observations (Pandora instruments) and GEOS-Chem chemical transport model simulations. We find good agreement between the diurnal variations in NO 2 columns in GEMS, Pandora, and GEOS-Chem, and we use GEOS-Chem to interpret these variations. NOx emissions are 4 times higher in the daytime than at night, driving an accumulation of NO 2 over the course of the day, offset by losses from chemistry and transport (horizontal flux divergence). For the urban core, where the Pandora instruments are located, we find that NO 2 in winter increases throughout the day due to high daytime emissions and increasing NO2/NOx ratio from entrainment of ozone, partly balanced by loss from transport and with a negligible role of chemistry. In summer, by contrast, chemical loss combined with transport drives a minimum in the NO 2 column at 13:00–14:00 local time (LT). Segregation of the GEMS data by wind speed further demonstrates the effect of transport, with NO 2 in winter accumulating throughout the day at low winds but flat at high winds. The effect of transport can be minimized in summer by spatially averaging observations over the broader metropolitan scale, under which conditions the diurnal variation in NO 2 reflects a dynamic balance between emission and chemical loss. [ABSTRACT FROM AUTHOR]

Anthropogenic emissions of aerosols and precursor gases have changed significantly in the past few decades around the world. In this study, the Explicit Aerosol Source Tagging (EAST) system is merged into the Energy Exascale Earth System Model version 1 (E3SMv1) to quantify the variations in anthropogenic aerosol concentrations, source contributions, and their subsequent radiative impact in four major emission regions across the globe during 1850–1980, 1980–2010, and 2010–2017. In North America and Europe, changes in anthropogenic PM2.5 were mainly caused by changes in emissions from local energy and industrial sectors. The local industrial sector caused the largest increase in PM2.5 in East Asia during 1980–2010 and decrease during 2010–2017. In South Asia, the increase in energy-related emissions dominated the rise in PM2.5 levels during 1980–2017. During 1850–1980, the increases in emissions from North America contributed to the increase in the European PM2.5 burden by 1.7 mgm-2 and the sources from the Europe were also responsible for the PM2.5 burden increase in East Asia and South Asia by about 1.0 mgm-2. During 1980–2010, East Asia contributed to an increase of 0.4–0.6 mgm-2 in the PM2.5 burden in North America and Europe, while South Asia contributed about 0.3 mgm-2. During 2010–2017, the contributions from East Asia to the PM2.5 burdens in the North America, Europe, and South Asia declined by 0.3–0.6 mgm-2 due to the clean air actions in China, while the contributions from South Asia still increased due to the continuous increase in emissions in South Asia. The historical changes in aerosols had an impact on effective radiative forcing through aerosol–radiation interactions (ERFari). During 1980–2010, a decline in North American aerosols resulted in a positive ERFari change (warming effect) in Europe and a decline in aerosols in Europe caused a warming effect in Russia and northern China. The changes in ERFari from the increase and decrease in aerosols in China during 1980–2010 and 2010–2017, respectively, are comparable in magnitude. The continuous aerosol increases in South Asia from 1980 to 2017 resulted in negative ERFari (cooling) changes in South Asia, Southeast Asia, and southern China. [ABSTRACT FROM AUTHOR]

The current best-estimate of the global annual mean radiative forcing (RF) attributable to contrail cirrus is thought to be 3 times larger than the RF from aviation's cumulative CO 2 emissions. Here, we simulate the global contrail RF for 2019–2021 using reanalysis weather data and improved engine emission estimates along actual flight trajectories derived from Automatic Dependent Surveillance–Broadcast telemetry. Our 2019 global annual mean contrail net RF (62.1 mW m -2) is 44 % lower than current best estimates for 2018 (111 [33, 189] mW m -2 , 95 % confidence interval). Regionally, the contrail net RF is largest over Europe (876 mW m -2) and the USA (414 mW m -2), while the RF values over East Asia (64 mW m -2) and China (62 mW m -2) are close to the global average, because fewer flights in these regions form persistent contrails resulting from lower cruise altitudes and limited ice supersaturated regions in the subtropics due to the Hadley Circulation. Globally, COVID-19 reduced the flight distance flown and contrail net RF in 2020 (- 43 % and - 56 %, respectively, relative to 2019) and 2021 (- 31 % and - 49 %, respectively) with significant regional variations. Around 14 % of all flights in 2019 formed a contrail with a net warming effect, yet only 2 % of all flights caused 80 % of the annual contrail energy forcing. The spatiotemporal patterns of the most strongly warming and cooling contrail segments can be attributed to flight scheduling, engine particle number emissions, tropopause height, and background radiation fields. Our contrail RF estimates are most sensitive to corrections applied to the global humidity fields, followed by assumptions on the engine particle number emissions, and are least sensitive to radiative heating effects on the contrail plume and contrail–contrail overlapping. Using this sensitivity analysis, we estimate that the 2019 global contrail net RF could range between 34.8 and 74.8 mW m -2. [ABSTRACT FROM AUTHOR]

The interactions between the terrestrial biosphere, atmospheric chemistry, and climate involve complex feedbacks that have traditionally been modeled separately. We present a new framework that couples the Yale Interactive terrestrial Biosphere (YIBs) model, a dynamic plant-chemistry model, with the RegCM-Chem model. RegCM-Chem–YIBs integrates meteorological variables and atmospheric chemical composition from RegCM-Chem with land surface parameters from YIBs. The terrestrial carbon flux calculated by YIBs is fed back into RegCM-Chem interactively, thereby representing the interactions between fine particulate matter (PM 2.5), ozone (O 3), and carbon dioxide (CO 2). For testing purposes, we carry out a 1-year simulation (2016) at a 30 km horizontal resolution over East Asia with RegCM-Chem–YIBs. The model accurately captures the spatio-temporal distribution of climate, chemical composition, and ecological parameters. In particular, the estimated O 3 and PM 2.5 are consistent with ground observations, with correlation coefficients (R) of 0.74 and 0.65, respectively. The simulated CO 2 concentration is consistent with observations from six sites (R ranged from 0.89 to 0.97) and exhibits a similar spatial pattern when compared with carbon assimilation products. RegCM-Chem–YIBs produces reasonably good gross primary productivity (GPP) and net primary productivity (NPP), showing seasonal and spatial distributions consistent with satellite observations, and mean biases (MBs) of 0.13 and 0.05 kg C m -2 yr -1. This study illustrates that RegCM-Chem–YIBs is a valuable tool to investigate coupled interactions between the terrestrial carbon cycle, atmospheric chemistry, and climate change at a higher resolution on a regional scale. [ABSTRACT FROM AUTHOR]

The use of remote sensing methods to accurately measure cloud properties and their spatiotemporal changes has been widely welcomed in many fields of atmospheric research. The Nanjing Joint Institute for Atmospheric Sciences (NJIAS) Himawari-8/9 Cloud Feature Dataset (HCFD) provides a comprehensive description of cloud features over the East Asia and west North Pacific regions for the 7-year period from April 2016 to December 2022. Multiple cloud variables, such as cloud mask, phase/type, top height, optical thickness, and particle effective radius, as well as snow, dust, and haze masks, were generated from the visible and infrared measurements of the Advanced Himawari Imager (AHI) on board the Japanese geostationary satellites Himawari-8 and Himawari-9 using a series of recently developed cloud retrieval algorithms. Verifications with the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) 1 km cloud layer product and the Moderate Resolution Imaging Spectroradiometer (MODIS) Level-2 cloud product (MYD06) demonstrate that the NJIAS HCFD gives higher skill scores than the Japanese Himawari-8/9 operational cloud product for all cloud variables except for cloud particle effective radius. The NJIAS HCFD even outperforms the MYD06 in nighttime cloud detection; cloud-top height, pressure, and temperature estimation; and infrared-only cloud-top phase determination. All evaluations are performed at the nominal 2 km scale, not including the effects of sub-pixel cloudiness or very thin cirrus. Two examples are presented to demonstrate applications of the NJIAS HCFD for climate and typhoon research. The NJIAS HCFD has been published in the Science Data Bank (https://doi.org/10.57760/sciencedb.09950 , Zhuge 2023a; https://doi.org/10.57760/sciencedb.09953 , Zhuge 2023b; https://doi.org/10.57760/sciencedb.09954 , Zhuge 2023c; https://doi.org/10.57760/sciencedb.10158 , Zhuge 2023d; https://doi.org/10.57760/sciencedb.09945 , Zhuge 2023e). [ABSTRACT FROM AUTHOR]

Over the past few decades, the tropospheric ozone precursor anthropogenic emissions: nitrogen oxides (NOx) and reactive carbon (RC) from mid-latitude regions have been decreasing, and those from Asia and tropical regions have been increasing, leading to an equatorward emission redistribution. In this study, we quantify the contributions of various sources of NOx and RC emissions to tropospheric ozone using a source attribution technique during the 2000–2018 period in a global chemistry transport model: CAM4-Chem. We tag the ozone molecules with the source of their NOx or RC precursor emission in two separate simulations, one for each of NOx and RC. These tags include various natural (biogenic, biomass burning, lightning and methane), and regional anthropogenic (North American, European, East Asian, South Asian etc.) precursor emission sources. We simulate ~336 Tg O3 with an increasing trend of 0.91 Tg O3/yr (0.28 %/yr), largely contributed (and trend driven) by anthropogenic NOx emissions and methane. The ozone production efficiency of regional anthropogenic NOx emissions increases significantly when emissions decrease (Europe, North American and Russia-Belarus-Ukraine region's emissions) and decreases significantly when emissions increase (South Asian, Middle Eastern, International Shipping etc.). Tropical regions, despite smaller emissions, contribute more to tropospheric ozone burden compared to emissions from higher latitudes, consistent with previous work, due to large convection at the tropics thereby lifting O3 and its precursor NOx molecules into the free troposphere where ozone's lifetime is longer. We contrast the contribution to tropospheric ozone burden with that of the contribution to the global surface ozone. We simulate a smaller relative contribution from tropical regions to the global mean surface ozone compared to their contribution to the tropospheric ozone burden. The global population-weighted mean ozone (related to ozone exposure) is much larger compared to surface mean, mainly due to large anthropogenic emissions from densely populated regions: East Asia, South Asia, and other tropical regions, and a substantial contribution from international ship NOx emissions. The increasing trends in anthropogenic emissions from these regions are the main drivers of increasing global population-weighted mean ozone. [ABSTRACT FROM AUTHOR]

The concentration of carbonaceous aerosols, black carbon (BC) and organic aerosol (OA), in the atmosphere is related to co-emitted or co-produced trace gases. In this study, we investigate the most relevant proportional relationships between both BC and OA with the following trace gases: carbon monoxide (CO), formaldehyde (HCHO), nitrogen dioxide (NO2), ozone (O3), and sulfur dioxide (SO2). One motivation for selecting these trace gases is that they can be observed using remote sensing measurements from satellite instrumentation, and could therefore be used to predict spatial changes in the amounts of BC and OA. Airborne measurements are optimal for the analysis of both the composition of aerosols and trace gases in different environments ranging from unpolluted oceanic air masses to those in heavily polluted city plumes. The two aircraft campaigns of the EMeRGe (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global Scales) project have created a unique database, with flight plans dedicated to studying city plumes in two regions, Europe (2017) and East Asia (2018), along with identical instrumental payload. Using linear regression analysis, three relevant relationships between carbonaceous aerosol and trace gases are identified: - The BC/OA ratio observed in the Asian campaign is three times higher (≈ 0.3) than in the European campaign (≈ 0.1), whereas the Pearson correlation coefficient (R) between BC and OA is much higher in Europe (R ≈ 0.8) than in Asia (R ≈ 0.6). - The CO/BC ratio is also observed higher in the Asian campaign (≈ 240) than in the European campaign (≈ 170), whereas the R-value between CO and BC is similar for both campaigns (R ≈ 0.7). - The HCHO/OA ratio is similar in both campaigns (≈0.32), but the observed R-values between HCHO and OA is higher in Europe than in the Asia (R ≈ 0.7 compared to ≈ 0.3). By focusing on heavily polluted air masses sampled downwind in the city plumes, the ratios between the observed carbonaceous aerosols and the five trace gases change, and the R-values increase with O3 for both BC and OA (R ≈ 0.5). To assess the performance of atmospheric models with respect to the most relevant observed relationships, an air quality model ensemble is used to represent the current state of atmospheric modeling, consisting of two global and two regional simulations. The evaluation shows that these proportional relationships are not satisfactorily reproduced by the model ensemble. The relationships between BC and OA or between CO and BC are modeled with stronger correlations than the observed ones, and their higher ratios observed in Asia compared to Europe are not reproduced. Furthermore, the modeled HCHO/OA ratio is underestimated in the Asian campaign and overestimated in the European campaign. This analysis of the proportional relationships between carbonaceous aerosols and trace gases implies that the observed relationships can be used to constrain models and improve anthropogenic emission inventories. In addition, it implies that information about the lower tropospheric concentration of carbonaceous aerosols can potentially be inferred from satellite retrievals of trace gases, particularly in the plumes from megacities. [ABSTRACT FROM AUTHOR]

Biogenic volatile organic compounds (BVOCs) are important precursors to ozone and secondary organic aerosols in the atmosphere, affecting air quality, clouds, and climate. However, the trend in BVOC emissions and driving factors for the emission changes in different geographic regions over the past 2 decades has remained unclear. Here, regional to global changes in BVOC emissions during 2001–2020 are simulated using the latest Model of Emission of Gases and Aerosols from Nature (MEGANv3.2) with the input of time-varying satellite-retrieved vegetation and reanalysis meteorology data. Comparison of model simulations with the site observations shows that the model can reasonably reproduce the magnitude of isoprene and monoterpene emission fluxes. The spatial distribution of the modeled isoprene emissions is generally comparable to the satellite retrievals. The estimated annual average global BVOC emissions are 835.4 Tg yr -1 with the emissions from isoprene, monoterpenes, sesquiterpenes, and other BVOC comprised of 347.7, 184.8, 23.3, and 279.6 Tg yr -1 , respectively. We find that the decrease in global isoprene emissions (-0.07 % per year) caused by the increase in CO 2 concentrations (-0.20 % per year) is stronger than that caused by changes in vegetation (-0.03 % per year) and meteorological factors (0.15 % per year). However, regional disparities are large. Isoprene emissions increase significantly in Europe, East Asia, and South Asia (0.37 % per year–0.66 % per year). Half of the increasing trend is contributed by increased leaf area index (LAI) (maximum over 0.02 m 2 m -2 yr -1) and tree cover. Changes in meteorological factors contribute to another half, with elevated temperature dominating in Europe and increased soil moisture dominating in East and South Asia. In contrast, in South America and Southeast Asia, shifts in vegetation type associated with the BVOC emission capacity, which partly results from the deforestation and agricultural expansion, decrease the BVOC emission and offset nearly half of the emission increase caused by changes in meteorological factors. Overall, isoprene emission increases by 0.35 % per year and 0.25 % per year in South America and Southeast Asia, respectively. In Central Africa, a decrease in temperature dominates the negative emission trend (-0.74 % per year). Global monoterpene emissions show a significantly increasing trend (0.34 % per year, 0.6 Tg yr -1) compared to that of isoprene (-0.07 % per year, -0.2 Tg yr -1) , especially in strong greening hotspots. This is mainly because the monoterpene emissions are more sensitive to changes in LAI and are not subject to the inhibition effect of CO 2. The findings highlight the important roles of vegetation cover and biomass, temperature, and soil moisture in modulating the temporal variations of global BVOC emissions in the past 2 decades. [ABSTRACT FROM AUTHOR]

Organic aerosols from marine sources over the western Pacific Ocean of East Asia were investigated using an online coupled regional chemistry–climate model RIEMS-Chem for the entire year 2014. Model evaluation against a wide variety of observations from research cruises and in situ measurements demonstrated a good skill of the model in simulating temporal variation and spatial distribution of particulate matter with aerodynamic diameter less than 2.5 and 10 µm (PM 2.5 and PM 10), black carbon (BC), organic carbon (OC), sodium, and aerosol optical depth (AOD) in the marine atmosphere. The inclusion of marine organic aerosols improved model performance on OC concentration by reducing model biases of up to 20 %. The regional and annual mean near-surface marine organic aerosol (MOA) concentration was estimated to be 0.27 µgm-3 , with the maximum in spring and the minimum in winter, and contributed 26 % of the total organic aerosol concentration on average over the western Pacific. Marine primary organic aerosol (MPOA) accounted for the majority of marine organic aerosol (MOA) mass, and the MPOA concentration exhibited the maximum in autumn and the minimum in summer, whereas marine secondary organic aerosol (MSOA) was approximately 1–2 orders of magnitude lower than MPOA, having a distinct summer maximum and a winter minimum. MOA induced a direct radiative effect (DRE MOA) of - 0.27 Wm-2 and an indirect radiative effect (IRE MOA) of - 0.66 Wm-2 at the top of the atmosphere (TOA) in terms of annual and oceanic average over the western Pacific, with the highest seasonal mean IRE MOA up to - 0.94 Wm-2 in spring. IRE MOA was stronger than, but in a similar magnitude to, the IRE due to sea salt aerosol on average, and it was approximately 9 % of the IRE due to anthropogenic aerosols in terms of annual mean over the western Pacific. This ratio increased to 19 % in the northern parts of the western Pacific in autumn. This study reveals an important role of MOA in perturbing cloud properties and shortwave radiation fluxes in the western Pacific of East Asia. [ABSTRACT FROM AUTHOR]

In this study, the WRF-Chem v4.4 model was utilized to evaluate the sensitivity of O 3 simulations with three bottom-up emission inventories (EDGAR-HTAP v2 and v3 and KORUS v5) using surface and aircraft data in East Asia during the Korea-United States Air Quality (KORUS-AQ) campaign period in 2016. All emission inventories were found to reproduce the diurnal variations of O 3 and its main precursor NO 2 as compared to the surface monitor data. However, the spatial distributions of the daily maximum 8 h average (MDA8) O 3 in the model do not completely align with the observations. The model MDA8 O 3 had a negative (positive) bias north (south) of 30° N over China. All simulations underestimated the observed CO by 50 %–60 % over China and South Korea. In the Seoul Metropolitan Area (SMA), EDGAR-HTAP v2 and v3 and KORUS v5 simulated the vertical shapes and diurnal patterns of O 3 and other precursors effectively, but the model underestimated the observed O 3 , CO, and HCHO concentrations. Notably, the model aromatic volatile organic compounds (VOCs) were significantly underestimated with the three bottom-up emission inventories, although the KORUS v5 shows improvements. The model isoprene estimations had a positive bias relative to the observations, suggesting that the Model of Emissions of Gases and Aerosols from Nature (MEGAN) version 2.04 overestimated isoprene emissions. Additional model simulations were conducted by doubling CO and VOC emissions over China and South Korea to investigate the causes of the model O 3 biases and the effects of the long-range transport on the O 3 over South Korea. The doubled CO and VOC emission simulations improved the model O 3 simulations for the local-emission-dominant case but led to the model O 3 overestimations for the transport-dominant case, which emphasizes the need for accurate representations of the local VOC emissions over South Korea. [ABSTRACT FROM AUTHOR]

This study explores the differences in performance and results by various versions of the ISORROPIA thermodynamic module implemented within the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. Three different versions of the module were used, ISORROPIA II v1, ISORROPIA II v2.3, and ISORROPIA-lite. First, ISORROPIA II v2.3 replaced ISORROPIA II v1 in EMAC to improve pH predictions close to neutral conditions. The newly developed ISORROPIA-lite has been added to EMAC alongside ISORROPIA II v2.3. ISORROPIA-lite is more computationally efficient and assumes that atmospheric aerosols exist always as supersaturated aqueous (metastable) solutions, while ISORROPIA II includes the option to allow for the formation of solid salts at low RH conditions (stable state). The predictions of EMAC by employing all three aerosol thermodynamic models were compared to each other and evaluated against surface measurements from three regional observational networks in the polluted Northern Hemisphere (Interagency Monitoring of Protected Visual Environments (IMPROVE), European Monitoring and Evaluation Programme (EMEP), and Acid Deposition Monitoring Network of East Asia (EANET)). The differences between ISORROPIA II v2.3 and ISORROPIA-lite were minimal in all comparisons with the normalized mean absolute difference for the concentrations of all major aerosol components being less than 11 % even when different phase state assumptions were used. The most notable differences were lower aerosol concentrations predicted by ISORROPIA-lite in regions with relative humidity in the range of 20 % to 60 % compared to the predictions of ISORROPIA II v2.3 in stable mode. The comparison against observations yielded satisfactory agreement especially over the USA and Europe but higher deviations over East Asia, where the overprediction of EMAC for nitrate was as high as 4 µ g m -3 (∼20%). The mean annual aerosol pH predicted by ISORROPIA-lite was on average less than a unit lower than ISORROPIA II v2.3 in stable mode, mainly for coarse-mode aerosols over the Middle East. The use of ISORROPIA-lite accelerated EMAC by nearly 5 % compared to the use of ISORROPIA II v2.3 even if the aerosol thermodynamic calculations consume a relatively small fraction of the EMAC computational time. ISORROPIA-lite can therefore be a reliable and computationally efficient alternative to the previous thermodynamic module in EMAC. [ABSTRACT FROM AUTHOR]

Atmospheric deposition is an important source of marine metallic elements, which have a non-negligible impact on marine ecology. Atmospheric trace metals come from different sources, undergo their respective transport processes, and are deposited into seas finally. This study aims to provide gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals by the modified Community Multiscale Air Quality (CMAQ) model. A monthly emission inventory of six metals – Fe, Al, V, Ni, Zn, and Cu – from land anthropogenic, ship, and dust sources in East Asia (0–55° N, 85–150° E) in 2017 was developed. Most metals came mainly from land-based sources, contributing over 80 %. The annual marine atmospheric deposition fluxes of Fe, Al, V, Ni, Zn, and Cu were 9614, 15000, 102, 84, 171, 88 μg·m-2, and soluble deposition fluxes were 646.8, 1799.6, 43.3, 36.3, 118.4, 42.9 μg·m-2, respectively. Contributions of each source for trace metals varied in emissions, atmospheric concentrations, and depositions. Dust source, as a main contributor of Fe and Al, accounted for a higher proportion of emissions (~90 %) than marine deposition fluxes (~20 %). However, anthropogenic sources have larger shares of marine deposition flux compared with emissions. The deposition of Zn, Cu, and soluble Fe in East Asian seas was dominated by land anthropogenic sources, while V and Ni were dominated by shipping. The seasonal gridded data and the identification of the dominant source of metal deposition offer a foundation for dynamic assessments of the marine ecological effects of atmospheric trace metals. This study also implies the importance of potential co-synthesis and complementation effects of multiple trace elements deposited into marine ecosystems. [ABSTRACT FROM AUTHOR]

Reliable attribution of Asian summer monsoon variations to aerosol forcing is critical to reducing uncertainties in future projections of regional water availability, which is of utmost importance for risk management and adaptation planning in this densely populated region. Yet, simulating the monsoon remains a challenge for climate models which suffer from long-standing biases, undermining their reliability in attributing anthropogenically-forced changes. We analyse a suite of climate model experiments to identify a link between model biases and monsoon responses to Asian aerosols, and the physical mechanism underpinning this link, including the role of large-scale circulation changes. The aerosol impact on monsoon precipitation and circulation is strongly influenced by a model's ability to simulate the spatial distribution and temporal variability of the climatological monsoon winds, clouds and precipitation across Asia, which critically modulates the magnitude and efficacy of aerosol-cloud-precipitation interactions, the predominant driver of the total aerosol response. There is a strong interplay between South and East Asia monsoon precipitation biases and their relative predominance in driving the overall monsoon response. We found a striking contrast between the early and late summer aerosol-driven changes ascribable to opposite signs and seasonal evolution of the biases in the two regions. A realistic simulation of the evolution of the large-scale atmospheric circulation is crucial to realise the full extent of the aerosol impact over Asia. These findings provide important implications to better understand and constrain the diversity and inconsistencies of model responses to aerosol changes over Asia in historical simulations and future projections. [ABSTRACT FROM AUTHOR]

Methods based on the absorption Ångström exponent (AAE) are widely used to estimate the absorption by brown carbon (BrC), and the estimated absorption by BrC can be significantly different from 0, even for pure black carbon (BC). However, few studies have systematically quantified the effects of BC microphysical properties. Moreover, the conditions under which AAE-based methods are applicable are still unclear. In this work, we used BC models partially coated with non-absorbing materials to calculate the total absorption. Since the total absorption is entirely due to BC, the estimated BrC absorption should be 0 if the retrieval methods are accurate. Thus, the ratio of the estimated BrC absorption to BC absorption (ABS BrC) should be the proportion of the BC absorption that is incorrectly attributed to BrC. The results show that a BC AAE of 1 can generally provide reasonable estimates for freshly emitted BC, since ABS BrC is generally in the range of -4.8 % to 2.7 % during that period. However, when BC aerosols are aged, ABS BrC can sometimes reach about 38.7 %. The wavelength dependence of the AAE (WDA) method does not necessarily improve the estimates; sometimes a negative ABSBrC of about -40.8 % is found for partially coated BC. By combining simulations of a global chemical transport model, this work also quantified the effects of BC microphysical properties on BrC global aerosol absorption optical depth (AAOD) estimates. The AAE = 1 method sometimes leads to a misassigned global mean AAOD of about - 0.43– 0.46×10-3 if the BC aerosols have a complex morphology. The WDA method does not necessarily improve the estimates. In our cases, the WDA methods based on spherical models could lead to a global-mean misassigned AAOD range of about -0.87 – 0.04×10-3. At the regional scale, the AAE = 1 method sometimes leads to a distributed AAOD of about -7.3 to 5.7×10-3 in some specific regions. Mie-theory-based WDA methods lead to an estimated AAOD error of about -22×10-3 in some regions (e.g., East Asia). This work also showed that the misattributed BrC absorption would lead to substantial uncertainties in the estimation of the global direct radiative forcing (DRF) of absorbing aerosols from different sources. [ABSTRACT FROM AUTHOR]