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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 surge (CS) is considered a favorable weather process to improve air quality and is widely recognized. However, there is no detailed study on the differences in the dispersion ability of different types of CSs in relation to haze days in eastern China (HD EC). This paper uses the hierarchical clustering algorithm to classify the cool-season (November to February of the following year) CSs across eastern China into blocking CSs and wave-train CSs and compares their influences on the number of HD EC from 1980 to 2017. Results show that the wave-train CSs can significantly improve the visibility in eastern China and generally improve air quality for about 2 d longer than the blocking CSs, which indicates that the blocking CSs have a weaker ability to dissipate HD EC compared with the wave-train CSs. The CSs affect the HD EC by changing meteorological elements like thermal inversion potential, horizontal surface wind, sea level pressure (SLP), and surface air temperature (SAT). A period of 4 d after the outbreak of CSs, the variations of thermal inversion potential and horizontal surface wind of two types of CSs tend to be consistent. However, the negative SAT anomalies and the positive SLP anomalies caused by the blocking CSs lasted shorter than those caused by the wave-train CSs, forming favorable conditions for the rapid growth of HD EC. Furthermore, results show that in recent years, especially after the 1990s, the frequency of wave-train CSs has decreased significantly, while the frequency of blocking CSs has slightly increased, indicating that the overall ability of CSs to dissipate HD EC has weakened in general. This work may provide reference for the future formulation of haze control policies in East Asia. [ABSTRACT FROM AUTHOR]

When calibrating simulations of dust clouds, both the intensity and the position are important. Intensity errors arise mainly from uncertain emission and sedimentation strengths, while position errors are attributed either to imperfect emission timing or to uncertainties in the transport. Though many studies have been conducted on the calibration or correction of dust simulations, most of these focus on intensity solely and leave the position errors mainly unchanged. In this paper, a grid-distorted data assimilation, which consists of an image-morphing method and an ensemble-based variational assimilation, is designed for realigning a simulated dust plume to correct the position error. This newly developed grid-distorted data assimilation has been applied to a dust storm event in May 2017 over East Asia. Results have been compared for three configurations: a traditional assimilation configuration that focuses solely on intensity correction, a grid-distorted data assimilation that focuses on position correction only and the hybrid assimilation that combines these two. For the evaluated case, the position misfit in the simulations is shown to be dominant in the results. The traditional emission inversion only slightly improves the dust simulation, while the grid-distorted data assimilation effectively improves the dust simulation and forecasting. The hybrid assimilation that corrects both position and intensity of the dust load provides the best initial condition for forecasting of dust concentrations. [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]

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]

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), 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, are fed back into RegCM-Chem interactively, thereby representing the interactions between fine particulate matter (PM2.5), ozone (O3), and carbon dioxide (CO2). For testing purposes, we carry out a one-year simulation (2016) at a 30 km horizontal resolution over East Asia with RegCM-Chem-YIBs. The model accurately captures the spa-tio-temporal distribution of climate, chemical composition, and ecological parameters. In particular, the estimated O3 and PM2.5 are consistent with ground observations, with correlation coefficients (R) of 0.74 and 0.65, respec-tively. The simulated CO2 concentration is consistent with observations from six sites (R ranged from 0.89 to 0.97) and exhibits a similar spatial pattern when compared to 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 year-1. This study illustrates that the 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 in regional scale. [ABSTRACT FROM AUTHOR]

The cosmogenic radionuclides 7 Be and 10 Be are useful tracers for atmospheric transport studies. Combining 7 Be and 10 Be measurements with an atmospheric transport model can not only improve our understanding of the radionuclide transport and deposition processes but also provide an evaluation of the transport process in the model. To simulate these aerosol tracers, it is critical to evaluate the influence of radionuclide production uncertainties on simulations. Here we use the GEOS-Chem chemical transport model driven by the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) reanalysis to simulate 7 Be and 10 Be with the state-of-the-art production rate from the CRAC:Be (Cosmic Ray Atmospheric Cascade: Beryllium) model considering realistic spatial geomagnetic cutoff rigidities (denoted as P16spa). We also perform two sensitivity simulations: one with the default production rate in GEOS-Chem based on an empirical approach (denoted as LP67) and the other with the production rate from the CRAC:Be but considering only geomagnetic cutoff rigidities for a geocentric axial dipole (denoted as P16). The model results are comprehensively evaluated with a large number of measurements including surface air concentrations and deposition fluxes. The simulation with the P16spa production can reproduce the absolute values and temporal variability of 7 Be and 10 Be surface concentrations and deposition fluxes on annual and sub-annual scales, as well as the vertical profiles of air concentrations. The simulation with the LP67 production tends to overestimate the absolute values of 7 Be and 10 Be concentrations. The P16 simulation suggests less than 10 % differences compared to P16spa but a significant positive bias (∼18 %) in the 7 Be deposition fluxes over East Asia. We find that the deposition fluxes are more sensitive to the production in the troposphere and downward transport from the stratosphere. Independent of the production models, surface air concentrations and deposition fluxes from all simulations show similar seasonal variations, suggesting a dominant meteorological influence. The model can also reasonably simulate the stratosphere–troposphere exchange process of 7 Be and 10 Be by producing stratospheric contribution and 10Be/7Be ratio values that agree with measurements. Finally, we illustrate the importance of including the time-varying solar modulations in the production calculation, which significantly improve the agreement between model results and measurements, especially at mid-latitudes and high latitudes. Reduced uncertainties in the production rates, as demonstrated in this study, improve the utility of 7 Be and 10 Be as aerosol tracers for evaluating and testing transport and scavenging processes in global models. For future GEOS-Chem simulations of 7 Be and 10 Be, we recommend using the P16spa (versus default LP67) production rate. [ABSTRACT FROM AUTHOR]

Using the reanalysis and multiple observations, the possible impact of the Madden–Julian Oscillation (MJO) on early summer (June–July) rainfall in eastern China and its modulation by the Quasi-Biennial Oscillation (QBO) are examined. The composite results show that the suppressed (enhanced) convection anomalies for MJO phases 8–1 (4–5) are more concentrated over the maritime continent and the western Pacific during easterly QBO (EQBO). As a consequence, more significant wet (dry) anomalies develop in South (eastern) China during MJO phases 8–1 (4–5) configured with easterly (westerly) QBO. The enhancement and expansion of the anomalous tropical convection band do not necessarily correspond to enhancement of the extratropical circulation response to MJO phases 8–1 (4–5) configured with westerly (easterly) QBO. The anomalous high (low) over the maritime continent and western Pacific associated with MJO phases 8–1 (4–5) is intensified (deepened) during easterly (westerly) QBO, leading to large southwesterly (northeasterly) anomalies in South China and the coasts, carrying abundant (sparse) moisture. Two anomalous meridional circulation cells are observed for MJO phases 8–1 in the East Asia sector, with downwelling anomalies around 5–20 ∘ N, upwelling anomalies around 20–30 ∘ N, and another downwelling branch northward of 30 ∘ N, which are enhanced during easterly QBO. The anomalous meridional circulation cells are reversed for MJO phases 4–5, which are stronger during westerly QBO with the anomalous downwelling and dry anomalies covering eastern China. The combined impact of MJO phases 8–1 and easterly QBO on the early summer rainfall is noticeable in 1996, 2016, and 2020. The enormous rainfall amount appeared along the Yangtze River in 1996, 2016, and 2020 due to the extended period of MJO phases 8–1 under the background of the easterly QBO. [ABSTRACT FROM AUTHOR]

Trace metals in aerosol particles impact Earth's radiative budget, human health, and ocean biogeochemistry. Semi-continuous measurements of the elemental composition of fine-mode (PM 2.5) aerosols were conducted using an automated X-ray fluorescence analyzer on a remote island of Japan during the spring of 2018. Temporal variations in mass concentrations of geochemically important elements for this period, such as Pb, Cu, Si, Fe, and Mn, and their relationships with the emission tracers, carbon monoxide (CO) and black carbon (BC), were reported. The Integrated Massively Parallel Atmospheric Chemical Transport (IMPACT) model was used to evaluate the source apportionment of these components and was evaluated in terms of emissions and wet removal processes. Pb and Cu originated mainly from anthropogenic sources (98 % and 93 % on average, respectively) over the East Asian continent. Positive correlations of Pb and Cu with BC and CO and the similarity of their concentration-weighted trajectories indicated that the emission sources of these metals share the region where the large CO (and BC) emission sources are located and that CO can be regarded as a tracer of continental anthropogenic emissions. The air masses with minimized impacts of the wet removal during transport were extracted to elucidate the "top-down" emission ratio of Pb and Cu to CO, which were, for the first time, evaluated as 152.7 and 63.1 µg g -1 , respectively, during the spring of 2018 in the East Asian outflow. The analysis of the tagged tracer simulations by the IMPACT model confirmed that BC and Si could be used as tracers for anthropogenic and dust emissions, respectively, during the observation period. The source apportionment of Fe and Mn in PM 2.5 aerosols was conducted using Si and BC tracers, which revealed that the anthropogenic contribution was 17 % and 44 % on average, respectively. Based on the air mass origins of Fe and Mn, their anthropogenic fraction varied from 2 % to 29 % and 9 % to 68 %, respectively, during the high-PM 2.5 -concentration periods. However, despite the non-dominant anthropogenic contributions of Fe, they could adversely affect human health and ocean biogeochemistry, owing to their higher water solubility. The modeled BC, Pb, Cu, and Fe were evaluated by separately diagnosing their emission and transport. Ratios of modeled to observed concentrations for these components were analyzed in terms of the accumulated precipitation along the transport from the East Asian continent. The current model simulations were found to overestimate the emissions (based on the Community Emissions Data System, CEDS v2021-02-05) of BC by 44 % and underestimate Cu by 45 %, anthropogenic Fe by 28 % in East Asia, and the wet deposition rates for BC and Pb. Overall, Cu in East Asia exhibited a different nature from BC and Pb in terms of emission sources and wet removal. [ABSTRACT FROM AUTHOR]

The economic and environmental impacts of persistent droughts in East Asia are of growing concern, and therefore it is important to study the cyclicity and causes of these regional droughts. The self-calibrating Palmer drought severity index (scPDSI) has been extensively employed to describe the severity of regional drought, and several scPDSI reconstructions based on tree rings have been produced. We compiled a tree-ring chronology for Hailar pine (Pinus sylvestris var. mongolica) from two sites in the Hailar region in the upper Heilongjiang (Amur) River basin. Analysis of the climate response revealed that scPDSI was the primary factor limiting tree ring growth from May to July. The mean May to July scPDSI in the Hailar region since 1796 was reconstructed from the tree-ring width chronology. The results of spatial correlation analysis revealed that the reconstructed scPDSI in this region responded significantly to climate change. Analysis of the synoptic climatology indicated that the drought in the upper Heilongjiang (Amur) River basin is closely related to El Niño–Southern Oscillation (ENSO) and the Silk Road teleconnection. The results of atmospheric water cycle analysis show that water vapor transport processes are the dominant factor in the development of drought in this region. [ABSTRACT FROM AUTHOR]

Organic aerosols from marine sources over the western Pacific Ocean of East Asia were investigated by 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 μm and 10 μm (PM2.5 and PM10), black carbon (BC), organic carbon (OC), sodium, and aerosol optical depth (AOD) in the marine atmosphere. The inclusion of marine organic aerosols apparently improved model performance on OC aerosol concentration. The regional and annual mean near surface marine organic aerosol (MOA) concentration was estimated to be 0.27 μg m-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 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 (DREMOA) of -0.27 W m-2, and an indirect radiative effect (IREMOA) of -0.66 W m-2 at TOA (IREMOA) in terms of annual and oceanic average over the western Pacific, with the highest seasonal mean IREMOA up to -0.94 W m-2 in spring. IREMOA 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 anthropogenic aerosols in terms of annual mean over the western Pacific, and 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]

The atmospheric deposition of iron (Fe) promotes primary production in the surface ocean, which results in the enhanced uptake of carbon dioxide into surface seawater. Given that microorganisms in seawater utilize dissolved Fe (d-Fe) as a nutrient, the bioavailability of Fe in aerosol particles depends on its solubility. However, the factors controlling fractional Fe solubility (Fe sol %) in aerosol particles have not been fully understood. This study performed annual observations of the total and dissolved metal concentrations in size-fractionated (seven fractions) aerosol particles at Higashi-Hiroshima, Japan. The feasibility of the molar concentration ratio of d-Fe relative to dissolved Al ([d-Fe] / [d-Al]) as an indicator of sources of d-Fe in aerosol particles was investigated because this ratio is likely dependent on the emission sources of Fe (e.g., mineral dust, fly ash, and anthropogenic Fe oxides) and their dissolution processes (proton- and ligand-promoted dissolutions). Approximately 70 % of the total Fe in total suspended particulates (TSPs) was present in coarse aerosol particles, whereas about 70 % of d-Fe in TSPs was mainly found in fine aerosol particles. The average Fe sol % in fine aerosol particles (11.4 ± 7.0 %) was higher than that of coarse aerosol particles (2.19 ± 2.27 %). In addition, the average ratio of [d-Fe] / [d-Al] in coarse aerosol particles (0.408 ± 0.168) was lower than that in fine aerosol particles (1.15 ± 0.80). The range of [d-Fe] / [d-Al] ratios in the coarse aerosol particles (0.121–0.927) was similar to that obtained by proton-promoted dissolution of mineral dust (0.1–1.0), which indicates that the d-Fe in coarse aerosol particles was derived from mineral dust. The [d-Fe] / [d-Al] ratios of fine aerosol particles ranged from 0.386 to 4.67, and [d-Fe] / [d-Al] ratios greater than 1.50 cannot be explained by proton- and ligand-promoted dissolutions (1.00 < [d-Fe] / [d-Al] < 1.50). The [d-Fe] / [d-Al] ratio correlated with the enrichment factor of Fe in fine aerosol particles (r : 0.505), which indicates that anthropogenic Fe with a high [d-Fe] / [d-Al] ratio was the source of d-Fe in fine aerosol particles. The high [d-Fe] / [d-Al] ratio was attributed to anthropogenic Fe oxides emitted from high-temperature combustions. Finally, the fraction of anthropogenic Fe oxides to d-Fe in TSPs was calculated based on the [d-Fe] / [d-Al] ratio of aerosols and their emission source samples. As a result, the fraction of anthropogenic Fe oxides to d-Fe in TSPs varied from 1.48 % to 80.7 %. A high fraction was observed in summer when air masses originated from industrial regions in Japan. By contrast, approximately 10 % of d-Fe in the TSPs collected in spring and during Asian dust events was derived from anthropogenic Fe oxides when air masses were frequently transported from East Asia to the Pacific Ocean. Thus, mineral dust was the dominant source of d-Fe in Asian outflow to the Pacific Ocean. [ABSTRACT FROM AUTHOR]

Shipping contributes significantly to air pollutant emissions and atmospheric particulate matter (PM) concentrations. At the same time, worldwide maritime transport volumes are expected to continue to rise in the future. The Mediterranean Sea is a major short-sea shipping route within Europe and is the main shipping route between Europe and East Asia. As a result, it is a heavily trafficked shipping area, and air quality monitoring stations in numerous cities along the Mediterranean coast have detected high levels of air pollutants originating from shipping emissions. The current study is a part of the EU Horizon 2020 project SCIPPER (Shipping Contributions to Inland Pollution – Push for the Enforcement of Regulations), which intends to investigate how existing restrictions on shipping-related emissions to the atmosphere ensure compliance with legislation. To demonstrate the impact of ships on relatively large scales, the potential shipping impacts on various air pollutants can be simulated with chemical transport models. To determine the formation, transport, chemical transformation, and fate of particulate matter < 2.5 µ m (PM 2.5) in the Mediterranean Sea in 2015, five different regional chemical transport models (CAMx – Comprehensive Air Quality Model with Extensions, CHIMERE, CMAQ – Community Multiscale Air Quality model, EMEP – European Monitoring and Evaluation Programme model, and LOTOS-EUROS) were applied. Furthermore, PM 2.5 precursors (ammonia (NH 3), sulfur dioxide (SO 2), nitric acid (HNO 3)) and inorganic particle species (sulfate (SO 42-), ammonia (NH 4+), nitrate (NO 3-)) were studied, as they are important for explaining differences among the models. STEAM (see "List of abbreviations" in Appendix A) version 3.3.0 was used to compute shipping emissions, and the CAMS-REG version 2.2.1 dataset was used to calculate land-based emissions for an area encompassing the Mediterranean Sea at a resolution of 12 × 12 km 2 (or 0.1 ∘ × 0.1 ∘). For additional input, like meteorological fields and boundary conditions, all models utilized their regular configuration. The zero-out approach was used to quantify the potential impact of ship emissions on PM 2.5 concentrations. The model results were compared with observed background data from monitoring sites. Four of the five models underestimated the actual measured PM 2.5 concentrations. These underestimations are linked to model-specific mechanisms or underpredictions of particle precursors. The potential impact of ships on the PM 2.5 concentration is between 15 % and 25 % at the main shipping routes. Regarding particle species, SO 42- is the main contributor to the absolute ship-related PM 2.5 and to total PM 2.5 concentrations. In the ship-related PM 2.5 , a higher share of inorganic particle species can be found when compared with the total PM 2.5. The seasonal variabilities in particle species show that NO 3- is higher in winter and spring, while the NH 4+ concentrations displayed no clear seasonal pattern in any models. In most cases with high concentrations of both NH 4+ and NO 3- , lower SO 42- concentrations are simulated. Differences among the simulated particle species distributions might be traced back to the aerosol size distribution and how models distribute emissions between the coarse and fine modes (PM 2.5 and PM 10). The seasonality of wet deposition follows the seasonality of the precipitation, showing that precipitation predominates wet deposition. [ABSTRACT FROM AUTHOR]

We apply a local ensemble transform Kalman smoother (LETKS) in combination with the global aerosol–climate model ECHAM–HAM to estimate aerosol emissions from POLDER-3/PARASOL (POLarization and Directionality of the Earth's Reflectances) observations for the year 2006. We assimilate aerosol optical depth at 550 mnm (AOD550), the Ångström exponent at 550 and 865 nm (AE550–865), and single-scattering albedo at 550 nm (SSA550) in order to improve modeled aerosol mass, size and absorption simultaneously. The new global aerosol emissions increase to 1419 Tgyr-1 (+ 28 %) for dust, 1850 Tgyr-1 (+ 75 %) for sea salt, 215 Tgyr-1 (+ 143 %) for organic aerosol and 13.3 Tgyr-1 (+ 75 %) for black carbon, while the sulfur dioxide emissions increase to 198 Tgyr-1 (+ 42 %) and the total deposition of sulfates to 293 Tgyr-1 (+ 39 %). Organic and black carbon emissions are much higher than their prior values from bottom-up inventories, with a stronger increase in biomass burning sources (+ 193 % and + 90 %) than in anthropogenic sources (115 % and 70 %). The evaluation of the experiments with POLDER (assimilated) and AERONET as well as MODIS Dark Target (independent) observations shows a clear improvement compared with the ECHAM–HAM control run. Specifically based on AERONET, the global mean error in AOD550 improves from - 0.094 to - 0.006, while absorption aerosol optical depth at 550 nm (AAOD550) improves from - 0.009 to - 0.004 after the assimilation. A smaller improvement is also observed in the AE550–865 mean absolute error (from 0.428 to 0.393), with a considerably higher improvement over isolated island sites at the ocean. The new dust emissions are closer to the ensemble median of AEROCOM I, AEROCOM III and CMIP5 as well as some of the previous assimilation studies. The new sea salt emissions have become closer to the reported emissions from previous studies. Indications of a missing fraction of coarse dust and sea salt particles are discussed. The biomass burning changes (based on POLDER) can be used as alternative biomass burning scaling factors for the Global Fire Assimilation System (GFAS) inventory distinctively estimated for organic carbon (2.93) and black carbon (1.90) instead of the recommended scaling of 3.4 (Kaiser et al., 2012). The estimated emissions are highly sensitive to the relative humidity due to aerosol water uptake, especially in the case of sulfates. We found that ECHAM–HAM, like most of the global climate models (GCMs) that participated in AEROCOM and CMIP6, overestimated the relative humidity compared with ERA5 and as a result the water uptake by aerosols, assuming the kappa values are not underestimated. If we use the ERA5 relative humidity, sulfate emissions must be further increased, as modeled sulfate AOD is lowered. Specifically, over East Asia, the lower AOD can be attributed to the underestimated precipitation and the lack of simulated nitrates in the model. [ABSTRACT FROM AUTHOR]

Atmospheric ammonia (NH 3) is a reactive nitrogen compound that pollutes our environment and threatens public health. Monitoring the spatial and temporal variations is important for quantifying its emissions and depositions and evaluating the strategies for managing anthropogenic sources of NH 3. In this study, we present an NH 3 retrieval algorithm based on the optimal estimation method for the Geostationary Interferometric Infrared Sounder (GIIRS) on board China's FengYun-4B satellite (FY-4B/GIIRS). In particular, we examine the information content based on the degree of freedom for signal (DOFS) in retrieving the diurnal NH 3 in East Asia, with a focus on two source regions including the North China Plain and North India. Our retrieval is based on the FengYun Geostationary satellite Atmospheric Infrared Retrieval (FY-GeoAIR) algorithm and exploits the strong NH 3 absorption window of 955–975 cm -1. Retrieval results using FY-4B/GIIRS spectra from July to December 2022 show that the DOFS for the majority ranges from 0 to 1.0, mainly depending on the thermal contrast (TC) defined as the temperature difference between the surface and the lowest atmospheric layer. Consistent with retrievals from low-Earth-orbit (LEO) infrared sounders, the detection sensitivity, as quantified by the averaging kernel (AK) matrix, peaks in the lowest 2 km atmospheric layers. The DOFS and TC are highly correlated, resulting in a typical "butterfly" shape. That is, the DOFS increases when TC becomes either more positive or more negative. The NH 3 columns from FY-4B/GIIRS exhibit significant diurnal cycles that are consistent with the day–night gradient from the collocated IASI retrievals in the North China Plain and North India for the averages in July–August, September–October, and November–December, respectively. A collocated point-by-point intercomparison with the IASI NH 3 dataset shows generally good agreement with a small systematic difference in the summer months that may be attributed to the slight difference in a priori profiles. This study demonstrates the capability of FY-4B/GIIRS in capturing the diurnal NH 3 changes in East Asia, which will have the potential to improve regional and global air quality and climate research. [ABSTRACT FROM AUTHOR]

Nitrogen oxides (NOx=NO+NO2) emissions are estimated in three regions in the Northern Hemisphere, generally located in North America, Europe, and East Asia, by calculating the directional derivatives of NO2 column amounts observed by the TROPOspheric Monitoring Instrument (TROPOMI) with respect to the horizontal wind vectors. We present monthly averaged emissions from 1 May 2018 to 31 January 2023 to capture variations before and after the COVID-19 pandemic. We focus on a diverse collection of 54 cities, 18 in each region. A spatial resolution of 0.04 ∘ resolves intracity emission variations and reveals NOx emission hotspots at city cores, industrial areas, and sea ports. For each selected city, post-COVID-19 changes in NOx emissions are estimated by comparing monthly and annually averaged values to the pre-COVID-19 year of 2019. While emission reductions are initially found during the first outbreak of COVID-19 in early 2020 in most cities, the cities' paths diverge afterwards. We group the selected cities into four clusters according to their normalized annual NOx emissions in 2019–2022 using an unsupervised learning algorithm. All but one of the selected North American cities fall into cluster 1 characterized by weak emission reduction in 2020 (- 7 % relative to 2019) and an increase in 2022 by + 5 %. Cluster 2 contains mostly European cities and is characterized by the largest reduction in 2020 (- 31 %), whereas the selected East Asian cities generally fall into clusters 3 and 4, with the largest impacts in 2022 (- 25 % and - 37 %). This directional derivative approach has been implemented in object-oriented, open-source Python and is available publicly for high-resolution and low-latency emission estimation for different regions, atmospheric species, and satellite instruments. [ABSTRACT FROM AUTHOR]

Under future net zero emission policies, reductions in emissions of ozone (O3) precursors are expected to alter the temporal and spatial distribution of tropospheric O3. In this study, we quantify changes in the tropospheric O3 budget, spatiotemporal distribution of surface O3 in East Asia and the contributions from regional emissions, intercontinental transport and climate change between the present day and 2060 under a net zero scenario, using the NCAR Community Earth System Model (CESM) with online tagging of O3 and its precursors. The results reveal that the global tropospheric O3 burden is likely to decrease by more than 20 %, from 316 Tg in present day to 247 Tg in 2060, under a net zero scenario. The burden of stratospheric O3 in the troposphere is expected to increase from 69 to 77 Tg. The mean lifetime of tropospheric O3 increases by 2 days, ~10 %. Changes in climate under a net zero pathway are relatively small, and only lead to small increases in tropospheric O3. Over East China, surface O3 increases in winter, due to the weakened titration of O3 by NO associated with reduced anthropogenic NO emissions, and to enhanced stratospheric input. In summer, surface O3 decreases by more than 30 ppbv, and peak concentrations shift from July to May. Local contributions from anthropogenic emissions to surface O3 over East Asia are highest in summer, but drop substantially, from 30 % to 14 %, under a net zero scenario. The contribution of biogenic sources is enhanced, and forms the dominant contributor to future surface O3, especially in summer, ~40 %. This enhanced contribution is mainly due to the increased O3 production efficiency under lower anthropogenic precursor emissions. Over Eastern China, local anthropogenic contributions decrease from 50 % to 30 %. The decreases in surface O3 are strongly beneficial, and are more than sufficient to counteract the increases in surface O3 observed in China over recent years. This study thus highlights the important co-benefits of net zero policies that target climate change in addressing surface O3 pollution over East Asia. [ABSTRACT FROM AUTHOR]

As a natural aerosol with the largest emissions on land, dust has important impacts on the atmospheric environment and climate systems. Both the emissions and transport of dust aerosols are tightly connected to meteorological conditions and as a result are confronted with strong modulations by the changing climate. Here, we project the changes in the global dust emissions and loading by the end of the 21st century, using an ensemble of model outputs from the Coupled Model Intercomparison Project version 6 (CMIP6) under four Shared Socioeconomic Pathways (SSPs). Based on the validations against site-level observations, we select 9 out of 14 models and estimate an ensemble global dust emissions of 2566 ± 1996 Tga-1 (1 Tg = 10 12 g) for the present day, in which 68 % is dry deposited and 31 % is wet deposited. Compared to 2005–2014, global dust emissions show varied responses, with a reduction of - 5.6 ± 503 Tga-1 under the SSP3–7.0 scenario but increased emissions up to 60.7 ± 542 Tga-1 under the SSP5–8.5 scenario at 2090–2099. For all scenarios, the most significant increase in the dust emissions appears in North Africa (0.6 %–5.6 %) due to the combined effects of reduced precipitation but strengthened surface wind. In contrast, all scenarios show decreased emissions in the Taklimakan and Gobi deserts (- 0.8 % to - 11.9 %) because of the increased precipitation but decreased wind speed on a regional scale. The dust loading shows uniform increases over North Africa (1.6 %–13.5 %) and the downwind Atlantic, following the increased emissions but decreases over East Asia (- 1.3 % to - 10.5 %), and the downwind Pacific, partly due to enhanced local precipitation that promotes wet deposition. In total, global dust loading will increase by 2.0 %–12.5 % at the end of the 21st century under different climate scenarios, suggesting a likelihood of strengthened radiative and climatic perturbations by dust aerosols in a warmer climate. [ABSTRACT FROM AUTHOR]

The absorption Ångström exponent (AAE)-based methods are widely used to estimate brown carbon (BrC) absorption, and the estimated BrC absorption 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, it is still unclear under which conditions the AAE-based method is applicable. In this work, we used BC models partially coated with non-absorbing materials to calculate the total absorption. Since the total absorption is entirely from BC, the estimated BrC absorption should be 0 if the retrieval methods are accurate. Thus, the estimated BrC absorption (ABSBrC) should be the absorption from BC 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 at this time ABSBrC is generally in the range of -3 % to 4.5 %. However, when BC aerosols are aged, ABSBrC of about 35 % could be observed. The WDA method does not necessarily improve the estimates, sometimes a negative ABSBrC of -40 % can be 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 optical absorption aerosol depth (AAOD) estimates. The AAE = 1 method could sometimes lead to a misassigned global mean AAOD of about -0.4 – 0.5 × 10-3 if BC aerosols have a complex morphology, leading to a global mean direct radiation factor (DRF) of about -0.068 ± 0.0172 to +0.085 ± 0.0215 W/m2 from BC, which is incorrectly assigned to BrC. The WDA method does not necessarily improve the estimates. In our cases, the WDA methods based on the spherical models can lead to a range of about -0.9 – 0.05 × 10-3 of misassigned AAOD, which could lead to a global mean DRF error range of -0.153 ± 0.0387 to +0.0085 ± 0.0022 W/m2. At the regional scale, the AAE = 1 method in East Asia sometimes leads to a distributed AAOD of over 3 × 10-3, resulting in a BC DRF of about +0.51 ± 0.129 W/m2, which is incorrectly attributed to BrC. Mie theory-based WDA methods would lead to an estimated AAOD error of more than 6 × 10-3 in some regions (e.g., East Asia), resulting in an estimated misattributed DRF of +1.0 ± 0.258 W/m2. [ABSTRACT FROM AUTHOR]

In response to the need for an up-to-date emissions inventory and the recent achievement of geostationary observations afforded by the Geostationary Environment Monitoring Spectrometer (GEMS) and its sister instruments, this study aims to establish a top-down approach for adjusting aerosol precursor emissions over East Asia. This study involves a series of the TROPOspheric Monitoring Instrument (TROPOMI) NO 2 product, the GEMS aerosol optical depth (AOD) data fusion product and its proxy product, and chemical transport model (CTM)-based inverse modeling techniques. We begin by sequentially adjusting bottom-up estimates of nitrogen oxides (NOx) and primary particulate matter (PM) emissions, both of which significantly contribute to aerosol loadings over East Asia to reduce model biases in AOD simulations during the year 2019. While the model initially underestimates AOD by 50.73 % on average, the sequential emissions adjustments that led to overall increases in the amounts of NOx emissions by 122.79 % and of primary PM emissions by 76.68 % and 114.63 % (single- and multiple-instrument-derived emissions adjustments, respectively) reduce the extents of AOD underestimation to 33.84 % and 19.60 %, respectively. We consider the outperformance of the model using the emissions constrained by the data fusion product to be the result of the improvement in the quantity of available data. Taking advantage of the data fusion product, we perform sequential emissions adjustments during the spring of 2022, the period during which the substantial reductions in anthropogenic emissions took place accompanied by the COVID-19 pandemic lockdowns over highly industrialized and urbanized regions in China. While the model initially overestimates surface PM 2.5 concentrations by 47.58 % and 20.60 % in the North China Plain (NCP) region and South Korea (hereafter referred to as Korea), the sequential emissions adjustments that led to overall decreases in NOx and primary PM emissions by 7.84 % and 9.03 %, respectively, substantially reduce the extents of PM 2.5 underestimation to 19.58 % and 6.81 %, respectively. These findings indicate that the series of emissions adjustments, supported by the TROPOMI and GEMS-involved data fusion products, performed in this study are generally effective at reducing model biases in simulations of aerosol loading over East Asia; in particular, the model performance tends to improve to a greater extent on the condition that spatiotemporally more continuous and frequent observational references are used to capture variations in bottom-up estimates of emissions. In addition to reconfirming the close association between aerosol precursor emissions and AOD as well as surface PM 2.5 concentrations, the findings of this study could provide a useful basis for how to most effectively exploit multisource top-down information for capturing highly varying anthropogenic emissions. [ABSTRACT FROM AUTHOR]

To quantify CH4 emissions at policy-relevant spatial scales, the Korea Meteorological Administration (KMA) started monitoring its atmospheric levels in 1999 at Anmyeondo (AMY) and expanded monitoring to Jeju Gosan Suwolbong (JGS) and Ulleungdo (ULD) in 2012. The monitoring system consists of a cavity ring-down spectrometer (CRDS) and a new cryogenic drying method, with a measurement uncertainty (68 % c.i. (confidence interval)) of ± 0.7–0.8 ppb. To determine the regional characteristics of CH4 at each KMA station, we assessed the CH4 level relative to local background (CH4xs), analyzed local surface winds and CH4 with bivariate polar plots, and investigated CH4 diurnal cycles. We also compared the CH4 levels measured at KMA stations with those measured at the Mt. Waliguan (WLG) station in China and Ryori (RYO) station in Japan. CH4xs followed the order AMY (55.3 ± 37.7 ppb) > JGS (24.1 ± 10.2 ppb) > ULD (7.4 ± 3.9 ppb). Although CH4 was observed in well-mixed air at AMY, it was higher than at other KMA stations, indicating that it was affected not only by local sources but also by distant air masses. Annual mean CH4 was highest at AMY among all East Asian stations, while its seasonal amplitude was smaller than at JGS, which was strongly affected in the summer by local biogenic activities. From the long-term records at AMY, we confirmed that growth rate increased by 3.3 ppbyr-1 during 2006/2010 and by 8.3 ppbyr-1 from 2016 to 2020, which is similar to the global trend. Studies indicated that the recent global accelerated CH4 -growth rate was related to biogenic sources. However, δ13CH4 indicates that the CH4 trend in East Asia is derived from both biogenic and fossil fuel sources from 2006 to 2020. We confirmed that long-term high-quality data can help understand changes in CH4 emissions in East Asia. [ABSTRACT FROM AUTHOR]

The reduction of fine particles (PM 2.5) and reactive N (N r) and S (S r) species is a key objective for air pollution control policies because of their major adverse effects on human health, ecosystem diversity, and climate. The sensitivity of global and regional N r , S r , and PM 2.5 to 20 % and 40 % individual and collective reductions in anthropogenic emissions of NH 3 , NO x , and SO x (with respect to a 2015 baseline) is investigated using the EMEP MSC-W (European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West) atmospheric chemistry transport model with WRF (Weather Research and Forecasting) meteorology. Regional comparisons reveal that the individual emissions reduction has multiple co-benefits and small disbenefits on different species, and those effects are highly geographically variable. A 40 % NH 3 emission reduction decreases regional average NH 3 concentrations by 47 %–49 % but only decreases NH 4+ by 18 % in Euro_Medi, 15 % in East Asia, 12 % in North America, and 4 % in South Asia. This order follows the regional ammonia richness. A disbenefit is the increased SO 2 concentrations in these regions (10 %–16 % for 40 % reductions) because reduced NH 3 levels decrease SO 2 deposition through altering atmospheric acidity. A 40 % NO x emission reduction reduces NO x concentrations in East Asia by 45 %, Euro_Medi and North America by ∼ 38 %, and South Asia by 22 %, whilst the regional order is reversed for fine NO 3- , which is related to enhanced O 3 levels in East Asia (and also, but by less, in Euro_Medi) and decreased O 3 levels in South Asia (and also, but by less, in North America). Consequently, the oxidation of NO x to NO 3- and of SO 2 to SO 42- is enhanced in East Asia but decreased in South Asia, which causes a less effective decrease in NO 3- and even an increase in SO 42- in East Asia but quite the opposite in South Asia. For regional policy making, it is thus vital to reduce three precursors together to minimize such adverse effects. A 40 % SO x emission reduction is slightly more effective in reducing SO 2 (42 %–45 %) than SO 42- (34 %–38 %), whilst the disbenefit is that it yields a ∼ 12 % increase in total NH 3 deposition in the four regions, which further threatens ecosystem diversity. This work also highlights important messages for policy makers concerning the mitigation of PM 2.5. More emissions controls focusing on NH 3 and NO x are necessary for regions with better air quality, such as northern Europe and eastern North America. In East Asia, the three individual reductions are equally effective, whilst in South Asia only SO x reduction is currently effective. The geographically varying non-one-to-one proportionality of chemical responses of N r , S r , and PM 2.5 to emissions reductions revealed by this work show the importance of both prioritizing emissions strategies in different regions and combining several precursor reductions together to maximize the policy effectiveness. [ABSTRACT FROM AUTHOR]

Reanalysis data play a vital role in weather and climate study as well as meteorological resource development and application. In this work, the East Asia Reanalysis System (EARS) was developed using the Weather Research and Forecasting (WRF) model and the Gridpoint Statistical Interpolations (GSI) data assimilation system. The regional reanalysis system is forced by the European Centre for Medium-Range Weather Forecasts (ECMWF) global reanalysis ERA-Interim data at 6 h intervals. Hourly surface observations are assimilated by the Four-Dimension Data Assimilation (FDDA) scheme during the WRF model integration; upper observations are assimilated in three-dimensional variational data assimilation (3D-VAR) mode at the analysis moment. It should be highlighted that many of the assimilated observations have not been used in other reanalysis systems. The reanalysis runs from 1980 to 2018, producing a regional reanalysis dataset covering East Asia and surrounding areas at 12 km horizontal resolution, 74 sigma levels, and 3 h intervals. Finally, an evaluation of EARS has been performed with respect to the root mean square error (RMSE), based on the 10-year (2008–2017) observational data. Compared to the global reanalysis data of ERA-Interim, the regional reanalysis data of EARS are closer to the observations in terms of RMSE in both surface and upper-level fields. The present study provides evidence for substantial improvements seen in EARS compared to the ERA-Interim reanalysis fields over East Asia. The study also demonstrates the potential use of the EARS data for applications over East Asia and proposes further plans to provide the latest reanalysis in real-time operation mode. Simple data and updated information are available on Zenodo at 10.5281/zenodo.7404918 (Yin et al., 2022), and the full datasets are publicly accessible on the Data-as-a-Service platform of the China Meteorological Administration (CMA) at http://data.cma.cn (last access: 19 May 2023). [ABSTRACT FROM AUTHOR]

Using the reanalysis and multiple observations, the possible impact of the Madden-Julian Oscillation (MJO) on early summer rainfall in eastern China and its modulation by the Quasi-Biennial Oscillation (QBO) is examined. The composite results show that the suppressed (enhanced) convection anomalies for MJO phases 8-1 (4-5) more concentrated over maritime continent and western Pacific during EQBO (WQBO). As a consequence, more significant wet (dry) anomalies develop in South (eastern) China during MJO phases 8-1 (4-5) configured with easterly (westerly) QBO. The enhancement and expansion of the anomalous tropical convection band do not necessarily correspond to enhancement of the extratropical circulation response to MJO phases 8-1 (4-5) configured with westerly (easterly) QBO. The anomalous high (low) over the maritime continent and western Pacific associated with MJO phases 8-1 (4-5) is intensified (deepened) during easterly (westerly) QBO, leading to large southwesterly (northeasterly) anomalies in South China and coasts, carrying abundant (sparse) moisture. Two anomalous meridional circulation cells are observed for MJO phases 8-1 in the East Asia sector, with downwelling anomalies around 5–20° N, upwelling anomalies around 20–30° N, and another downwelling branch northward of 30° N, which are enhanced during easterly QBO. The anomalous meridional circulation cells are reversed for MJO phases 4-5, which are stronger during westerly QBO with the anomalous downwelling and dry anomalies covering eastern China. The combined impact of MJO phases 8-1 and easterly QBO on the early summer rainfall is noticeable in 1996 and 2020. The enormous rainfall amount appeared along the Yangtze River in 1996 and 2020 due to the extended period of the MJO phases 8-1 under the background of the easterly QBO. [ABSTRACT FROM AUTHOR]

Despite the importance of aerosol height information for events such as volcanic eruptions and long-range aerosol transport, spatial coverage of its retrieval is often limited because of a lack of appropriate instruments and algorithms. Geostationary satellite observations in particular provide constant monitoring for such events. This study assessed the application of different viewing geometries for a pair of geostationary imagers to retrieve aerosol top height (ATH) information. The stereoscopic algorithm converts a lofted aerosol layer parallax, calculated using image-matching of two visible images, to ATH. The sensitivity study provides a reliable result using a pair of Advanced Himawari Imager (AHI) and Advanced Geostationary Radiation Imager (AGRI) images at 40 ∘ longitudinal separation. The pair resolved aerosol layers above 1 km altitude over East Asia. In contrast, aerosol layers must be above 3 km for a pair of AHI and Advanced Meteorological Imager (AMI) images at 12.5 ∘ longitudinal separation to resolve their parallax. Case studies indicate that the stereoscopic ATH retrieval results are consistent with aerosol heights determined using extinction profiles from the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP). Comparisons between the stereoscopic ATH and the CALIOP 90 % extinction height, defined by extinction coefficient at 532 nm data, indicated that 88.9 % of ATH estimates from the AHI and AGRI are within 2 km of CALIOP 90 % extinction heights, with a root-mean-squared difference (RMSD) of 1.66 km. Meanwhile, 24.4 % of ATH information from the AHI and AMI was within 2 km of the CALIOP 90 % extinction height, with an RMSD of 4.98 km. The ability of the stereoscopic algorithm to monitor hourly aerosol height variations is demonstrated by comparison with a Korea Aerosol Lidar Observation Network dataset. [ABSTRACT FROM AUTHOR]

Air quality network data in China and South Korea show very high year-round mass concentrations of coarse particulate matter (PM), as inferred by the difference between PM 10 and PM 2.5. Coarse PM concentrations in 2015 averaged 52 µ g m -3 in the North China Plain (NCP) and 23 µ g m -3 in the Seoul Metropolitan Area (SMA), contributing nearly half of PM 10. Strong daily correlations between coarse PM and carbon monoxide imply a dominant source from anthropogenic fugitive dust. Coarse PM concentrations in the NCP and the SMA decreased by 21 % from 2015 to 2019 and further dropped abruptly in 2020 due to COVID-19 reductions in construction and vehicle traffic. Anthropogenic coarse PM is generally not included in air quality models but scavenges nitric acid to suppress the formation of fine particulate nitrate, a major contributor to PM 2.5 pollution. GEOS-Chem model simulation of surface and aircraft observations from the Korea–United States Air Quality (KORUS-AQ) campaign over the SMA in May–June 2016 shows that consideration of anthropogenic coarse PM largely resolves the previous model overestimate of fine particulate nitrate. The effect is smaller in the NCP which has a larger excess of ammonia. Model sensitivity simulations for 2015–2019 show that decreasing anthropogenic coarse PM directly increases PM 2.5 nitrate in summer, offsetting 80 % the effect of nitrogen oxide and ammonia emission controls, while in winter the presence of coarse PM increases the sensitivity of PM 2.5 nitrate to ammonia and sulfur dioxide emissions. Decreasing coarse PM helps to explain the lack of decrease in wintertime PM 2.5 nitrate observed in the NCP and the SMA over the 2015–2021 period despite decreases in nitrogen oxide and ammonia emissions. Continuing decrease of fugitive dust pollution means that more stringent nitrogen oxide and ammonia emission controls will be required to successfully decrease PM 2.5 nitrate. [ABSTRACT FROM AUTHOR]

Nitrogen oxides (NO x = NO + NO2) emissions are estimated in three regions in the Northern hemisphere, generally located in North America, Europe, and East Asia, by calculating the directional derivatives of NO2 column amounts observed by the TROPOMI instrument with respect to the horizontal wind vectors. We present monthly averaged emissions from 1 May 2018 to 31 January 2023 to capture variations before and after the COVID-19 pandemic. We focus on a diverse collection of 54 cities, 18 in each region. A spatial resolution of 0.04° resolves intracity emission variations and reveals NO x emission hot spots at city cores, industrial areas, and sea ports. For each selected city, COVID-19-induced changes in NO x emissions are estimated by comparing monthly and annually averaged values to the pre-COVID-19 year of 2019. While emission reductions are initially found during the first outbreak of COVID-19 in early 2020 in most cities, the cities' paths diverge afterwards. We group the selected cities into 4 clusters according to their normalized annual NO x emissions in 2019–2022 using an unsupervised learning algorithm. All but one selected North American cities fall into cluster 1 characterized by weak emission reduction in 2020 (−7 % relative to 2019) and increase in 2022 by +5 %. Cluster 2 contains mostly European cities and is characterized by the largest reduction in 2020 (−31 %), whereas the selected East Asian cities generally fall into clusters 3 and 4 with the largest impacts in 2022 (−25 % and −37 %). This directional derivative approach has been implemented in object-oriented, open-source Python and is available publicly for high-resolution and low-latency emission estimation for different regions, atmospheric species, and satellite instruments. [ABSTRACT FROM AUTHOR]

Stable water isotopes are natural tracers in the hydrological cycle and have been applied in hydrology, atmospheric science, ecology, and paleoclimatology. However, the factors controlling the isotopic distribution, both at spatial and temporal scales, are debated in low and middle latitude regions, due to the significant influence of large-scale atmospheric circulation and complex sources of water vapor. For the first time, we made in situ observations of near-surface vapor isotopes over a large region (over 10 000 km) across China in both pre-monsoon and monsoon seasons, using a newly designed vehicle-based vapor isotope monitoring system. Combined with daily and multiyear monthly mean outputs from the isotope-incorporated global spectral model (Iso-GSM) and infrared atmospheric sounding interferometer (IASI) satellite to calculate the relative contribution, we found that the observed spatial variations in both periods represent mainly seasonal mean spatial variations, but are influenced by more significant synoptic-scale variations during the monsoon period. The spatial variations of vapor δ18 O are mainly controlled by Rayleigh distillation along air mass trajectories during the pre-monsoon period, but are significantly influenced by different moisture sources, continental recycling processes, and convection during moisture transport in the monsoon period. Thus, the North–South gradient observed during the pre-monsoon period is counteracted during the monsoon period. The seasonal variation of vapor δ18 O reflects the influence of the summer monsoon convective precipitation in southern China and a dependence on temperature in the North. The spatial and seasonal variations in d-excess reflect the different moisture sources and the influence of continental recycling. Iso-GSM successfully captures the spatial distribution of vapor δ18 O during the pre-monsoon period, but the performance is weaker during the monsoon period, maybe due to the underestimation of local or short-term high-frequency synoptic variations. These results provide an overview of the spatial distribution and seasonal variability of water isotopic composition in East Asia and their controlling factors, and they emphasize the need to interpret proxy records in the context of the regional system. [ABSTRACT FROM AUTHOR]

Nitrogen oxides (NO x≡ NO + NO 2) are of central importance for air quality, climate forcing, and nitrogen deposition to ecosystems. The Geostationary Environment Monitoring Spectrometer (GEMS) is now providing hourly NO 2 satellite observations over East Asia, offering the first direct measurements of NO 2 diurnal variation from space to guide understanding of NO x emissions and chemistry. The NO 2 retrieval requires independent vertical profile information from a chemical transport model (CTM) to compute the air mass factor (AMF) that relates the NO 2 column measured along the line of sight to the NO 2 vertical column. Here, we use aircraft observations from the Korea-United States Air Quality (KORUS-AQ) campaign over the Seoul metropolitan area (SMA) and around the Korean Peninsula in May–June 2016 to better understand the factors controlling the NO 2 vertical profile, its diurnal variation, the implications for the AMFs, and the ability of the GEOS-Chem CTM to compute the NO 2 vertical profiles used for AMFs. Proper representation of oxidant chemistry is critical for the CTM simulation of NO 2 vertical profiles and is achieved in GEOS-Chem through new model developments, including aerosol nitrate photolysis, reduced uptake of hydroperoxy (HO 2) radicals by aerosols, and accounting for atmospheric oxidation of volatile chemical products (VCPs). We find that the tropospheric NO 2 columns measured from space in the SMA are mainly contributed by the planetary boundary layer (PBL) below 2 km altitude, reflecting the highly polluted conditions. Repeated measurements of NO 2 vertical profiles over the SMA at different times of day show that diurnal change in mixing depth affecting the NO 2 vertical profile induces a diurnal variation in AMFs of comparable magnitude to the diurnal variation in the NO 2 column. GEOS-Chem captures this diurnal variation in AMFs and more generally the variability in the AMFs for the KORUS-AQ NO 2 vertical profiles (2.7 % mean bias, 7.6 % precision), with some outliers in the morning due to errors in the timing of mixed-layer growth. [ABSTRACT FROM AUTHOR]

Shipping has a significant share in the emissions of air pollutants such as NO x and particulate matter (PM), and the global maritime transport volumes are projected to increase further in the future. The major route for short sea shipping within Europe and the main shipping route between Europe and East Asia are found in the Mediterranean Sea. Thus, it is a highly frequented shipping area, and high levels of air pollutants with significant potential impacts from shipping emissions are observed at monitoring stations in many cities along the Mediterranean coast. The present study is part of the EU H2020 project SCIPPER (Shipping contribution to Inland Pollution Push for the Enforcement of Regulations). Five different regional chemistry transport models (CAMx – Comprehensive Air Quality Model with Extensions, CHIMERE, CMAQ, EMEP – European Monitoring and Evaluation Programme, LOTOS-EUROS) were used to simulate the transport, chemical transformation and fate of atmospheric pollutants in the Mediterranean Sea for 2015. Shipping emissions were calculated with the Ship Traffic Emission Assessment Model (STEAM) version 3.3.0, and land-based emissions were taken from the CAMS-REG v2.2.1 dataset for a domain covering the Mediterranean Sea at a resolution of 12 km × 12 km (or 0.1∘×0.1∘). All models used their standard setup for further input. The potential impact of ships was calculated with the zero-out method. The model results were compared to each other and to measured background data at monitoring stations. The model results differ regarding the time series and pattern but are similar concerning the overall underestimation of NO 2 and overestimation of O 3. The potential impact from ships on the total NO 2 concentration was especially high on the main shipping routes and in coastal regions (25 % to 85 %). The potential impact from ships on the total O 3 concentration was lowest in regions with the highest NO 2 impact (down to -20 %). CAMx and CHIMERE simulated the highest potential impacts of ships on the NO 2 and O 3 air concentrations. Additionally, the strongest correlation was found between CAMx and CHIMERE, which can be traced back to the use of the same meteorological input data. The other models used different meteorological input due to their standard setup. The CMAQ-, EMEP- and LOTOS-EUROS-simulated values were within one range for the NO 2 and O 3 air concentrations. Regarding simulated deposition, larger differences between the models were found when compared to air concentration. These uncertainties and deviations between models are caused by deposition mechanisms, which are unique within each model. A reliable output from models simulating ships' potential impacts can be expected for air concentrations of NO 2 and O 3. [ABSTRACT FROM AUTHOR]

The national and global restrictions in response to the COVID-19 pandemic led to a sudden, albeit temporary, emission reduction of many greenhouse gases (GHGs) and anthropogenic aerosols, whose near-term climate impact were previously found to be negligible when focusing on global- and/or annual-mean scales. Our study aims to investigate the monthly scale coupled climate-and-circulation response to regional, COVID-19-related aerosol emission reductions, using the output from 10 Earth system models participating in the Covid model intercomparison project (CovidMIP). We focus on January–February and March–May 2020, which represent the seasons of largest emission changes in sulfate (SO2) and black carbon (BC). During January–February (JF), a marked decrease in aerosol emissions over eastern China, the main emission region, resulted in a lower aerosol burden, leading to an increase in surface downwelling radiation and ensuing surface warming. Regional sea-level pressure and circulation adjustments drive a precipitation increase over the Maritime Continent, embedded in a negative Pacific Decadal Oscillation (PDO)- and/or El Niño–Southern Oscillation (ENSO)-like response over the Pacific, in turn associated with a northwestward displacement and zonal shrinking of the Indo-Pacific Walker cell. Remote climate anomalies across the Northern Hemisphere, including a weakening of the Siberian High and Aleutian Low, as well as anomalous temperature patterns in the northern mid-latitudes, arise primarily as a result of stationary Rossby wave trains generated over East Asia. The anomalous climate pattern and driving dynamical mechanism reverse polarity between JF and MAM (March–May) 2020, which is shown to be consistent with an underlying shift of the dominant region of SO2 emission reduction from eastern China in JF to India in MAM. Our findings highlight the prominent role of large-scale dynamical adjustments in generating a hemispheric-wide aerosol climate imprint even on short timescales, which are largely consistent with longer-term (decadal) trends. Furthermore, our analysis shows the sensitivity of the climate response to the geographical location of the aerosol emission region, even after relatively small, but abrupt, emission changes. Scientific advances in understanding the climate impact of regional aerosol perturbations, especially the rapidly evolving emissions over China and India, are critically needed to reduce current uncertainties in near-future climate projections and to develop scientifically informed hazard mitigation and adaptation policies. [ABSTRACT FROM AUTHOR]

Atmospheric rivers (ARs) are closely associated with historical extreme precipitation events over East Asia. The projected increase in such weather systems under global warming has been extensively discussed in previous studies, while the role of stratospheric aerosol, particularly for the implementation of stratospheric aerosol intervention (SAI), in such a change remains unknown. Based on an ensemble of the UK Earth System Model (UKESM1) simulations, here we investigate changes in the frequency of ARs and their associated mean and extreme precipitation under a range of climate forcing, including greenhouse gas emission scenarios of high (SSP5–8.5) and medium (SSP2–4.5) levels, the deployment of SAI geoengineering (G6sulfur), and solar dimming (G6solar). The result indicates a significant increase in AR frequency and AR-related precipitation over most of East Asia in a warmer climate, and the most pronounced changes are observed in southern China. Comparing G6solar and both the Shared Socioeconomic Pathway (SSP) scenarios, the G6sulfur simulations indicate that SAI is effective at partly ameliorating the increases in AR activity over the subtropical region; however, it may result in more pronounced increases in ARs and associated precipitation over the upper-midlatitude regions, particularly northeastern China. Such a response is associated with the further weakening of the subtropical westerly jet stream under SAI that favours the upper-midlatitude AR activity. This is driven by the decreased meridional gradient of thermal expansion in the mid–high troposphere associated with aerosol cooling across the tropical region, though SAI effectively ameliorates the widespread increase in thermal expansion under climate warming. Such a side effect of SAI over the populated region implies that caution must be taken when considering geoengineering approaches to mitigating hydrological risk under climate change. [ABSTRACT FROM AUTHOR]

Forests disturbance by tropical cyclones is mostly documented by field studies of exceptionally strong cyclones and satellite-based approaches attributing decreases in leaf area. By starting their analysis from the observed damage, these studies are biased and may, therefore, limit our understanding of the impact of cyclones in general. This study overcomes such biases by jointly analyzing the cyclone tracks, climate reanalysis, and changes in satellite-based leaf area following the passage of 140 ± 41 cyclones. Sixty days following their passage, 18 ± 8 % of the cyclones resulted in a decrease and 48 ± 18 % showed no change in leaf area compared to nearby forest outside the storm track. For a surprising 34 ± 7 % of the cyclones, an increase in leaf area was observed. Cyclones resulting in higher leaf area in their affected compared to their reference area coincided with an atmospheric pressure dipole steering the cyclone towards a region experiencing a dry spell caused by the same dipole. When the dipole was present, the destructive power of cyclones was offset by their abundant precipitation enabling forest canopies in the affected area to recover faster from the dry spell than canopies in the reference area. This study documents previously undocumented widespread antagonist interactions on forest leaf area between tropical cyclones and droughts. [ABSTRACT FROM AUTHOR]

Concurrent floods in multiple locations pose systemic risks to the interconnected economy in East Asia via supply chain disruptions. Despite these significant economic impacts, understanding of the interconnection between rainfall patterns in the region is still currently limited. Here, we analyzed the spatial dependence of the rainfall patterns of 24 megacities in the region using complex analysis theory and discussed the technique's applicability. Each city and rainfall similarity were represented by a node and a link, respectively. Vital-node identification and clustering analysis were conducted using adjacency information entropy and multiresolution community detection. The results of vital-node identification analysis show that high-ranking nodes are cities that are located near main vapor providers in East Asia. Using multiresolution community detection, the groups were clustered to reflect the spatial characteristics of the climate. In addition, the climate links between each group were identified using cross-mutual information considering the delay time for each group. We found a strong bond between Northeast China and the southern Indochinese Peninsula and verified that the links between each group originated from the summer climate characteristics of East Asia. The results of the study show that complex network analysis could be a valuable method for analyzing the spatial relationships between climate factors. [ABSTRACT FROM AUTHOR]

With high emissions of aerosols and the known world's "Third Pole" of the Tibet Plateau (TP) in East Asia, knowledge on the energy budget over this region has been widely concerned. This study first attempts to estimate the present-day land energy balance over East Asia by combining surface and satellite observations as well as the atmospheric reanalysis and Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations. Compared to the global land budget, a substantially larger fraction of atmospheric shortwave radiation of 5.2 % is reflected, highly associated with the higher aerosol loadings and more clouds over East Asian land. While a slightly smaller fraction of atmospheric shortwave absorption of 0.6 % is unexpectedly estimated, possibly related to the lower water vapor content effects due to the thinner air over the TP to overcompensate for the aerosol and cloud effects over East Asian land. The weaker greenhouse effect and fewer low clouds due to the TP are very likely the causes of the smaller fraction of East Asian land surface downward longwave radiation. Hence, high aerosol loadings, clouds, and the TP over East Asia play vital roles in the shortwave budgets, while the TP is responsible for the longwave budgets during this regional energy budget assessment. The further obtained cloud radiative effects suggest that the presence of clouds results in a larger cooling effect on the climate system over East Asian land than that over the globe. This study provides a perspective to understand fully the roles of potential factors in influencing the different energy budget assessments over regions. [ABSTRACT FROM AUTHOR]

Millennial-scale East Asian monsoon variability is closely associated with natural hazards through long-term variability in flood and drought cycles. Therefore, exploring what drives the millennial-scale variability is of significant importance for future prediction of extreme climates. Here we present a new East Asian summer monsoon (EASM) rainfall reconstruction from the northwest Chinese Loess Plateau (CLP) spanning the past 650 kyr. The magnitude of millennial-scale variability (MMV) in EASM rainfall is linked to ice volume and greenhouse gas (GHG) at the 100 kyr eccentricity band and to GHG and summer insolation at the precession band. At the glacial–interglacial timescale, gradual changes in CO 2 during intermediate glaciations lead to increased variability in North Atlantic stratification and Atlantic meridional overturning circulation, propagating abrupt climate changes into East Asia via the westerlies. Within the 100 kyr cycle, precession variability further enhances the response, showing that stronger insolation and increased atmospheric GHG cause increases in the MMV of EASM rainfall. These findings indicate increased extreme precipitation events under future warming scenarios, consistent with model results. [ABSTRACT FROM AUTHOR]

Atmospheric rivers (ARs) are closely associated with historical extreme precipitation events over East Asia. The projected increase in such weather systems under global warming has been extensively discussed in previous studies, while the role of stratospheric aerosol, particularly for the implementation of stratospheric aerosol intervention (SAI), in such a change remains unknown. Based on an ensemble of the UK Earth System Model (UKESM1) simulations, here we investigate changes in the frequency of ARs and their associated mean and extreme precipitation under a range of climate forcing, including greenhouse gas emission scenarios of high (SSP5-8.5) and medium (SSP2-4.5) levels, the deployment of SAI geoengineering (G6sulfur) and solar dimming (G6solar). The result indicates a significant increase in AR frequency and AR-related precipitation over most of East Asia in a warmer climate and the most pronounced changes are observed in southern China. Comparing to G6solar and both the SSPs scenarios, the G6sulfur simulations indicate that SAI is effective in partly ameliorating the increases in AR activity over the subtropical region; however, it may result in more pronounced increases in ARs and associated precipitation over the mid-high latitude regions, particularly northeastern China and Japan. Such a response is associated with the further weakening of the mid-latitude westerly jet stream under SAI that favours the high-latitude AR activity. This is driven by the decreased meridional gradient of thermal expansion in the mid-high troposphere associated with aerosol cooling across the tropical region, though SAI effectively ameliorates the widespread increase in thermal expansion under climate warming. Such a side effect of SAI over the populated region implies that caution must be taken when considering geoengineering approaches to mitigating hydrological risk under climate change. [ABSTRACT FROM AUTHOR]