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Understanding carbon sources and sinks across the Earth's surface is fundamental in climate science and policy; thus, these topics have been extensively studied but have yet to be fully resolved and are associated with massive debate regarding the sign and magnitude of the carbon budget from global to regional scales. Developing new models and estimates based on state-of-the-art algorithms and data constraints can provide valuable knowledge and contribute to a final ensemble model in which various optimal carbon budget estimates are integrated, such as the annual global carbon budget paper. Here, we develop a new atmospheric inversion system based on the 4D local ensemble transform Kalman filter (4D-LETKF) coupled with the GEOS-Chem global transport model to infer surface-to-atmosphere net carbon fluxes from Orbiting Carbon Observatory-2 (OCO-2) V10r XCO 2 retrievals. The 4D-LETKF algorithm is adapted to an OCO-2-based global carbon inversion system for the first time in this work. On average, the mean annual terrestrial and oceanic fluxes between 2015 and 2020 are estimated as - 2.02 and - 2.34 GtC yr -1 , respectively, compensating for 21 % and 24 %, respectively, of global fossil carbon dioxide (CO 2) emissions (9.80 GtC yr -1). Our inversion results agree with the CO 2 atmospheric growth rates reported by the National Oceanic and Atmospheric Administration (NOAA) and reduce the modeled CO 2 concentration biases relative to the prior fluxes against surface and aircraft measurements. Our inversion-based carbon fluxes are broadly consistent with those provided by other global atmospheric inversion models, although discrepancies still occur in the land–ocean flux partitioning schemes and seasonal flux amplitudes over boreal and tropical regions, possibly due to the sparse observational constraints of the OCO-2 satellite and the divergent prior fluxes used in different inversion models. Four sensitivity experiments are performed herein to vary the prior fluxes and uncertainties in our inversion system, suggesting that regions that lack OCO-2 coverage are sensitive to the priors, especially over the tropics and high latitudes. In the further development of our inversion system, we will optimize the data-assimilation configuration to fully utilize current observations and increase the spatial and seasonal representativeness of the prior fluxes over regions that lack observations. [ABSTRACT FROM AUTHOR]

The cloud radiative kernel method is a popular approach to quantify cloud feedbacks and rapid cloud adjustments to increased CO2 concentrations and to partition contributions from changes in cloud amount, altitude, and optical depth. However, because this method relies on cloud property histograms derived from passive satellite sensors or produced by passive satellite simulators in models, changes in obscuration of lower-level clouds by upper-level clouds can cause apparent low-cloud feedbacks and adjustments, even in the absence of changes in lower-level cloud properties. Here, we provide a methodology for properly diagnosing the impact of changing obscuration on cloud feedbacks and adjustments and quantify these effects across climate models. Averaged globally and across global climate models, properly accounting for obscuration leads to weaker positive feedbacks from lower-level clouds and stronger positive feedbacks from upper-level clouds while simultaneously removing a mostly artificial anti-correlation between them. Given that the methodology for diagnosing cloud feedbacks and adjustments using cloud radiative kernels has evolved over several papers, and obscuration effects have only occasionally been considered in recent papers, this paper serves to establish recommended best practices and to provide a corresponding code base for community use. [ABSTRACT FROM AUTHOR]

This paper describes the methods that are used in the SAPRC mechanism generation system, MechGen, to estimate rate constants and derive mechanisms for gas-phase reactions of volatile organic compounds (VOCs) in the lower atmosphere. Versions of this system have been used for over 20 years in the development of the SAPRC mechanisms for air quality models, but this is the first complete documentation of the scientific basis for the chemical mechanisms it derives. MechGen can be used to derive explicit gas-phase mechanisms for most compounds with C, H, O, or N atoms. Included are reactions of organic compounds with hydroxy (OH) and nitrate (NO3) radicals, O3, and O3P; photolysis or unimolecular reactions; and the reactions of the radicals they form in the presence of O2 and oxides of nitrogen (NOx) at lower-atmospheric temperatures and pressures. Measured or theoretically calculated rate constants and branching ratios are used when data are available, but in most cases rate constants and branching ratios are estimated using various structure–reactivity or other estimation methods. Types of reactions include initial reactions of organics with atmospheric oxidants or by photolysis; unimolecular and bimolecular reactions of carbon-centered, alkoxy, and peroxy radicals; and those of Criegee and other intermediates that are formed. This paper documents the methods, assignments, and estimates currently used to derive these reactions and provides examples of MechGen predictions. Many of the estimation methods discussed here have not been published previously, and others have not been used previously in developing comprehensive mechanisms. Our knowledge of atmospheric reactions of organic compounds rapidly and continuously evolves, and therefore mechanism generation systems such as MechGen also need to evolve to continue to represent the current state of the science. This paper points out areas where MechGen may need to be modified when the system is next updated. This paper concludes with a summary of the major areas of uncertainty where further experimental, theoretical, or mechanism development research is most needed to improve predictions of atmospheric reaction mechanisms of volatile organic compounds. [ABSTRACT FROM AUTHOR]

Long-term experimental stratospheric NO 2 and NO partial columns measured by means of solar Fourier-transform infrared (FTIR) spectrometry at Zugspitze (47.42° N, 10.98° E; 2964 m a.s.l.), Germany, were used to create a set of experiment-based monthly scaling factors (SF exp). The underlying data set is published in a companion paper (Nürnberg et al., 2024) and comprises over 25 years of measurements depicting the daytime variability of stratospheric NO 2 and NO partial columns with respect to local solar time (LST). In accordance with simulation-based scaling factors recently published by Strode et al. (2022), we created SF exp normalized to SZA =72° for NO 2 and NO for every month of the year as a function of solar zenith angle (SZA). Apart from a boundary value problem at minimum SZA values originating from averaging over different times of the month, the obtained scaling factors SF exp (NO 2) and SF exp (NO) as a function of SZA represent the daytime behavior already shown in model simulations and experiments in the literature very well. This shows a well-pronounced increase in the NO 2 and NO stratospheric partial column with the time of the day and a flattening of this increase after noon. In addition to the discussion of SF exp , we validate the simulation-based scaling factors SF sim (NO 2) (Strode et al., 2022) and present simulation-based scaling factors for NO SF sim (NO). The simulation-based scaling factors show excellent agreement with the experiment-based ones; i.e., for NO 2 and NO the mean value of the modulus between the experiment and simulation over all SZAs and months is only 0.02 %. We show that recently used model simulations can describe the real behavior of nitrogen oxide (NO x) variability in the stratosphere very well. Furthermore, we conclude that ground-based FTIR measurements can be used for validation of the output of photochemistry models and for creating experiment-based data sets describing the daytime stratospheric NO x variability as a function of SZA. This is a contribution to improved satellite validation and a better understanding of stratospheric photochemistry. [ABSTRACT FROM AUTHOR]

Open burning of household solid waste is a large source of air pollutants worldwide, especially in the Global South. However, waste burning emissions are either missing or have large uncertainties in local, regional, or global emission inventories due to limited emission factor (EF) and activity data. Detailed particulate matter (PM) chemical speciation data are even less available. This paper reports source profiles and EFs for PM 2.5 species as well as acidic and alkali gases measured from laboratory combustion of 10 waste categories that represent open burning in South Africa. Carbonaceous materials contributed more than 70 % of PM 2.5 mass. Elemental carbon (EC) was most abundant from flaming materials (e.g., plastic bags, textiles, and combined materials), and its climate forcing exceeded the corresponding CO 2 emissions by a factor of 2–5. Chlorine had the highest EFs among elements measured by X-ray fluorescence (XRF) for all materials. Vegetation emissions showed high abundances of potassium, consistent with its use as a marker for biomass burning. Fresh PM 2.5 emitted from waste burning appeared to be acidic. Moist vegetation and food discards had the highest hydrogen fluoride (HF) and PM fluoride EFs due to fluorine accumulation in plants, while burning rubber had the highest hydrogen chloride (HCl) and PM chloride EFs due to high chlorine content in the rubber. Plastic bottles, plastic bags, rubber, and food discards had the highest EFs for polycyclic aromatic hydrocarbons (PAHs) and nitro-PAHs as well as their associated toxicities. Distinct differences between odd and even carbon preferences were found for alkanes from biological and petroleum-based materials: dry vegetation, paper, textiles, and food discards show preference for the odd-numbered alkanes, while the opposite is true for plastic bottles, plastic bags, and rubber. As phthalates are used as plasticizers, their highest EFs were found for plastic bottles and bags, rubber, and combined materials. Data from this study will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment. [ABSTRACT FROM AUTHOR]

A 30-year (1980–2010) climatology of the major variables and terms of the transformed Eulerian-mean (TEM) momentum and thermodynamic equations is constructed by using four global atmospheric reanalyses: the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2); the Japanese 55-year Reanalysis (JRA-55); the European Centre for Medium-Range Weather Forecasts (ECMWF) interim reanalysis (ERA-Interim); and the Climate Forecast System Reanalysis (CFSR). Both the reanalysis ensemble mean (REM) and the differences in each reanalysis from the REM are investigated in the latitude–pressure domain for December–January–February and for June–July–August. For the REM investigation, two residual vertical velocities (the original one and one evaluated from residual meridional velocity) and two mass streamfunctions (from meridional and vertical velocities) are compared. Longwave (LW) radiative heating and shortwave (SW) radiative heating are also shown and discussed. For the TEM equations, the residual terms are also calculated and investigated for their potential usefulness, as the residual term for the momentum equation should include the effects of parameterized processes such as gravity waves, while that for the thermodynamic equation should indicate the analysis increment. Inter-reanalysis differences are investigated for the mass streamfunction, LW and SW heating, the two major terms of the TEM momentum equation (the Coriolis term and the Eliassen–Palm flux divergence term), and the two major terms of the TEM thermodynamic equation (the vertical temperature advection term and the total diabatic heating term). The spread among reanalysis TEM momentum balance terms is around 10 % in Northern Hemisphere winter and up to 50 % in Southern Hemisphere winter. The largest uncertainties in the thermodynamic equation (about 50 %) are found in the vertical advection, for which the structure is inconsistent with the differences in heating. The results shown in this paper provide basic information on the degree of agreement among recent reanalyses in the stratosphere and upper troposphere in the TEM framework. [ABSTRACT FROM AUTHOR]

Nitrogen oxides (NOx = NO + NO2) are air pollutants which are co-emitted with CO2 during high-temperature combustion processes. Monitoring NOx emissions is crucial for assessing air quality and for providing proxy estimates of CO2 emissions. Satellite observations, such as those from the TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel-5P satellite, provide global coverage at high temporal resolution. However, satellites measure only NO2 , necessitating a conversion to NOx. Previous studies have applied a constant NO2 -to- NOx conversion factor. In this paper, we develop a more realistic model for NO2 -to- NOx conversion and apply it to TROPOMI data of 2020 and 2021. To achieve this, we analysed plume-resolving simulations from the MicroHH large-eddy simulation model with chemistry for the Bełchatów (PL), Jänschwalde (DE), Matimba (ZA) and Medupi (ZA) power plants, as well as a metallurgical plant in Lipetsk (RU). We used the cross-sectional flux method to calculate NO , NO2 and NOx line densities from simulated NO and NO2 columns and derived NO2 -to- NOx conversion factors as a function of the time since emission. Since the method of converting NO2 to NOx presented in this paper assumes steady-state conditions and that the conversion factors can be modelled by a negative exponential function, we validated the conversion factors using the same MicroHH data. Finally, we applied the derived conversion factors to TROPOMI NO2 observations of the same sources. The validation of the NO2 -to- NOx conversion factors shows that they can account for the NOx chemistry in plumes, in particular for the conversion between NO and NO2 near the source and for the chemical loss of NOx further downstream. When applying these time-since-emission-dependent conversion factors, biases in NOx emissions estimated from TROPOMI NO2 images are greatly reduced from between - 50 % and - 42 % to between only - 9.5 % and - 0.5 % in comparison with reported emissions. Single-overpass estimates can be quantified with an uncertainty of 20 %–27 %, while annual NOx emission estimates have uncertainties in the range of 4 %–21 % but are highly dependent on the number of successful retrievals. Although more simulations covering a wider range of meteorological and trace gas background conditions will be needed to generalise the approach, this study marks an important step towards a consistent, uniform, high-resolution and near-real-time estimation of NOx emissions – especially with regard to upcoming NO2 -monitoring satellites such as Sentinel-4, Sentinel-5 and CO2M. [ABSTRACT FROM AUTHOR]

The rapid development of the economy and the implementation of environmental policies adapted in India have led to fast changes of regional SO2 emissions. We present a monthly SO2 emission inventory for India covering December 2018 to November 2023 based on the Tropospheric Monitoring Instrument (TROPOMI) Level-2 COBRA SO2 dataset, using an improved flux-divergence method and estimated local SO2 lifetime, which includes both its chemical loss and dry deposition. We update the methodology to use the daily CAMS model output estimates of the hydroxyl-radical distribution as well as the measured dry deposition velocity to account for the variability in the tropospheric SO2 lifetime. It is the first effort to derive the local SO2 lifetime for application in the divergence method. The results show the application of the local SO2 lifetime improves the accuracy of SO2 emissions estimation when compared to calculations using a constant lifetime. Our improved flux-divergence method reduced the spreading of the point-source emissions compared to the standard flux-divergence method. Our derived averaged SO2 emissions covering the recent 5 years are about 5.2 Tg yr−1 with a monthly mean uncertainty of 40 %, which is lower than the bottom-up emissions of 11.0 Tg yr−1 from CAMS-GLOB-ANT v5.3. The total emissions from the 92 largest point-source emissions are estimated to be 2.9 Tg yr−1, lower than the estimation of 5.2 Tg yr−1 from the global SO2 catalog MSAQSO2LV4. We claim that the variability in the SO2 lifetime is important to account for in estimating top-down SO2 emissions. [ABSTRACT FROM AUTHOR]

Global chemistry–climate models (CCMs) play an important role in assessing the climate and air pollution implications of aerosols and chemically reactive gases. Evaluating these models under past conditions and constraining historical sources and sinks necessitate reliable records of atmospheric mixing ratios spanning preindustrial times. Such precious records were recently obtained for carbon monoxide (CO), documenting for the first time the evolution of this reactive compound over the industrial era. In this study, we compare the simulated atmospheric surface CO mixing ratios ([CO]) from two different sets of chemistry–climate models and emissions within the frameworks of CMIP5 and of CMIP6 (Coupled Model Intercomparison Project Phases 5 and 6) to recent bipolar ice archive reconstructions for the period spanning 1850 to the present. We analyse how historical (1850–2014) [CO] outputs from 16 ACCMIP (Atmospheric Chemistry and Climate Model Intercomparison Project) models and 7 AerChemMIP (Aerosol Chemistry Model Intercomparison Project) models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. While most models underestimate [CO] at northern high latitudes, a reduction in this bias is observed between the ACCMIP and the AerChemMIP exercise. Over the 1980–2010 CE period (common era; all subsequent years in the paper are reported in CE), trends in ice archive and firn air observations and AerChemMIP outputs align remarkably well at northern and southern high latitudes, indicating improved quantification of anthropogenic CO emissions and the main CO sink (OH oxidation) compared to ACCMIP. From 1850 to 1980, AerChemMIP models and observations consistently show increasing [CO] in both the Northern Hemisphere (NH) and Southern Hemisphere (SH), suggesting a robust understanding of the CO budget evolution. However, a divergence in the [CO] growth rate emerges in the NH between models and observations over the 1920–1980 period, attributed to uncertainties in CO emission factors (EFs), particularly EFs for the RCO (residential, commercial, and other) and transportation sectors, although we cannot totally rule out the possibility that the CO record based on the Greenland ice archives may be biased high by CO chemical production processes occurring in the ice prior to the measurements (i.e. in situ CO production). In the Southern Hemisphere, AerChemMIP models simulate an increase in atmospheric [CO] from 1850 to 1980 that closely reproduces the observations (22 ± 10 ppb and 13 ± 7 ppb, respectively). Such agreement supports CMIP6 biomass burning CO emission inventories, which do not reveal a peak in CO emissions in the late 19th century. Furthermore, both SH models and observations reveal an accelerated growth rate in [CO] during 1945–1980 relative to 1850–1945, likely linked to increased anthropogenic transportation emissions. [ABSTRACT FROM AUTHOR]

Independent estimation and verification of fossil CO2 emissions on a regional and national scale are crucial for evaluating the fossil CO2 emissions and reductions reported by countries as part of their nationally determined contributions (NDCs). Top-down methods, such as the assimilation of in situ and satellite observations of different tracers (e.g., CO2 , CO , Δ14CO2 , XCO2), have been increasingly used for this purpose. In this paper, we use the Lund University Modular Inversion Algorithm (LUMIA) to estimate fossil CO2 emissions and natural fluxes by simultaneously inverting in situ synthetic observations of CO2 and Δ14CO2 over Europe. We evaluate the inversion system by conducting a series of observing system simulation experiments (OSSEs). We find that in regions with a dense sampling network, such as western/central Europe, adding Δ14CO2 observations in an experiment where the prior fossil CO2 and biosphere fluxes are set to zero allows LUMIA to recover the time series of both categories. This reduces the prior-to-truth root mean square error (RMSE) from 1.26 to 0.12 TgC d−1 in fossil CO2 and from 0.97 to 0.17 TgC d−1 in biosphere fluxes, reflecting the true total CO2 budget by 91 %. In a second set of experiments using realistic prior fluxes, we find that in addition to retrieving the time series of the optimized fluxes, we are able to recover the true regional fossil CO2 budget in western/central Europe by 95 % and in Germany by 97 %. In all experiments, regions with low sampling coverage, such as southern Europe and the British Isles, show poorly resolved posterior fossil CO2 emissions. Although the posterior biosphere fluxes in these regions follow the seasonal patterns of the true fluxes, a significant bias remains, making it impossible to close the total CO2 budget. We find that the prior uncertainty of fossil CO2 emissions does not significantly impact the posterior estimates, showing similar results in regions with good sampling coverage like western/central Europe and northern Europe. Finally, having a good prior estimate of the terrestrial isotopic disequilibrium is important to avoid introducing additional noise into the posterior fossil CO2 fluxes. [ABSTRACT FROM AUTHOR]

General circulation models (GCMs), unlike other lines of evidence, indicate that anthropogenic aerosols cause a global-mean increase in cloud liquid water path (L) and thus a negative adjustment to radiative forcing of the climate by aerosol–cloud interactions. In part 1 of this series of papers, we showed that this is true even in models that reproduce the negative correlation observed in present-day internal variability in L and cloud droplet number concentration (Nd). We studied several possible confounding mechanisms that could explain the noncausal cloud–aerosol correlations in GCMs and that possibly contaminate observational estimates of radiative adjustments. Here, we perform single-column and full-atmosphere GCM experiments to investigate the causal model-physics mechanisms underlying the model radiative adjustment estimate. We find that both aerosol–cloud interaction mechanisms thought to be operating in real clouds – precipitation suppression and entrainment evaporation enhancement – are active in GCMs and behave qualitatively in agreement with physical process understanding. However, the modeled entrainment enhancement has a negligible global-mean effect. This raises the question of whether the GCM estimate is incorrect due to parametric or base-state representation errors or whether the process understanding gleaned from a limited set of canonical cloud cases is insufficiently representative of the diversity of clouds in the real climate. Regardless, even at limited resolution, the GCM physics appears able to parameterize the small-scale microphysics–turbulence interplay responsible for the entrainment enhancement mechanism. We suggest ways to resolve tension between current and future (storm-resolving) global modeling systems and other lines of evidence in synthesis climate projections. [ABSTRACT FROM AUTHOR]

The paper evaluates the long-term (2007–2016) impact of biogenic volatile organic compound (BVOC) emissions on urban ozone patterns over central Europe, specifically focusing on the contribution of urban vegetation using a regional climate model coupled offline to a chemistry transport model. BVOCs are emitted by terrestrial ecosystems, and their impact is considered especially important over NOx-rich environments such as urban areas. The study evaluates the impact of BVOC emissions on ozone (O3), formaldehyde (HCHO), and hydroxyl radical (OH) near-surface concentrations, showing an increase in summer ozone by 6 %–10 % over large areas in central Europe due to their emissions. It also demonstrates a substantial increase in formaldehyde concentrations. Additionally, the impact of BVOC emissions on hydroxyl radical concentrations shows a decrease over most of the modeled region by 20 %–60 %, with some increases over urban areas. Impacts on peroxy radicals (HO2 and higher RO2) are shown too. Importantly, the study explores the partial role of urban vegetation in modulating ozone and evaluates its contribution to the overall ozone formation due to all BVOC emissions. The findings reveal that urban BVOC emissions contribute to around 10 % of the total impact on ozone and formaldehyde concentrations in urban areas, indicating their significant but localized influence. The study also conducts sensitivity analyses to assess the uncertainty arising from the calculation of the urban fraction of BVOC emissions. The results show that the impact of urban BVOC emissions responds to their magnitude nearly linearly, with variations up to 4-fold, emphasizing the importance of accurately quantifying the urban BVOC fluxes. Overall, the study sheds light on the intricate relationship between urban vegetation, BVOC emissions, and their impact on atmospheric chemistry, providing valuable insights into the regional chemistry of BVOC emissions over central Europe and the causes of urban ozone pollution. [ABSTRACT FROM AUTHOR]

Nitrous acid (HONO) is a main precursor of hydroxyl radicals (OH), which contribute to the formation of numerous secondary air pollutants in the troposphere. Despite its importance in atmospheric chemistry, HONO chemistry has not been fully incorporated into many chemical transport models (CTMs). Due to the lack of atmospheric HONO processes, CTM simulations often tend to underestimate atmospheric mixing ratios of HONO. This study was undertaken because simulations with the current Community Multiscale Air Quality (CMAQ) model have a strong tendency to underestimate the HONO mixing ratio. In search of missing sources of atmospheric HONO, we attempted to sequentially incorporate the following potential HONO sources and processes into the CMAQ modeling framework: (i) gas-phase HONO reactions, (ii) traffic HONO emissions, (iii) soil HONO emissions, (iv) heterogeneous HONO production on the surfaces of aerosols, (v) heterogeneous HONO formation on tree leaf and building surfaces, and (vi) photolysis reactions of particulates and deposited HNO3 /nitrates called "renoxification". The simulation performances of the modified CMAQ models were then evaluated by comparing the modeled HONO mixing ratios with the HONO mixing ratios observed at the Olympic Park station in Seoul, South Korea. When HONO processes were fully added to the CMAQ model, average daily HONO mixing ratios increased from 0.06 to 1.18 ppb. The daytime HONO mixing ratios produced from the CMAQ model run with a full account of atmospheric HONO processes were found to be in better agreement with observations than those from the original CMAQ model (CMAQv5.2.1) runs with improved statistical metrics (e.g., the index of agreement (IOA) increased from 0.59 to 0.68, while the mean bias (MB) decreased dramatically from -0.57 to -0.34 ppb). In addition, we investigated the contributions of individual atmospheric HONO processes to HONO mixing ratios, as well as the impacts of HONO atmospheric processes on the concentrations of other atmospheric species in South Korea. All these issues are also discussed in this paper. [ABSTRACT FROM AUTHOR]

Mineral dust significantly influences the Earth's climate system by affecting the radiative balance through the emission, absorption and scattering of solar and terrestrial radiation. Estimating the dust radiative effect remains challenging due to the lack of detailed information on the physical and chemical properties of dust. High-spectral-resolution instruments in the infrared (IR) spectrum, such as the Infrared Atmospheric Sounding Instrument (IASI), have demonstrated the ability to quantify these aerosol properties. A crucial parameter for characterizing mineral dust from space is the complex refractive index (CRI), as it links the dust's physical and chemical properties to its optical properties. This paper examines the impact of six prior laboratory CRI datasets to improve the characterization of dust microphysical properties using IASI. The CRIs include older measurements obtained through the classical pellet method, commonly employed in mineral dust applications, as well as newer datasets that incorporate the latest advancements in laboratory measurement techniques for aerosol generation. These datasets are tested on IASI measurements during a dust storm event over the Gobi Desert in May 2017. We evaluate the sensitivity of IASI to different CRI datasets using the Atmospheric Radiation Algorithm for High-Spectral Resolution Measurements from Infrared Spectrometer (ARAHMIS) radiative transfer algorithm and explore the datasets' impact on retrieving size distribution parameters by mapping their spatial distributions. The results indicate that the laboratory CRI datasets decrease the total error in the covariance matrix by 30 %. In addition, we assess the ability to accurately reconstruct IASI detections and the extent to which we can retrieve the microphysical properties of dust particles. The choice of CRI significantly impacts the accuracy of dust detection and characterization from satellite observations. Notably, datasets that incorporate recent aerosol generation techniques with higher spectral resolution and samples from the case study region show improved compatibility with IASI observations. The outcomes of this research emphasize two key points: the crucial link between chemical composition of dust and its optical properties and the importance of considering the specific composition of the CRI dataset for improved retrieval of the microphysical parameters. Furthermore, this study highlights the critical role of ongoing enhancements in CRI measurement approaches, as well as the potential of high-spectral-resolution infrared sounders for aerosol atmospheric investigation and for understanding the radiative impacts of sounders. [ABSTRACT FROM AUTHOR]

In this study, we utilized a high-resolution (4 km) convection-permitting Weather Research and Forecasting (WRF) simulation spanning a 13-year period (2000–2013) to investigate the climatological features of low-level jets (LLJs) over North America. The 4 km simulation enabled us to represent the effects of orography and the underlying surface on the boundary layer winds better. Focusing on the continental US and the adjacent border regions of Canada and Mexico, this study not only identified several well-known large-scale LLJs, such as the southerly Great Plains LLJ and the summer northerly California coastal LLJ, but also the winter Quebec northerly LLJ which received less focus before. All these LLJs reach their peak in the nighttime in the diurnal cycle. Thus, the different thermal and dynamic mechanisms forming these three significant LLJs are investigated in this paper. Inertial oscillation theory dominates in the Great Plain LLJ, and the California coastal LLJ is formed by the baroclinic theory, whereas the Quebec LLJ is associated with both theories. Moreover, the high-resolution simulation revealed climatic characteristics of weaker and smaller-scale LLJs or low-level wind maxima in regions with complex terrains, such as the northerly LLJs in the foothill regions of the Rocky Mountains and the Appalachians during the winter. This study provides valuable insights into the climatological features of LLJs in North America, and the high-resolution simulation offers a more detailed understanding of LLJ behavior near complex terrains and other smaller-scale features. [ABSTRACT FROM AUTHOR]

​​​​​​​At the altitudes of the mesosphere–lower thermosphere, OH and HO 2 play a significant role in many physicochemical processes. Thus, monitoring their spatiotemporal evolution, together with other chemically active trace gases, is one of the most important problems for this atmosphere region, in which direct measurements are difficult. This paper studies the nighttime OH and HO 2 chemical equilibria using the 3D chemical transport modeling within the general approach, which includes the identification of the main sources and sinks in the equilibrium space–time areas and the derivation of analytical criteria for equilibrium validity. The presented analysis shows that there are extended areas where nighttime HO 2 and OH are close to their local equilibrium concentrations, determined mainly by the reaction between HOx and Ox components among themselves and with H 2 O 2 , N, NO, NO 2 , and CO. In the upper mesosphere–lower thermosphere, the equilibrium expressions can be shortened so that they include the HOx – Ox chemistry only. These expressions describe the HO 2 and OH equilibria from the top down to some boundaries, the altitude positions of which vary in the interval between 72–73 and 85 km and depend essentially on season and latitude. The developed analytical criteria reproduce the main features of these boundaries well almost everywhere. Due to weak sensitivity to uncertainties of reaction rates and other parameters, the criteria can be regarded as a robust instrument for HO 2 and OH equilibrium validation. The obtained results allow us to extend previously proposed methods for the retrieval of poorly measured components from measurement data and to develop new approaches. [ABSTRACT FROM AUTHOR]

Knowledge of the chemical composition and mixing state of aerosols at a single-particle level is critical for gaining insights into atmospheric processes. One common tool to make these measurements is single-particle mass spectrometry. There remains a need to compare the performance of different single-particle mass spectrometers (SPMSs). An intercomparison of SPMSs was conducted at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber at the Karlsruhe Institute of Technology (KIT) in November 2014, as part of the first phase of the Fifth International Workshop on Ice Nucleation (FIN-01). In this paper we compare size distributions and mass spectra of atmospherically relevant particle types measured by five SPMSs. These include different minerals, desert and soil dusts, soot, bioaerosol (Snomax; protein granule), secondary organic aerosol (SOA), and SOA-coated mineral particles. Most SPMSs reported similar vacuum aerodynamic diameter (dva) within typical instrumental ranges from ∼100 –200 nm (lower limit) to ∼2 –3 µm (upper limit). In general, all SPMSs exhibited a wide dynamic range (up to ∼103) and high signal-to-noise ratio (up to ∼104) in mass spectra. Common spectral features with small diversities in mass spectra were found with high average Pearson's correlation coefficients, i.e., for average positive spectra ravg-pos=0.74 ± 0.12 and average negative spectra ravg-neg=0.67 ± 0.22. We found that instrument-specific detection efficiency (DE) was more dependent on particle size than particle type, and particle identification favored the use of bipolar, rather than monopolar, instruments. Particle classification from "blind experiments" showed that all instruments differentiated SOA, soot, and soil dust and detected subtle changes in the particle internal mixing but had difficulties differentiating among specific mineral types and dusts. This study helps to further understand the capabilities and limitations of the single-particle mass spectrometry technique in general and the specific performance of the instrument in characterizing atmospheric aerosol particles. [ABSTRACT FROM AUTHOR]

Aerosol distributions are of great relevance for air quality, especially for cities like Stuttgart, which has limited air exchange due to its location in a basin. We collected a comprehensive set of data from remote sensing and in situ methods including radiosondes for the urban background of downtown Stuttgart to determine the impact of boundary layer mixing processes on local air quality and to evaluate the simulation results of the high-resolution large eddy simulation (LES) model PALM-4U at 10 m grid spacing. Stagnant meteorological conditions caused accumulation of aerosols, and chemical composition analysis shows that ammonium nitrate (37 ± 9 %) and organic aerosol (OA; 34 ± 9 %) dominated during this winter study. Case studies show that clouds during previous nights can weaken temperature inversion and accelerate boundary layer mixing after sunrise by up to 3 h. This is important for ground-level aerosol dilution during the morning rush hour. Furthermore, our observations validate results of the LES model PALM-4U in terms of boundary layer heights and aerosol mixing for 48 h. The simulated aerosol concentrations follow the trend of our observations but are still underestimated by a factor of 4.5 ± 2.1 due to missing secondary aerosol formation processes and uncertainties of emissions and boundary conditions in the model. This paper firstly evaluates the PALM-4U model performance in simulating aerosol spatio-temporal distributions, which can help to improve the LES model and to better understand sources and sinks for air pollution as well as the role of horizontal and vertical transport. [ABSTRACT FROM AUTHOR]

The ozone layer is often noted to exhibit self-healing, whereby depletion of ozone aloft induces ozone increases below, explained as resulting from enhanced ozone production due to the associated increase in ultraviolet (UV) radiation below. Similarly, ozone enhancement aloft can reduce ozone below (reverse self-healing). This paper considers self-healing and reverse self-healing to manifest a general mechanism we call photochemical adjustment, whereby ozone perturbations lead to a downward cascade of anomalies in UV and ozone. Conventional explanations for self-healing imply that photochemical adjustment is stabilizing, damping perturbations towards the surface. However, photochemical adjustment can be destabilizing if the enhanced UV disproportionately increases the ozone sink, as can occur if the enhanced UV photolyzes ozone to produce atomic oxygen, which speeds up catalytic destruction of ozone. We analyze photochemical adjustment in two linear ozone models (Cariolle v2.9 and LINOZ), finding that (1) photochemical adjustment is destabilizing above 40 km in the tropical stratosphere and (2) self-healing often represents only a small fraction of the total photochemical stabilization. The destabilizing regime above 40 km is reproduced in a much simpler model: the Chapman cycle augmented with destruction of O and O 3 by generalized catalytic cycles and transport (the Chapman+2 model). The Chapman+2 model reveals that photochemical destabilization occurs where the ozone sink is more sensitive than the source to perturbations in overhead column ozone, which is found to occur when the window of overlapping absorption by O 2 and O 3 is optically unsaturated, i.e., when overhead slant column ozone is below approximately 10 18 molec. cm -2. [ABSTRACT FROM AUTHOR]

The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic oceans. In this paper we present and analyze a data set of 10 s (2 km) merged and gap-filled observations of the key reactive species driving the chemical budgets of O 3 and CH 4 (O 3 , CH 4 , CO, H 2 O, HCHO, H 2 O 2 , CH 3 OOH, C 2 H 6 , higher alkanes, alkenes, aromatics, NO x , HNO 3 , HNO 4 , peroxyacetyl nitrate, and other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O 3 and CH 4 photochemical tendencies from this modeling data stream for ATom 1. We find that 80 %–90 % of the total reactivity lies in the top 50 % of the parcels and 25 %–35 % in the top 10 %, supporting previous model-only studies that tropospheric chemistry is driven by a fraction of all the air. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100 km) differ only slightly from the 2 km ATom 10 s data, indicating that much of the heterogeneity in tropospheric chemistry can be captured with current global chemistry models. Comparing the ATom reactivities over the tropical oceans with climatological statistics from six global chemistry models, we find generally good agreement with the reactivity rates for O 3 and CH 4. Models distinctly underestimate O 3 production below 2 km relative to the mid-troposphere, and this can be traced to lower NO x levels than observed. Attaching photochemical reactivities to measurements of chemical species allows for a richer, yet more constrained-to-what-matters, set of metrics for model evaluation. This paper presents a corrected version of the paper published under the same authors and title (sans "corrected") as 10.5194/acp-21-13729-2021. [ABSTRACT FROM AUTHOR]

The Copernicus Atmosphere Monitoring Service (CAMS) provides daily analyses and forecasts of the composition of the atmosphere, including the reactive gases such as O3 , CO , NO2 , HCHO and SO2 ; aerosol species; and greenhouse gases. The global CAMS analysis system (IFS-COMPO) is based on the ECMWF Integrated Forecasting 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 IFS-COMPO and for NWP. The main IFS-COMPO innovations include the introduction of full stratospheric chemistry; a major update of the emissions; a major update of the aerosol model, including the representation of secondary organic aerosol; several updates of the dust life cycle and optics; updates to the inorganic chemistry in the troposphere; and the assimilation of Visible Infrared Imaging Radiometer Suite (VIIRS) aerosol optical depth (AOD) and TROPOspheric Monitoring Instrument (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 them 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 the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) observations between 10 and 200 hPa, with larger deviations between 1 and 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 the Infrared Atmospheric Sounding Interferometer (IASI) instead of the Measurements Of Pollution in The Troposphere (MOPITT) instrument, 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 scorecard, 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]

This paper presents large-eddy simulations with atmospheric chemistry of four large point sources world-wide, focusing on the evaluation of NOx (NO + NO 2) emissions with the TROPOspheric Monitoring Instrument (TROPOMI). We implemented a condensed chemistry scheme to investigate how the emitted NOx (95 % as NO) is converted to NO2 in the plume. To use NOx as a proxy for CO2 emission, information about its atmospheric lifetime and the fraction of NOx present as NO2 is required. We find that the chemical evolution of the plumes depends strongly on the amount of NOx that is emitted, as well as on wind speed and direction. For large NOx emissions, the chemistry is pushed in a high- NOx chemical regime over a length of almost 100 km downwind of the stack location. Other plumes with lower NOx emissions show a fast transition to an intermediate- NOx chemical regime, with short NOx lifetimes. Simulated NO2 columns mostly agree within 20 % with TROPOMI, signalling that the emissions used in the model were approximately correct. However, variability in the simulations is large, making a one-to-one comparison difficult. We find that temporal wind speed variations should be accounted for in emission estimation methods. Moreover, results indicate that common assumptions about the NO2 lifetime (≈ 4 h) and NOx:NO2 ratios (≈ 1.3) in simplified methods that estimate emissions from NO2 satellite data need revision. [ABSTRACT FROM AUTHOR]

Atmospheric transport inversions are a powerful tool for independently estimating surface CO 2 fluxes from atmospheric CO 2 concentration measurements. However, additional tracers are needed to separate the fossil fuel CO 2 (ffCO 2) emissions from non-fossil CO 2 fluxes. In this study, we focus on radiocarbon (14 C), the most direct tracer of ffCO 2 , and the continuously measured surrogate tracer carbon monoxide (CO), which is co-emitted with ffCO 2 during incomplete combustion. In the companion paper by Maier et al. (2024), we determined discrete 14 C-based and continuous Δ CO-based estimates of the ffCO 2 excess concentration (Δ ffCO 2) compared with a clean-air reference for the urban Heidelberg observation site in southwestern Germany. The Δ CO-based Δ ffCO 2 concentration was calculated by dividing the continuously measured Δ CO excess concentration by an average 14 C-based ΔCO/ΔffCO2 ratio. Here, we use the CarboScope inversion framework adapted for the urban domain around Heidelberg to assess the potential of both types of Δ ffCO 2 observations to investigate ffCO 2 emissions and their seasonal cycle. We find that, although they are more precise, 14 C-based Δ ffCO 2 observations from almost 100 afternoon flask samples collected in the 2 years of 2019 and 2020 are not well suited for estimating robust ffCO 2 emissions in the main footprint of this urban area, which has a very heterogeneous distribution of sources including several point sources. The benefit of the continuous Δ CO-based Δ ffCO 2 estimates is that they can be averaged to reduce the impact of individual hours with an inadequate model performance. We show that the weekly averaged Δ CO-based Δ ffCO 2 observations allow for a robust reconstruction of the seasonal cycle of the area source ffCO 2 emissions from temporally flat a priori emissions. In particular, the distinct COVID-19 signal – with a steep drop in emissions in spring 2020 – is clearly present in these data-driven a posteriori results. Moreover, our top-down results show a shift in the seasonality of the area source ffCO 2 emissions around Heidelberg in 2019 compared with the bottom-up estimates from the Netherlands Organization for Applied Scientific Research (TNO). This highlights the huge potential of Δ CO-based Δ ffCO 2 to validate bottom-up ffCO 2 emissions at urban stations if the ΔCO/ΔffCO2 ratios can be determined without biases. [ABSTRACT FROM AUTHOR]

The total aviation effective radiative forcing is dominated by non-CO2 effects. The largest contributors to the non-CO2 effects are contrails and contrail cirrus. There is the possibility of reducing the climate effect of aviation by avoiding flying through ice-supersaturated regions (ISSRs), where contrails can last for hours (so-called persistent contrails). Therefore, a precise prediction of the specific location and time of these regions is needed. But a prediction of the frequency and degree of ice supersaturation (ISS) on cruise altitudes is currently very challenging and associated with great uncertainties because of the strong variability in the water vapour field, the low number of humidity measurements at the air traffic altitude, and the oversimplified parameterisations of cloud physics in weather models. Since ISS is more common in some dynamical regimes than in others, the aim of this study is to find variables/proxies that are related to the formation of ISSRs and to use these in a regression method to predict persistent contrails. To find the best-suited proxies for regressions, we use various methods of information theory. These include the log-likelihood ratios, known from Bayes' theorem, a modified form of the Kullback–Leibler divergence, and mutual information. The variables (the relative humidity with respect to ice, RH iERA5 ; the temperature, T ; the vertical velocity, ω ; the divergence, DIV; the relative vorticity, ζ ; the potential vorticity, PV; the normalised geopotential height, Z ; and the local lapse rate, γ) come from ERA5, and RH iM/I , which we assume as the truth, comes from MOZAIC/IAGOS (Measurement of Ozone and Water Vapour on Airbus In-service Aircraft/In-service Aircraft for a Global Observing System; commercial aircraft measurements). It turns out that RH iERA5 is the most important predictor of ice supersaturation, in spite of its weaknesses, and all other variables do not help much to achieve better results. Without RH iERA5 , a regression to predict ISSRs is not successful. Certain modifications of RH iERA5 before the regression (as suggested in recent papers) do not lead to improvements of ISSR prediction. Applying a sensitivity study with artificially modified RH iERA5 distributions points to the origin of the problems with the regression: the conditional distributions of RH iERA5 (conditioned on ISS and non-ISS, from RH iM/I) overlap too heavily in the range of 70 %–100 %, so for any case in that range, it is not clear whether it belongs to an ISSR or not. Evidently, this renders the prediction of contrail persistence very difficult. [ABSTRACT FROM AUTHOR]

Previous research has shown that stratospheric aerosol causes only a small temperature change per unit forcing because they produce stronger cooling in the tropical Indian Ocean and the western Pacific Ocean than in the global mean. The enhanced temperature change in this so-called "warm-pool" region activates strongly negative local and remote feedbacks, which dampen the global mean temperature response. This paper addresses the question of why stratospheric aerosol forcing affects warm-pool temperatures more strongly than CO 2 forcing, using idealized MPI-ESM simulations. We show that the aerosol's enhanced effective forcing at the top of the atmosphere (TOA) over the warm pool contributes to the warm-pool-intensified temperature change but is not sufficient to explain the effect. Instead, the pattern of surface effective forcing, which is substantially different from the effective forcing at the TOA, is more closely linked to the temperature pattern. Independent of surface temperature changes, the aerosol heats the tropical stratosphere, accelerating the Brewer–Dobson circulation. The intensified Brewer–Dobson circulation exports additional energy from the tropics to the extratropics, which leads to a particularly strong negative forcing at the tropical surface. These results show how forced circulation changes can affect the climate response by altering the surface forcing pattern. Furthermore, they indicate that the established approach of diagnosing effective forcing at the TOA is useful for global means, but a surface perspective on the forcing must be adopted to understand the evolution of temperature patterns. [ABSTRACT FROM AUTHOR]

Open burning of household and municipal solid waste is a frequent practice in many developing countries. Due to limited resources for collection and proper disposal, solid waste is often disposed of in neighborhoods and open-burned in piles to reduce odors and create space for incoming waste. Emissions from these ground-level and low-temperature burns cause air pollution, leading to adverse health effects among community residents. In this study, laboratory combustion experiments were conducted to characterize gas and particle emissions from 10 waste categories representative of those burned in South Africa: paper, leather/rubber, textiles, plastic bottles, plastic bags, vegetation (with three different moisture content levels), food discards, and combined materials. Carbon dioxide (CO 2) and carbon monoxide (CO) were measured in real time to calculate modified combustion efficiencies (MCEs). MCE is used along with video observations to determine fuel-based emission factors (EFs) during flaming and smoldering phases as well as the entire combustion process. Fuel elemental composition and moisture content have strong influences on emissions. Plastic bags have the highest carbon content and the highest combustion efficiency, leading to the highest EFs for CO 2. Textiles have the highest nitrogen and sulfur content, resulting in the highest EFs for nitrogen oxides (NO x) and sulfur dioxide (SO 2). Emissions are similar for vegetation with 0 % and 20 % moisture content; however, EFs for CO and particulate matter (PM) from the vegetation with 50 % moisture content are 3 and 20–30 times, respectively, those from 0 % and 20 % moisture content. This study also shows that neglecting carbon in the ash and PM can lead to significant overestimation of EFs. Results from this study are applicable to emission inventory improvements as well as air quality management to assess the health and climate effects of household-waste open burning. [ABSTRACT FROM AUTHOR]

Brown carbon (BrC) is an absorbing organic aerosol (OA), primarily emitted through biomass burning (BB), which exhibits light absorption unique to both black carbon (BC) and other organic aerosols. Despite many field and laboratory studies seeking to constrain BrC properties, the radiative forcing (RF) of BrC is still highly uncertain. To better understand its climate impact, we introduced BrC to the One-Moment Aerosol (OMA) module of the GISS ModelE Earth system model (ESM). We assessed ModelE sensitivity to primary BrC processed through a novel chemical aging scheme and to secondary BrC formed from biogenic volatile organic compounds (BVOCs). Initial results show that BrC typically contributes a top-of-the-atmosphere (TOA) radiative effect of 0.04 Wm-2. Sensitivity tests indicate that explicitly simulating BrC (separating it from other OAs), including secondary BrC, and simulating chemical bleaching of BrC contribute distinguishable radiative effects and should be accounted for in BrC schemes. This addition of prognostic BrC to ModelE allows greater physical and chemical complexity in OA representation with no apparent trade-off in model performance, as the evaluation of ModelE aerosol optical depth against Aerosol Robotic Network (AERONET) and Moderate Resolution Imaging Spectroradiometer (MODIS) retrieval data, with and without the BrC scheme, reveals similar skill in both cases. Thus, BrC should be explicitly simulated to allow more physically based chemical composition, which is crucial for more detailed OA studies like comparisons to in situ measurement campaigns. We include a summary of best practices for BrC representation within ModelE at the end of this paper. [ABSTRACT FROM AUTHOR]

China stands out as a major contributor to anthropogenic methane (CH 4) emissions, with coal mine methane (CMM) playing a crucial role. To control and reduce CH 4 emissions, China has made a dedicated commitment and formulated an ambitious mitigation plan. To verify the progress made, the consistent acquisition of independent CH 4 emission data is required. This paper aims to implement a wind-assigned anomaly method for the precise determination of regional-scale CMM emissions within the coal-rich Shanxi province. We use the TROPOspheric Monitoring Instrument (TROPOMI) CH 4 observations from May 2018 to May 2023, coupled with ERA5 wind and a bottom-up inventory dataset based on the IPCC (Intergovernmental Panel on Climate Change) Tier 2 approach covering the Changzhi, Jincheng, and Yangquan regions of the Shanxi province. The derived emission strengths are 8.4 × 10 26 molec. s -1 (0.706 Tg yr -1 , ± 25 %), 1.4 × 10 27 molec. s -1 (1.176 Tg yr -1 , ± 20 %), and 4.9 × 10 26 molec. s -1 (0.412 Tg yr -1 , ± 21 %), respectively. Our results exhibit biases of - 18 %, 8 %, and 14 %, respectively, when compared to the IPCC Tier 2 bottom-up inventory. Larger discrepancies are found when comparing the estimates to the Copernicus Atmosphere Monitoring Service global anthropogenic emissions (CAMS-GLOB-ANT) and Emissions Database for Global Atmospheric Research (EDGARv7.0) inventories (64 %–176 %), suggesting that the two inventories may be overestimating CH 4 emissions from the studied coal mining regions. Our estimates provide a comprehensive characterization of the regions within the Shanxi province, contribute to the validation of emission inventories, and provide additional insights into CMM emission mitigation. [ABSTRACT FROM AUTHOR]

Cloud-radiative heating (CRH) within the atmosphere affects the dynamics and predictability of extratropical cyclones. However, CRH is uncertain in numerical weather prediction and climate models, and this could affect model predictions of extratropical cyclones. In this paper, we present a systematic quantification of CRH uncertainties. To this end, we study an idealized extratropical cyclone simulated at a convection-permitting resolution of 2.5 km and combine large-eddy-model simulations at a 300 m resolution with offline radiative transfer calculations. We quantify four factors contributing to the CRH uncertainty in different regions of the cyclone: 3D cloud-radiative effects, parameterization of ice optical properties, cloud horizontal heterogeneity, and cloud vertical overlap. The last two factors can be considered essentially resolved at 300 m but need to be parameterized at a 2.5 km resolution. Our results indicate that parameterization of ice optical properties and cloud horizontal heterogeneity are the two factors contributing most to the mean uncertainty in CRH at larger spatial scales and can be more relevant for the large-scale dynamics of the cyclone. On the other hand, 3D cloud-radiative effects are much smaller on average, especially for stratiform clouds within the warm conveyor belt of the cyclone. Our analysis in particular highlights the potential to improve the simulation of CRH by better representing ice optical properties. Future work should, in particular, address how uncertainty in ice optical properties affects the dynamics and predictability of extratropical cyclones. [ABSTRACT FROM AUTHOR]

Marine aerosol affects the global energy budget and regional weather. The production of marine aerosol is primarily driven by wind at the sea–air interface. Previous studies have explored the effects of wind on marine aerosol, mostly by examining the relationships between aerosol optical depth (AOD) and surface wind speed. In this paper, utilizing the synergy of aerosol and wind observations from Aeolus, the relationships between the marine aerosol optical properties at 355 nm and the instantaneous co-located wind speeds of remote oceans are investigated at two vertical layers (within and above the marine atmospheric boundary layer (MABL)). The results show that the enhancements of the extinction and backscatter coefficients caused by wind are larger within the MABL than above it. The correlation models between extinction and backscatter with wind speed were established using power-law functions. The slope variation points occur during extinction and backscatter coefficients increasing with wind speed, indicating that the wind-driven enhancement of marine aerosol involves two phases: a rapid-growth phase with high wind dependence, followed by a slower-growth phase after the slope variation points. We also compared the AOD–wind relationship acquired from Aeolus with CALIPSO-derived results from previous research. The variation in the lidar ratio with wind speed is examined, suggesting a possible "increasing–decreasing–increasing" trend of marine aerosol particle size as wind speed increases. This study enhances the comprehension of the correlation between marine aerosol optical properties and wind speed by providing vertical information and demonstrating that their relationships are more complex than a linear or exponential relation. [ABSTRACT FROM AUTHOR]

Observations of nitrogen dioxide (NO 2) and nitrogen oxide (NO) in the stratosphere are relevant to understand long-term changes and variabilities in stratospheric nitrogen oxide (NO x) and ozone (O 3) concentrations. Due to the versatile role of NO 2 and NO in stratospheric O 3 photochemistry, they are important for recovery and build-up of O 3 holes in the stratosphere and therefore can indirectly affect human life. Thus, we present in this work the evaluation of NO 2 and NO stratospheric partial columns (> 16 km altitude) retrieved from ground-based Fourier-transform infrared (FTIR) measurements of over 25 years at Zugspitze (47.42° N, 10.98° E; 2964 m a.s.l.) and 18 years at Garmisch (47.47° N, 11.06° E; 745 m a.s.l.), Germany. The obtained stratospheric columns are only weakly influenced by tropospheric pollution and show only a very small bias of 2.5 ± 0.2 % when comparing NO 2 above Zugspitze and Garmisch. Stratospheric columns of both NO 2 and NO show a diurnal increase that depends on local solar time (LST). We quantified this behavior by calculating diurnal increasing rates. Here, we find mean values for the NO 2 diurnal increasing rate of (0.89 ± 0.14) × 10 14 and (0.94 ± 0.14) × 10 14 cm -2 h -1 at Zugspitze and Garmisch, respectively. The mean NO morning diurnal increasing rate above Zugspitze is found to be (1.42 ± 0.12) × 10 14 cm -2 h -1. Regarding the seasonal dependency of these increasing rates, for the first time, we were able to experimentally detect a significant seasonal variation in both NO 2 diurnal increasing rates and NO morning diurnal increasing rates with a maximum of (1.13 ± 0.04) × 10 14 cm -1 h -1 for NO 2 and (1.76 ± 0.25) × 10 14 cm -1 h -1 for NO in September and a minimum of (0.71 ± 0.18) × 10 14 cm -1 h -1 in December for NO 2 and a minimum of (1.18 ± 0.41) × 10 14 cm -1 h -1 in November for NO. This similar behavior may be explained by the interconnection of both species in stratospheric photochemistry. The outcome of this work is a retrieval and analysis strategy of FTIR data for NO x stratospheric columns, which can help to further validate photochemical models or improve satellite validations. The first use of this data set is shown in the companion paper (Nürnberg et al., 2023) wherein experiment-based NO x scaling factors describing the diurnal increase in the retrieved partial columns are extracted and recently published model-based scaling factors are validated. [ABSTRACT FROM AUTHOR]

Absolute calibration of Earth observation (EO) sensors is key to ensuring long-term stability and interoperability, and it is essential for long-term global climate records and forecasts. The Moon provides a photometrically stable calibration source within the range of the Earth's radiometric levels and is free from atmospheric interference. However, to use this ideal calibration source, one must model the variation in its disc-integrated irradiance resulting from changes in Sun–Earth–Moon geometries. The Lunar Irradiance Model of the European Space Agency (LIME) is a new lunar irradiance model developed from ground-based observations acquired using a lunar radiometer operating from the Izaña Atmospheric Observatory near Mount Teide, located in Tenerife, Spain. Nightly top-of-atmosphere (TOA) irradiance is determined using the Langley plot method, and each observation is traceable to the international system of units (SI) through the radiometer calibration performed at the National Physical Laboratory (NPL). Approximately 590 lunar observations acquired between March 2018 and December 2022 currently contribute to the model parameter derivation, which builds on the widely used ROLO (Robotic Lunar Observatory) model analytical formulation. This paper presents the strategy used to derive LIME parameters: the characterisation of the lunar radiometer, the derivation of nightly top-of-atmosphere lunar irradiance and a description of the model parameter derivation, along with the associated metrologically rigorous uncertainty. The model output has been compared to PROBA-V, Pléiades and Sentinel-3B, as well as to the VITO implementation of the ROLO model. Initial results indicate that LIME predicts 3 %–5 % higher lunar-disc-integrated irradiance than the ROLO model for the visible and near-infrared channels. The model output has an expanded (k=2) radiometric uncertainty of ∼ 2 % at the lunar radiometer wavelengths, and it is expected that planned observations until at least 2024 further constrain the model parameters in subsequent updates. [ABSTRACT FROM AUTHOR]

The study of aerosols in high mountain regions is essential because particulate matter can play a role in altering the energy balance of high mountain regions, and aerosols can accelerate glacier melting in high mountain areas by darkening the ice surface, reducing its reflectivity (albedo). Studying aerosols in high mountain areas provides insights into long-range transport of pollutants, atmospheric dynamics, and climate change impacts. These regions can serve as valuable observatories for studying atmospheric processes. The main aim of this paper is to define the main sources of aerosols over an entire year of sampling at the Col Margherita Atmospheric Observatory (MRG; 46°22 ′ 0.059 ′′ N, 11°47 ′ 30.911 ′′ E; 2543 m a.s.l.), a high-altitude background site in the eastern Italian Alps. Here, we discuss the potential origins of more than 100 chemical markers (major ions, water-soluble organic compounds, trace elements, and rare earth elements) using different approaches. Some diagnostic ratios were applied, but source apportionment using positive matrix factorization (PMF) was used to define the main inputs of PM 10 collected at this high-altitude site, resulting in the identification of four factors: (1) Saharan dust events, (2) long-range marine/anthropogenic influence, (3) biogenic sources, and (4) biomass-burning and anthropogenic emissions. It can be inferred that, despite the distant location of the Col Margherita site, both regional pollution and long-range anthropogenic pollution have discernible effects on this area. [ABSTRACT FROM AUTHOR]

Desert dust is an important atmospheric aerosol that affects the Earth's climate, biogeochemistry, and air quality. However, current Earth system models (ESMs) struggle to accurately capture the impact of dust on the Earth's climate and ecosystems, in part because these models lack several essential aeolian processes that couple dust with climate and land surface processes. In this study, we address this issue by implementing several new parameterizations of aeolian processes detailed in our companion paper in the Community Earth System Model version 2 (CESM2). These processes include (1) incorporating a simplified soil particle size representation to calculate the dust emission threshold friction velocity, (2) accounting for the drag partition effect of rocks and vegetation in reducing wind stress on erodible soils, (3) accounting for the intermittency of dust emissions due to unresolved turbulent wind fluctuations, and (4) correcting the spatial variability of simulated dust emissions from native to higher spatial resolutions on spatiotemporal dust variability. Our results show that the modified dust emission scheme significantly reduces the model bias against observations compared with the default scheme and improves the correlation against observations of multiple key dust variables such as dust aerosol optical depth (DAOD), surface particulate matter (PM) concentration, and deposition flux. Our scheme's dust also correlates strongly with various meteorological and land surface variables, implying higher sensitivity of dust to future climate change than other schemes' dust. These findings highlight the importance of including additional aeolian processes for improving the performance of ESM aerosol simulations and potentially enhancing model assessments of how dust impacts climate and ecosystem changes. [ABSTRACT FROM AUTHOR]

As air pollution is regarded as the single largest environmental health risk in Europe it is important that communication to the public is up to date and accurate and provides means to avoid exposure to high air pollution levels. Long- and short-term exposure to outdoor air pollution is associated with increased risks of mortality and morbidity. Up-to-date information on present and coming days' air quality helps people avoid exposure during episodes with high levels of air pollution. Air quality forecasts can be based on deterministic dispersion modelling, but to be accurate this requires detailed information on future emissions, meteorological conditions and process-oriented dispersion modelling. In this paper, we apply different machine learning (ML) algorithms – random forest (RF), extreme gradient boosting (XGB), and long short-term memory (LSTM) – to improve 1, 2, and 3 d deterministic forecasts of PM 10 , NOx , and O 3 at different sites in Greater Stockholm, Sweden. It is shown that the deterministic forecasts can be significantly improved using the ML models but that the degree of improvement of the deterministic forecasts depends more on pollutant and site than on what ML algorithm is applied. Also, four feature importance methods, namely the mean decrease in impurity (MDI) method, permutation method, gradient-based method, and Shapley additive explanations (SHAP) method, are utilized to identify significant features that are common and robust across all models and methods for a pollutant. Deterministic forecasts of PM 10 are improved by the ML models through the input of lagged measurements and Julian day partly reflecting seasonal variations not properly parameterized in the deterministic forecasts. A systematic discrepancy by the deterministic forecasts in the diurnal cycle of NOx is removed by the ML models considering lagged measurements and calendar data like hour and weekday, reflecting the influence of local traffic emissions. For O 3 at the urban background site, the local photochemistry is not properly accounted for by the relatively coarse Copernicus Atmosphere Monitoring Service ensemble model (CAMS) used here for forecasting O 3 but is compensated for using the ML models by taking lagged measurements into account. Through multiple repetitions of the training process, the resulting ML models achieved improvements for all sites and pollutants. For NOx at street canyon sites, mean squared error (MSE) decreased by up to 60 %, and seven metrics, such as R2 and mean absolute percentage error (MAPE), exhibited consistent results. The prediction of PM 10 is improved significantly at the urban background site, whereas the ML models at street sites have difficulty capturing more information. The prediction accuracy of O 3 also modestly increased, with differences between metrics. Further work is needed to reduce deviations between model results and measurements for short periods with relatively high concentrations (peaks) at the street canyon sites. Such peaks can be due to a combination of non-typical emissions and unfavourable meteorological conditions, which are rather difficult to forecast. Furthermore, we show that general models trained using data from selected street sites can improve the deterministic forecasts of NOx at the station not involved in model training. For PM 10 this was only possible using more complex LSTM models. An important aspect to consider when choosing ML algorithms is the computational requirements for training the models in the deployment of the system. Tree-based models (RF and XGB) require fewer computational resources and yield comparable performance in comparison to LSTM. Therefore, tree-based models are now implemented operationally in the forecasts of air pollution and health risks in Stockholm. Nevertheless, there is big potential to develop generic models using advanced ML to take into account not only local temporal variation but also spatial variation at different stations. [ABSTRACT FROM AUTHOR]

This paper presents the first investigation of the solubility of iron in mineral dust aerosols collected at the Henties Bay Aerosol Observatory (HBAO), in Namibia, from April to December 2017. During the study period, 10 intense dust events occurred. Elemental iron reached peak concentrations as high as 1.5 µg m -3 , significantly higher than background levels. These events are attributed to wind erosion of natural soils from the surrounding gravel plains of the Namib desert. The composition of the sampled dust is found to be overall similar to that of aerosols from northern Africa but is characterized by persistent and high concentrations of fluorine which are attributed to local fugitive dust. The fractional solubility of Fe (%SFe) for both the identified dust episodes and background conditions ranged between 1.3 % and 20 % and averaged at 7.9 % (± 4.1 %) and 6.8 (± 3.3 %), respectively. Even under background conditions, the %SFe was correlated with that of Al and Si. The solubility was lower between June and August and increased from September onwards during the austral spring. The relation to measured concentrations of particulate MSA (methane sulfonic acid), solar irradiance, and wind speed suggests a possible two-way interaction whereby marine biogenic emissions from the coastal Benguela upwelling to the atmosphere would increase the solubility of iron-bearing dust according to the photo-reduction processes. This first investigation points to the western coast of southern Africa as a complex environment with multiple processes and active exchanges between the atmosphere and the Atlantic Ocean, requiring further research. [ABSTRACT FROM AUTHOR]

Black carbon (BC) exerts potential effects on climate, especially in the Tibetan Plateau (TP), where the cryosphere and environment are very sensitive to climate change. The TP saw a record-breaking aerosol pollution event during the period from 20 April to 10 May 2016. This paper investigates the meteorological causes of the severe aerosol pollution event, the transboundary transport flux of BC, the aerosol–meteorology feedback, and its effect on the transboundary transport flux of BC during the severe aerosol pollution event using observational and reanalysis datasets as well as simulation based on a coupled meteorology and aerosol/chemistry model, Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). By analyzing weather maps derived from the reanalysis dataset, it is found that the plateau vortex and southerly winds were key factors that contributed to the severe aerosol pollution event. Subsequently, due to the good performance of the WRF-Chem model for the spatiotemporal characteristics of meteorological conditions and aerosols, the transboundary transport flux of BC during the pollution event was investigated. The results show that the vertically integrated cross-Himalayan transport flux of BC decreases from west to east, with the largest transport flux of 20.8 mg m -2 s -1 occurring at the deepest mountain valley in southwestern TP. Results from simulations with and without aerosol–meteorology feedback show that aerosols induce significant changes in meteorological conditions in the southern TP and the Indo-Gangetic Plain (IGP), with the atmospheric stratification being more stable and the planetary boundary layer height decreasing in both regions, and the 10 m wind speed increasing in the southern TP but decreasing in the IGP. Changes in meteorological conditions in turn lead to a decrease in the surface BC concentration in the southern TP of up to 0.16 µ g m -3 (50 %) and an increase in the surface BC concentration in the IGP of up to 2.2 µ g m -3 (75 %). In addition, it is found that the aerosol–meteorology feedback decreases the vertically integrated transboundary transport flux of BC from the central and western Himalayas towards the TP. This study not only provides crucial policy implications for mitigating glacier melt caused by aerosols over the TP but is also of great significance for the protection of the ecological environment of the TP. [ABSTRACT FROM AUTHOR]

Aviation emissions that are dispersed into the Earth's atmosphere affect the climate and air pollution, with significant spatiotemporal variation owing to heterogeneous aircraft activity. In this paper, we use historical flight trajectories derived from Automatic Dependent Surveillance–Broadcast (ADS-B) telemetry and reanalysis weather data for 2019–2021 to develop the Global Aviation emissions Inventory based on ADS-B (GAIA). In 2019, 40.2 million flights collectively travelled 61 billion kilometres using 283 Tg of fuel, leading to CO 2 , NO X and non-volatile particulate matter (nvPM) mass and number emissions of 893 Tg, 4.49 Tg, 21.4 Gg and 2.8 × 10 26 respectively. Global responses to COVID-19 led to reductions in the annual flight distance flown and CO 2 and NO X emissions in 2020 (- 43 %, - 48 % and - 50 % respectively relative to 2019) and 2021 (- 31 %, - 41 % and - 43 % respectively), with significant regional variability. Short-haul flights with durations < 3 h accounted for 83 % of all flights but only for 35 % of the 2019 CO 2 emissions, while long-haul flights with durations > 6 h (5 % of all flights) were responsible for 43 % of CO 2 and 49 % of NO X emissions. Globally, the actual flight trajectories flown are, on average, ∼ 5 % greater than the great circle path between the origin and destination airports, but this varies by region and flight distance. An evaluation of 8705 unique flights between London and Singapore showed large variabilities in the flight trajectory profile, fuel consumption and emission indices. GAIA captures the spatiotemporal distribution of aviation activity and emissions and is provided for use in future studies to evaluate the negative externalities arising from global aviation. [ABSTRACT FROM AUTHOR]

The Tropospheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor (S5P) satellite is part of the latest generation of trace gas monitoring satellites and provides a new level of spatio-temporal information with daily global coverage, which enables the calculation of daily globally averaged CH4 concentrations. To investigate changes in atmospheric methane, the background CH4 level (i.e. the CH4 concentration without seasonal and short-term variations) has to be determined. CH4 growth rates vary in a complex manner and high-latitude zonal averages may have gaps in the time series, and thus simple fitting methods do not produce reliable results. In this paper we present an approach based on fitting an ensemble of dynamic linear models (DLMs) to TROPOMI data, from which the best model is chosen with the help of cross-validation to prevent overfitting. This method is computationally fast and is not dependent on additional inputs, allowing for fast and continuous analysis of the most recent time series data. We present results of global annual methane increases (AMIs) for the first 4.5 years of S5P/TROPOMI data, which show good agreement with AMIs from other sources. Additionally, we investigated what information can be derived from zonal bands. Due to the fast meridional mixing within hemispheres, we use zonal growth rates instead of AMIs, since they provide a higher temporal resolution. Clear differences can be observed between Northern Hemisphere and Southern Hemisphere growth rates, especially during 2019 and 2022. The growth rates show similar patterns within the hemispheres and show no short-term variations during the years, indicating that air masses within a hemisphere are well-mixed during a year. Additionally, the growth rates derived from S5P/TROPOMI data are largely consistent with growth rates derived from Copernicus Atmospheric Monitoring Service (CAMS) global-inversion-optimized (CAMS/INV) data, which use surface observations. In 2019 a reduction in growth rates can be observed for the Southern Hemisphere, while growth rates in the Northern Hemisphere stay stable or increase. During 2020 a strong increase in Southern Hemisphere growth rates can be observed, which is in accordance with recently reported increases in Southern Hemisphere wetland emissions. In 2022 the reduction in the global AMI can be attributed to decreased growth rates in the Northern Hemisphere, while growth rates in the Southern Hemisphere remain high. Investigations of fluxes from CAMS/INV data support these observations and suggest that the Northern Hemisphere decrease is mainly due to the decrease in anthropogenic fluxes, while in the Southern Hemisphere, wetland fluxes continued to rise. While the continued increase in Southern Hemisphere wetland fluxes agrees with existing studies about the causes of observed methane trends, the difference between Northern Hemisphere and Southern Hemisphere methane increases in 2022 has not been discussed before and calls for further research. [ABSTRACT FROM AUTHOR]

Paul Jozef Crutzen was a pioneer in the atmospheric sciences, a kind-hearted and humorous person with empathy for the private lives of his colleagues and students, and a man who upheld the highest scientific standards for himself and for others. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere, from the mesosphere to the stratosphere and from the stratosphere to the troposphere. In particular, he was the first to describe the NOx -driven ozone depletion cycle in the stratosphere, he was among the first to develop the idea of chemical formation of ozone in the troposphere, he provided key concepts to explain the "ozone hole", and he made fundamental discoveries about the effects of biomass burning on the troposphere. Understanding and addressing the causes of anthropogenic air pollution and climate change were the driving motivations for his scientific work. In his work, he did not shy away from challenge and provocation. His work on smoke from fires after a potential nuclear war inspired new research on a concept now known as "nuclear winter". He also initiated the reopening of the debate on "geoengineering" – a concept now referred to as "climate intervention". He also brought the term "Anthropocene" to the popular debate. Moreover, he had a strong influence on atmospheric science through his educational role; there is a very large number of outstanding scientists who started their career with scientific work with Paul. In 2000, Paul was among the founders of the journal Atmospheric Chemistry and Physics, which was unique at the time in providing public discussion of published preprints as well as what we now call "open access" to published articles. Paul's work on human impacts on atmosphere and climate has had a profound impact on the environmental policies of many countries for decades. In the future, his work will continue to be a guide for generations of scientists and environmental policymakers to come. [ABSTRACT FROM AUTHOR]

Tropical cirrus clouds, i.e., any type of ice cloud with tops above 400 hPa, play a critical role in the climate system and are a major source of uncertainty in our understanding of global warming. Tropical cirrus clouds involve processes spanning a wide range of spatial and temporal scales, from ice microphysics on cloud scales to mesoscale convective organization and planetary wave dynamics. This complexity makes tropical cirrus clouds notoriously difficult to model and has left many important questions stubbornly unanswered. At the same time, their multi-scale nature makes them well-positioned to benefit from the rise of global, high-resolution simulations of Earth's atmosphere and a growing abundance of remotely sensed and in situ observations. Rapid progress on our understanding of tropical cirrus requires coordinated efforts to take advantage of these modern computational and observational abilities. In this opinion paper, we review recent progress in cirrus studies, highlight important unanswered questions, and discuss promising paths forward. Significant progress has been made in understanding the life cycle of convectively generated "anvil" cirrus and the response of their macrophysical properties to large-scale controls. On the other hand, much work remains to be done to fully understand how small-scale anvil processes and the climatological anvil radiative effect will respond to global warming. Thin, in situ formed cirrus clouds are now known to be closely tied to the thermal structure and humidity of the tropical tropopause layer, but microphysical uncertainties prevent a full understanding of this link, as well as the precise amount of water vapor entering the stratosphere. Model representation of ice-nucleating particles, water vapor supersaturation, and ice depositional growth continue to pose great challenges to cirrus modeling. We believe that major advances in the understanding of tropical cirrus can be made through a combination of cross-tool synthesis and cross-scale studies conducted by cross-disciplinary research teams. [ABSTRACT FROM AUTHOR]

To be able to meet global grand challenges (climate change; biodiversity loss; environmental pollution; scarcity of water, food and energy supplies; acidification; deforestation; chemicalization; pandemics), which all are closely interlinked with each other, we need comprehensive open data with proper metadata, along with open science. The large data sets from ground-based in situ observations, ground and satellite remote sensing, and multiscale modeling need to be utilized seamlessly. In this opinion paper, we demonstrate the power of the SMEAR (Station for Measuring Earth surface–Atmosphere Relations) concept via several examples, such as detection of new particle formation and the particles' subsequent growth, quantifying atmosphere–ecosystem feedback loops, and combining comprehensive observations with emergency science and services, as well as studying the effect of COVID-19 restrictions on different air quality and climate variables. The future needs and the potential of comprehensive observations of the environment are summarized. [ABSTRACT FROM AUTHOR]

As the near-surface atmosphere over the Antarctic Plateau is cold and pristine, its physico-chemical conditions resemble to a certain extent those of the high troposphere where cirrus clouds form. In this paper, we carry out an observational analysis of two shallow fog clouds forming in situ at cirrus temperatures – that is, temperatures lower than 235 K – at Dome C, inner Antarctic Plateau. The combination of lidar profiles with temperature and humidity measurements from advanced thermo-hygrometers along a 45 m mast makes it possible to characterise the formation and development of the fog. High supersaturations with respect to ice are observed before the initiation of fog, and the values attained suggest that the nucleation process at play is the homogeneous freezing of solution aerosol droplets. This is the first time that in situ observations show that this nucleation pathway can be at the origin of an ice fog. Once nucleation occurs, the relative humidity gradually decreases down to subsaturated values with respect to ice in a few hours, owing to vapour deposition onto ice crystals and turbulent mixing. The development of fog is tightly coupled with the dynamics of the boundary layer which, in the first study case, experiences a weak diurnal cycle, while in the second case, it transits from a very stable to a weakly stable dynamical regime. Overall, this paper highlights the potential of the site of Dome C for carrying out observational studies of very cold cloud microphysical processes in natural conditions and using in situ ground-based instruments. [ABSTRACT FROM AUTHOR]

In this paper, we exploit the first 10-year data record (2008–2017) of nitric acid (HNO3) total columns measured by the IASI-A/MetOp infrared sounder, characterized by an exceptional daily sampling and a good vertical sensitivity in the lower-to-mid stratosphere (around 50 hPa), to monitor the relationship between the temperature decrease and the observed HNO3 loss that occurs each year in the Antarctic stratosphere during the polar night. Since the HNO3 depletion results from the formation of polar stratospheric clouds (PSCs), which trigger the development of the ozone (O3) hole, its continuous monitoring is of high importance. We verify here, from the 10-year time evolution of HNO 3 together with temperature (taken from reanalysis at 50 hPa), the recurrence of specific regimes in the annual cycle of IASI HNO3 and identify (for each year) the day and the 50 hPa temperature ("drop temperature") corresponding to the onset of strong HNO3 depletion in the Antarctic winter. Although the measured HNO3 total column does not allow for the uptake of HNO3 by different types of PSC particles along the vertical profile to be differentiated, an average drop temperature of 194.2 ± 3.8 K , close to the nitric acid trihydrate (NAT) existence threshold (∼ 195 K at 50 hPa), is found in the region of potential vorticity lower than - 10 × 10 -5 Km2kg-1s-1 (similar to the 70–90 ∘ S equivalent latitude region during winter). The spatial distribution and interannual variability of the drop temperature are investigated and discussed. This paper highlights the capability of the IASI sounder to monitor the evolution of polar stratospheric HNO3 , a key player in the processes involved in the depletion of stratospheric O3. [ABSTRACT FROM AUTHOR]

The semi-permanent stratocumulus clouds over the south-eastern Atlantic Ocean (SEA) can act as an "air conditioner" to the regional and global climate system. The interaction of aerosols and clouds becomes important in this region and can lead to negative radiative effects, partially offsetting the positive radiative forcing of greenhouse gases. A key pathway by which aerosols affect cloud properties is by acting as cloud condensation nuclei (CCN). In this paper, we use the United Kingdom Earth System Model (UKESM1) to investigate the sources of CCN (from emissions and atmospheric processes) in the SEA as well as the response of the cloud droplet number concentration (CDNC), the cloud liquid water path (LWP), and radiative forcing to these sources during 2016 and 2017. Overall, free and upper troposphere nucleated aerosols are the dominant source of the boundary layer CCN concentration at 0.2 % supersaturation (CCN 0.2%), contributing an annual average of ∼ 41 % as they subside and entrain into the marine boundary layer, which is consistent with observations highlighting the important role of nucleation in the boundary layer CCN concentration. In terms of emission sources, anthropogenic emissions (from energy, industry, agriculture, etc.) contribute the most to the annual average CCN 0.2% in the marine boundary layer (∼ 26 %), followed by biomass burning (BB, ∼ 17 %). In the cloud layer, BB contributes about 34 % of the annual CCN 0.2% , midway between the contributions from aerosol nucleation (36 %) and anthropogenic sources (31 %). The contribution of aerosols from different sources to the CDNC is consistent with their contribution to CCN 0.2% within the marine boundary layer, with free and upper troposphere aerosol nucleation being the most important source of the CDNC overall. In terms of emission sources, anthropogenic sources are also the largest contributors to the annual average CDNC, closely followed by BB. However, during the BB season, BB and free and upper troposphere aerosol nucleation are equally the most important sources of the CDNC. The contribution of BB to the CDNC is more significant than its increase to CCN 0.2% , mainly because BB aerosols are mostly located directly above the inversion layer in the model; thus, they can increase the in-cloud CDNC by enhancing the supersaturation through the dynamical feedback due to short-wave absorption. An aerosol source that shows an increase in the CDNC also shows an increase in the LWP resulting from a reduction in autoconversion. Due to the absorption effect, BB aerosol can enhance existing temperature inversions and reduce the entrainment of sub-saturated air, leading to a further increase in the LWP. As a result, the contribution of BB to the LWP is second only to aerosol nucleation on annual averages. These findings demonstrate that BB is not the dominant source of CCN within the marine boundary layer from an emission source perspective. However, as most BB aerosols are located directly above the inversion layer, their effect on clouds increases due to their absorption effect (about the same as anthropogenic sources for the CDNC and more than anthropogenic sources for the LWP), highlighting the crucial role of their radiative effect on clouds. The results on the radiative effects of aerosols show that BB aerosol exhibits an overall positive RF ari (radiative forcing associated with aerosol–radiation interactions), but its net effective radiative forcing remains negative due to its effect on clouds (mainly due to its absorbing effect). By quantifying aerosol and cloud properties affected by different sources, this paper provides a framework for understanding the effects of aerosol sources on marine stratocumulus clouds and radiation in the SEA. [ABSTRACT FROM AUTHOR]

This paper reveals the dynamic movement characteristics of thunderstorms using total lightning data obtained from very low- and low-frequency (VLF/LF) location measurements. Eight thunderstorms, which were evenly distributed in the morning, midday, afternoon and evening, are selected to compare the different kinematic features over the Pearl River Delta (PRD) region in the south of China from 17 to 23 May 2014. The connected-neighbourhood labelling method is used to identify lightning clusters and obtain the centroids. Significant characterisation parameters are put forward as metrics to reveal the kinematic features of thunderstorms, including the duration time, valid area (VA), movement velocity, movement direction and farthest distance in longitude and latitude during the life cycle of the storm. A common trend is that the storms initiate in the west of the PRD region, moving to the east and disappearing after the thunderstorm travels around 106.5 km in longitude. There are two kinds of distributions to depict the property of the valid area, which are one-peak distribution with the maximum in the mature stage and two-peak distribution with a relatively smaller peak in the early time of the storm. The velocity does not show the same trend as the variation in VA which shows a steady increase or decrease during the lifetime of thunderstorms. The biggest VA and highest velocity are 891 km 2 occurring on the evening of 17 May and 204.8 km h -1 occurring on the morning of 20 May. The 19 May evening storm was the weakest, with the maximum VA and velocity being 253 km 2 and 115.3 km h -1 , respectively. The motion of eight storms shows a distinct pattern as the spread of direction distributes tightly in the range of 0–180 ∘. The movement characteristics of thunderstorms and the associated parameters may help to improve the nowcasting and forecasting system of thunderstorms in the warm season. [ABSTRACT FROM AUTHOR]

Chemical losses of ambient reactive volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source apportionments. These losses substantially reduce the concentrations of highly reactive species in the apportioned factor profiles and result in the underestimation of source contributions. This review assesses the common methods and existing issues in ways to reduce losses and loss impacts in source analyses and suggests research directions for improved VOC source apportionments. Positive matrix factorization (PMF) is now the main VOC source analysis method compared to other mathematical models. The issue in using any apportionment tool is the processing of the data to be analyzed to reduce the impacts of reactive losses. Estimating the initial concentrations of ambient VOCs based on photochemical age has become the primary approach to reduce reactive loss effects in PMF, except for selecting low-reactivity species or nighttime data into the analysis. Currently, the initial concentration method only considers daytime reactions with hydroxyl (⚫ OH) radicals. However, the ⚫ OH rate constants vary with temperature, and that has not been considered. Losses from reactions with O3 and NO3 radicals, especially for alkene species, remain to be included. Thus, the accuracy of the photochemical age estimation is uncertain. Beyond developing accurate quantitative approaches for reactive losses, source analyses methods for the consumed VOCs and the accurate quantification of different source contributions to O3 and secondary organic aerosols are important additional directions for future research. [ABSTRACT FROM AUTHOR]

Carbon monoxide (CO) concentrations in the troposphere are decreasing globally, with Africa as an exception. Yet, the region is understudied, with a deficit of ground-based observations and highly uncertain CO emission inventories. This paper reports multiyear observational CO data from the Mt. Kenya Global Atmosphere Watch (GAW) station, as well as summertime CO isotope observations from both Mt. Kenya and Nairobi, Kenya. The CO variability at Mt. Kenya is characterized by slightly increased concentrations during dry periods and a strong influence of short-term pollution events. While some data gaps and differences in instrumentation complicate decadal-scale trend analysis, a small long-term increase is resolved. High-pollution events are consistent with isotopic signal from downwind savanna fires. The isotope fingerprint of CO in Nairobi indicates an overwhelming dominance (near 100 %) of primary emissions from fossil fuel combustion with implications for air pollution policy. In contrast, the isotope signature of CO intercepted at the large-footprint Mt. Kenya region suggests that at least 70 % is primary sourced, with a predominance likely from savanna fires in Africa. Taken together, this study provides quantitative constraints of primary vs. secondary CO in the eastern Africa region and in urban Nairobi, with implications for satellite-based emission inventories as well as for chemical transport and climate modeling. [ABSTRACT FROM AUTHOR]

This article begins with a review of important advances in the chemistry and related physics of the mesosphere and lower thermosphere (MLT) region of the atmosphere that have occurred over the past 2 decades, since the founding of Atmospheric Chemistry and Physics. The emphasis here is on chemistry, but we also discuss recent findings on atmospheric dynamics and forcings to the extent that these are important for understanding MLT composition and chemistry. Topics that are covered include observations, with satellite, rocket and ground-based techniques; the variability and connectedness of the MLT on various length scales and timescales; airglow emissions; the cosmic dust input and meteoric metal layers; and noctilucent/polar mesospheric ice clouds. The paper then concludes with a discussion of important unanswered questions and likely future directions for the field over the next decade. [ABSTRACT FROM AUTHOR]

Lightning can cause natural hazards that result in human and animal injuries and fatalities, infrastructure destruction, and wildfire ignition. Lightning-produced NOx (L NOx), a major NOx (NOx=NO+NO2) source, plays a vital role in atmospheric chemistry and global climate. The Earth has experienced marked global warming and changes in aerosol and aerosol precursor emissions (AeroPEs) since the 1960s. Investigating long-term historical (1960–2014) lightning and LNOx trends can provide important indicators for all lightning-related phenomena and for LNOx effects on atmospheric chemistry and global climate. Understanding how global warming and changes in AeroPEs influence historical lightning and LNOx trends can be helpful in providing a scientific basis for assessing future lightning and LNOx trends. Moreover, global lightning activities' responses to large volcanic eruptions such as the 1991 Pinatubo eruption are not well elucidated and are worth exploring. This study employed the widely used cloud top height lightning scheme (CTH scheme) and the newly developed ice-based ECMWF-McCAUL lightning scheme to investigate historical (1960–2014) lightning and LNOx trends and variations as well as their influencing factors (global warming, increases in AeroPEs, and the Pinatubo eruption) in the framework of the CHASER (MIROC) chemistry–climate model. The results of the sensitivity experiments indicate that both lightning schemes simulated almost flat global mean lightning flash rate anomaly trends during 1960–2014 in CHASER (the Mann–Kendall trend test (significance inferred as 5 %) shows no trend for the ECMWF-McCAUL scheme, but a 0.03 %yr-1 significant increasing trend is detected for the CTH scheme). Moreover, both lightning schemes suggest that past global warming enhances historical trends for global mean lightning density and global LNOx emissions in a positive direction (around 0.03 %yr-1 or 3 %K-1). However, past increases in AeroPEs exert an opposite effect on the lightning and LNOx trends (- 0.07 % to - 0.04 %yr-1 for lightning and - 0.08 % to - 0.03 %yr-1 for L NOx) when one considers only the aerosol radiative effects in the cumulus convection scheme. Additionally, effects of past global warming and increases in AeroPEs in lightning trends were found to be heterogeneous across different regions when analyzing lightning trends on the global map. Lastly, this paper is the first of study results suggesting that global lightning activities were markedly suppressed during the first year after the Pinatubo eruption as shown in both lightning schemes (global lightning activities decreased by as much as 18.10 % as simulated by the ECMWF-McCAUL scheme). Based on the simulated suppressed lightning activities after the Pinatubo eruption, the findings also indicate that global LNOx emissions decreased after the 2- to 3-year Pinatubo eruption (1.99 %–8.47 % for the annual percentage reduction). Model intercomparisons of lightning flash rate trends and variations between our study (CHASER) and other Coupled Model Intercomparison Project Phase 6 (CMIP6) models indicate great uncertainties in historical (1960–2014) global lightning trend simulations. Such uncertainties must be investigated further. [ABSTRACT FROM AUTHOR]