Long-term and continuous observations of mesospheric–lower thermospheric winds are rare, but they are important to investigate climatological changes at these altitudes on timescales of several years, covering a solar cycle and longer. Such long time series are a natural heritage of the mesosphere–lower thermosphere climate, and they are valuable to compare climate models or long-term runs of general

Statistics on the occurrence of clear skies, ice clouds, and mixed-phase clouds over Concordia Station, in the Antarctic Plateau, are provided for multiple timescales and analyzed in relation to simultaneous meteorological parameters measured at the surface. Results are obtained by applying a machine learning cloud identification and classification (CIC) code to 4 years of measurements between 2012–2015

Ship emissions and coastal air pollution around China are expected to be alleviated with the gradual implementation of ship domestic emission control area (DECA) policies. However, a comprehensive post-assessment on the policy's effectiveness is still lacking. This study developed a series of high-spatiotemporal ship emission inventories around China from 2016 to 2019 based on an updated Ship Emission

For the radiative impact of individual climate forcings, most previous studies focused on the global mean values at the top of the atmosphere (TOA), and less attention has been paid to surface processes, especially for black carbon (BC) aerosols. In this study, the surface radiative responses to five different forcing agents were analyzed by using idealized model simulations. Our analyses reveal that

Abstract. Extreme convective events in the troposphere not only have immediate impacts on the surface, they can also influence the dynamics and composition of the lower stratosphere (LS). One major impact is the moistening of the LS by overshooting convection. This effect plays a crucial role in climate feedback as small changes of water vapor in the upper troposphere and lower stratosphere (UTLS)

Gravity waves play a significant role in driving the semiannual oscillation (SAO) of the zonal wind in the tropics. However, detailed knowledge of this forcing is missing, and direct estimates from global observations of gravity waves are sparse. For the period 2002–2018, we investigate the SAO in four different reanalyses: ERA-Interim, JRA-55, ERA-5, and MERRA-2. Comparison with the SPARC zonal wind

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

We develop a new inversion method which is suitable for linear and nonlinear emission source (ES) modeling, based on the three-dimensional decoupled direct (DDM-3D) sensitivity analysis module in the Community Multiscale Air Quality (CMAQ) model and the three-dimensional variational (3DVAR) data assimilation technique. We established the explicit observation operator matrix between the ES and receptor

Abstract. Aerosols can enhance ecosystem productivity by increasing diffuse radiation. Such diffuse fertilization effects (DFEs) vary among different aerosol compositions and sky conditions. Here, we apply a suite of chemical, radiation, and vegetation models in combination with ground- and satellite-based measurements to assess the impacts of natural and anthropogenic aerosol species on gross primary

Abstract. Quantification of the radiative adjustment of marine low-clouds to aerosol perturbations, regionally and globally, remains the largest source of uncertainty in assessing current and future climate. An important step towards quantifying the role of aerosol in modifying cloud radiative properties is to quantify the susceptibility of cloud albedo and liquid water path (LWP) to perturbations

Abstract. We present a method for estimating fossil fuel methane emissions using observations of methane and ethane, accounting for uncertainty in their emission ratio. The ethane:methane emission ratio is incorporated as a variable parameter in a Bayesian model, with its own prior distribution and uncertainty. We find that using an emission ratio distribution mitigates bias from using a fixed, potentially

Abstract. The number of cloud droplets formed at the cloud base depends both on the properties of aerosol particles and the updraft velocity of an air parcel at the cloud base. As the spatial scale of updrafts is too small to be resolved in global atmospheric models, the updraft velocity is commonly parameterised based on the available turbulent kinetic energy. Here we present alternative methods through

Information on the spatiotemporal characteristics of Beijing's urban–rural near-surface air temperature difference, known as the canopy layer urban heat island (UHI), is important for future urban climate management strategies. This paper investigates the variation of near-surface air temperatures within Beijing at a neighbourhood-scale resolution (∼ 100 m) during winter 2016 and summer 2017. We perform

Non-methane volatile organic compounds (NMVOCs) are important precursors of ozone (O3) and secondary organic aerosol (SOA), which play key roles in tropospheric chemistry. A huge amount of NMVOC emissions from solvent use are complicated by a wide spectrum of sources and species. This work presents a long-term NMVOC emission inventory of solvent use during 2000–2017 in China. Based on a mass (material)

Sulfate is one of the main components of haze fine particles, and its formation mechanism remains controversial. A lack of detailed and comprehensive field data hinders the accurate evaluation of relative roles of prevailing sulfate formation pathways. Here, we analyzed the sulfate production rates using a state-of-the-art multiphase model constrained to the observed concentrations of transition metal

The OH-radical-initiated oxidation of 3-methyl-3-penten-2-one and 4-methyl-3-penten-2-one was investigated in two atmospheric simulation chambers at 298±3 K and 990±15 mbar using long-path FTIR spectroscopy. The rate coefficients of the reactions of 3-methyl-3-penten-2-one and 4-methyl-3-penten-2-one with OH radicals were determined to be (6.5±1.2)×10-11 and (8.1±1.3)×10-11 cm3molecule-1s-1, respectively

Abstract. Saturated aldehydes, e.g. 2-methylbutanal (2MB, CH3CH2CH(CH3)C(O)H), are emitted into the atmosphere by several biogenic sources. The first step in the daytime atmospheric degradation of 2MB involves gas-phase reactions initiated by hydroxyl (OH) radicals, chlorine (Cl) atoms and/or sunlight. In this work, we report the rate coefficients for the gas-phase reaction of 2MB with OH (kOH) and

Abstract. Marine atmospheric boundary layer clouds cover vast areas of the Southern Ocean (SO), where they are commonly organized into mesoscale cellular convection (MCC). Using three years of Himawari-8 geostationary satellite observations, open and closed MCC structures are identified using a hybrid convolutional neural network. The results of the climatology show that open MCC clouds are roughly

We describe in this study the analysis of small and large horizontal-scale gravity waves from datasets composed of images from multiple mesospheric airglow emissions as well as multistatic specular meteor radar (MSMR) winds collected in early November 2018, during the SIMONe–2018 (Spread-spectrum Interferometric Multi-static meteor radar Observing Network) campaign. These ground-based measurements

The Indian megacity of Delhi suffers from some of the poorest air quality in the world. While ambient NO2 and particulate matter (PM) concentrations have received considerable attention in the city, high ground-level ozone (O3) concentrations are an often overlooked component of pollution. O3 can lead to significant ecosystem damage and agricultural crop losses, and adversely affect human health. During

Mixed-phase clouds are globally omnipresent and play a major role in the Earth's radiation budget and precipitation formation. The existence of liquid droplets in the presence of ice particles is microphysically unstable and depends on a delicate balance of several competing processes. Understanding mechanisms that govern ice initiation and moisture supply are important to understand the life cycle

Abstract. While the burden caused by air pollution in urban areas is well documented, the origin of this pollution and therefore the responsibility of the urban areas in generating this pollution is still a subject of scientific discussion. Source Apportionment represents a useful technique to quantify the city responsibility but the approaches and applications are not harmonized, therefore not comparable

Abstract. The dispersion of cooking-generated aerosols from an urban street canyon is examined with building-resolving computational fluid dynamics (CFD). Using a comprehensive urban CFD model (PALM) with a sectional aerosol module (SALSA), emissions from deep frying and boiling are considered for near-ground and elevated sources. It is found that, with representative choices of the source flux, the

Abstract. Aerosol particles form in the atmosphere by clustering of certain atmospheric vapors. After growing to larger particles by condensation of low volatile gases, they can affect the Earth’s climate directly by scattering light and indirectly by acting as cloud condensation nuclei. Observations of low-volatility aerosol precursor gases have been reported around the world but longer-term measurement

Abstract. Mineral dust impacts key processes in the Earth system, including the radiation budget, clouds, and nutrient cycles. We evaluate dust aerosols in 16 models participating in the sixth phase of the Coupled Model Intercomparison Project (CMIP6) against multiple reanalyses and satellite observations. Most models, and particularly the multi-model ensemble mean (MEM), capture the spatial patterns

Abstract. Atmospheric new particle formation (NPF) is an important source of climate-relevant aerosol particles which has been observed at many locations globally. To study this phenomenon, the first step is to identify whether an NPF event occurs or not on a given day. In practice, NPF event identification is performed visually by classifying the NPF event or non-event days from the particle number

Abstract. Variations in the strength of the Northern Hemisphere winter polar stratospheric vortex can influence surface variability in the Atlantic sector. Disruptions of the vortex, known as sudden stratospheric warmings (SSW), are associated with an equatorward shift and deceleration of the North Atlantic jet stream, negative phases of the North Atlantic Oscillation as well as cold snaps over Eurasia

This study analyzed the nature, mechanisms and drivers for hot-and-polluted episodes (HPEs) in the Pearl River Delta, China. Numerical model simulations were conducted for the summer and autumn of 2009–2011. A total of eight HPEs were identified, mainly occurring in August and September. K-means clustering was applied to group the HPEs into three clusters based on their characteristics and mechanisms

From 27 July to 10 August 2017, the airborne StratoClim mission took place in Kathmandu, Nepal, where eight mission flights were conducted with the M-55 Geophysica up to altitudes of 20 km. New particle formation (NPF) was identified by the abundant presence of nucleation-mode aerosols, with particle diameters dp smaller than 15 nm, which were in-situ-detected by means of condensation nuclei (CN) counter

The acidity of aqueous atmospheric solutions is a key parameter driving both the partitioning of semi-volatile acidic and basic trace gases and their aqueous-phase chemistry. In addition, the acidity of atmospheric aqueous phases, e.g., deliquesced aerosol particles, cloud, and fog droplets, is also dictated by aqueous-phase chemistry. These feedbacks between acidity and chemistry have crucial implications

The Brewer–Dobson circulation (BDC) is a key feature of the stratosphere that models need to accurately represent in order to simulate surface climate variability and change adequately. For the first time, the Climate Model Intercomparison Project includes in its phase 6 (CMIP6) a set of diagnostics that allow for careful evaluation of the BDC. Here, the BDC is evaluated against observations and reanalyses

Rate coefficients for the reaction of NO3 radicals with a series of aromatic aldehydes were measured in a 7300 L simulation chamber at ambient temperature and pressure by relative and absolute methods. The rate coefficients for benzaldehyde (BA), ortho-tolualdehyde (O-TA), meta-tolualdehyde (M-TA), para-tolualdehyde (P-TA), 2,4-dimethyl benzaldehyde (2,4-DMBA), 2,5-dimethyl benzaldehyde (2,5-DMBA)

Using radiosonde observations at five stations in the tropical western Pacific and reanalysis data for the 15 years from 2005 to 2019, we report an extremely negative anomaly in atmospheric water vapor during the super El Niño winter of 2015/16 and compare the anomaly with that in the other three El Niño winters of the period. A strong specific humidity anomaly is concentrated below 8 km of the troposphere

Abstract. This study demonstrates the ability of large-eddy simulation (LES) forced by a large-scale model to reproduce plume dispersion in an actual field campaign. Our aim is to bring together field observations taken under non-ideal conditions and LES to show that this combination can help to derive point source strengths from sparse observations. We prepared a one-day case study based on data collected

Abstract. Various atmospheric sources and sinks regulate the abundance of tropospheric formaldehyde (HCHO) which is an important trace gas impacting the HOx (≡ HO2 + OH) budget and the concentration of ozone (O3). In this study, we present the formation and destruction terms of ambient HCHO and O3 calculated from in-situ observations of various atmospheric trace gases measured at three different sites

Abstract. The intensity and position of the Southern Hemisphere stratospheric polar vortex edge is evaluated as a function of equivalent latitude over the 1979–2020 period on three isentropic levels (475 K, 550 K and 675 K) from ECMWF ERA-Interim reanalysis. The study also includes an analysis of the onset and breakup dates of the polar vortex, which are determined from wind thresholds (e.g. 15.2 m

Abstract. Correlations of night-time atmospheric methane (CH4) and 222Radon (222Rn) observations in Heidelberg, Germany, were evaluated with the Radon Tracer Method (RTM) to estimate the trend of annual CH4 emissions from 1996–2020 in the catchment area of the station. After an initial 30 % decrease of emissions from 1996 to 2004, no further systematic trend but small inter-annual variations were observed

Abstract. The Global Monitoring Plan of the Minamata Convention on Mercury was established to generate long-term data necessary for evaluating the effectiveness of regulatory measures at a global scale. After 25 years monitoring (since 1995), Mace Head is one of the atmospheric monitoring stations with the longest mercury record, and has produced sufficient data for the analysis of temporal trends

An advanced multiwavelength polarization Raman lidar was operated aboard the icebreaker Polarstern during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition to continuously monitor aerosol and cloud layers in the central Arctic up to 30 km height. The expedition lasted from September 2019 to October 2020 and measurements were mostly taken between 85 and 88

Medicanes are mesoscale tropical-like cyclones that develop in the Mediterranean basin and represent a great hazard for the coastal population. The skill to accurately simulate them is of utmost importance to prevent economical and personal damage. Medicanes are fueled by the latent heat released in the condensation process associated with convective activity, which is regulated by the presence and

We derived two observation-based global monthly mean dust aerosol optical depth (DAOD) climatological datasets from 2007 to 2019 with a 2∘ (latitude) × 5∘ (longitude) spatial resolution, one based on Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and the other on Moderate Resolution Imaging Spectroradiometer (MODIS) observations. In addition, the CALIOP climatological dataset also includes

Explosive volcanic eruptions influence near-surface temperature and precipitation especially in the monsoon regions, but the impact varies with different eruption seasons and latitudes. To study this variability, two groups of ensemble simulations are performed with volcanic eruptions in June and December at 0∘ representing an equatorial eruption (EQ) and at 30∘ N and 30∘ S representing Northern and

Reaction of stabilized Criegee intermediates (SCIs) with SO2 was proposed as an additional pathway of gaseous sulfuric acid (H2SO4) formation in the atmosphere, supplementary to the conventional mechanism of H2SO4 production by oxidation of SO2 in reaction with OH radicals. However, because of a large uncertainty in mechanism and rate coefficients for the atmospheric formation and loss reactions of

Abstract. By synthesising remote-sensing measurements made in the central Arctic into a model-gridded Cloudnet cloud product, we evaluate how well the Met Office Unified Model (UM) and European Centre for Medium-Range Weather Forecasting Integrated Forecasting System (IFS) capture Arctic clouds and their associated interactions with the surface energy balance and the thermodynamic structure of the

Abstract. Aerosol-cloud-precipitation interactions (ACIs) provide the greatest source of uncertainties in predicting changes in Earth’s energy budget due to poor representation of marine stratocumulus and the associated ACIs in climate models. Using in situ data from 329 cloud profiles across 24 research flights from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field

Abstract. This study investigates how the enhanced loading of microphysically and radiatively active aerosol particles impacts tropical sea breeze convection and whether these aerosol impacts are modulated by the multitudinous environments that support these cloud systems. To achieve these goals, we have performed two large numerical model ensembles, each comprised of 130 idealised simulations that

Abstract. From 23 January to 13 February 2020, twenty ATR-42 scientific flights were conducted in the framework of the EUREC4A field campaign over the tropical Atlantic, off the coast of Barbados (−58°30' W 13°30' N). By means of a side-pointing lidar, these flights allowed to retrieve the optical properties of the aerosols found in the sub-cloud layer and below the trade winds inversion. Two distinct

Abstract. In 2019/2020, Australia experienced its largest wildfire season on record. Smoke covered hundreds of square kilometers across the southeastern coast and reached the site of the 2020 COALA (Characterizing Organics and Aerosol Loading over Australia) field campaign in New South Wales. Using a subset of nighttime observations made by a proton-transfer-reaction time-of-flight mass spectrometer

Abstract. New particle formation (NPF), referring to the nucleation of molecular clusters and their subsequent growth into the cloud condensation nuclei (CCN) size range, is a globally significant and climate-relevant source of atmospheric aerosols. Classical NPF exhibiting continuous growth from a few nanometers to the Aitken mode around 60–70 nm is widely observed in the planetary boundary layer

While much research has been devoted to the subject of gaseous elemental mercury (GEM) and gaseous oxidized mercury (GOM) in the Arctic spring during atmospheric mercury depletion events, few studies have examined the behavior of GOM in the High Arctic summer. GOM, once deposited and incorporated into the ecosystem, can pose a threat to human and wildlife health, though there remain large uncertainties

The evolving nature of the COVID-19 pandemic necessitates timely estimates of the resultant perturbations to anthropogenic emissions. Here we present a novel framework based on the relationships between observed column abundance and wind speed to rapidly estimate the air-basin-scale NOx emission rate and apply it at the Po Valley in Italy using OMI and TROPOMI NO2 tropospheric column observations.

Abstract. An ensemble-variational inversion system is developed for the estimation of ammonia emissions using ammonia retrievals from the Cross-track Infrared Sounder (CrIS) for use in the Global Environmental Multiscale – Modelling Air quality and Chemistry (GEM-MACH) chemical weather model. A novel hybrid method to compare logarithmic retrieval parameters to model profiles is presented. Inversions

Abstract. Coordinated control of fine particulate matter (PM2.5) and ozone (O3) has become a new and urgent issue for China’s air pollution control. Biogenic volatile organic compounds (BVOCs) are important precursors of O3 and secondary organic aerosol (SOA) formation. China experienced a rapid increase in BVOC emissions as a result of increased vegetation biomass. We applied WRF-Chem3.8 coupling

Abstract. Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic, i.e. natural sources of aerosols

Using a Bayesian framework in the inverse problem of estimating the source of an atmospheric release of a pollutant has proven fruitful in recent years. Through Markov chain Monte Carlo (MCMC) algorithms, the statistical distribution of the release parameters such as the location, the duration, and the magnitude as well as error covariances can be sampled so as to get a complete characterisation of

Although the anthropogenic emissions of SO2 have decreased significantly in China, the decrease in SO42- in PM2.5 is much smaller than that of SO2. This implies an enhanced formation rate of SO42- in the ambient air, and the mechanism is still under debate. This work investigated the formation mechanism of particulate sulfate based on statistical analysis of long-term observations in Shijiazhuang and

Abstract. This paper concerns an in-depth analysis of an exceptional incursion of mineral dust over Southern Europe in late March 2020. This event was associated with an anomalous circulation pattern leading to several days of PM10 exceedances in connection with a dust source located in Central Asia a rare source of dust for Europe, more frequently affected by dust outbreaks from the Sahara desert

Cities represent a large and concentrated portion of global greenhouse gas emissions, including methane. Quantifying methane emissions from urban areas is difficult, and inventories made using bottom-up accounting methods often differ greatly from top-down estimates generated from atmospheric observations. Emissions from leaks in natural gas infrastructure are difficult to predict and are therefore

The formation, properties, and lifetime of secondary organic aerosols in the atmosphere are largely determined by gas–particle partitioning coefficients of the participating organic vapours. Since these coefficients are often difficult to measure and to compute, we developed a machine learning model to predict them given molecular structure as input. Our data-driven approach is based on the dataset

Biomass burning (BB) and coal combustion (CC) are important sources of brown carbon (BrC) in ambient aerosols. In this study, six biomass materials and five types of coal were combusted to generate fine smoke particles. The BrC fractions, including water-soluble organic carbon (WSOC), humic-like substance carbon (HULIS-C), and methanol-soluble organic carbon (MSOC), were subsequently fractionated,