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A new climatology of stratospheric BrO profiles based on a parameterization using dynamical and chemical indicators has been developed, with the aim to apply it to the retrieval of tropospheric BrO columns from space nadir measurements. The adopted parameterization is based on three years of output data from the 3-D chemistry transport model BASCOE. The impact of the atmospheric dynamics on the stratospheric BrO distribution is treated by means of Bry/ozone correlations built from 3-D-CTM model results, while photochemical effects are taken into account using stratospheric NO2 columns as an indicator of the BrO/Bry ratio. The model simulations have been optimized for bromine chemistry and budget, and validated through comparisons using an extensive data set of ground-based, balloon-borne and satellite limb (SCIAMACHY) stratospheric BrO observations. [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]

Given the urgency to decarbonize global energy systems, governments and industry are moving ahead with efforts to increase deployment of hydrogen technologies, infrastructure, and applications at an unprecedented pace, including USD billions in national incentives and direct investments. While zero- and low-carbon hydrogen hold great promise to help solve some of the world's most pressing energy challenges, hydrogen is also an indirect greenhouse gas whose warming impact is both widely overlooked and underestimated. This is largely because hydrogen's atmospheric warming effects are short-lived – lasting only a couple decades – but standard methods for characterizing climate impacts of gases consider only the long-term effect from a one-time pulse of emissions. For gases whose impacts are short-lived, like hydrogen, this long-term framing masks a much stronger warming potency in the near to medium term. This is of concern because hydrogen is a small molecule known to easily leak into the atmosphere, and the total amount of emissions (e.g., leakage, venting, and purging) from existing hydrogen systems is unknown. Therefore, the effectiveness of hydrogen as a decarbonization strategy, especially over timescales of several decades, remains unclear. This paper evaluates the climate consequences of hydrogen emissions over all timescales by employing already published data to assess its potency as a climate forcer, evaluate the net warming impacts from replacing fossil fuel technologies with their clean hydrogen alternatives, and estimate temperature responses to projected levels of hydrogen demand. We use the standard global warming potential metric, given its acceptance to stakeholders, and incorporate newly published equations that more fully capture hydrogen's several indirect effects, but we consider the effects of constant rather than pulse emissions over multiple time horizons. We account for a plausible range of hydrogen emission rates and include methane emissions when hydrogen is produced via natural gas with carbon capture, usage, and storage (CCUS) ("blue" hydrogen) as opposed to renewables and water ("green" hydrogen). For the first time, we show the strong timescale dependence when evaluating the climate change mitigation potential of clean hydrogen alternatives, with the emission rate determining the scale of climate benefits or disbenefits. For example, green hydrogen applications with higher-end emission rates (10 %) may only cut climate impacts from fossil fuel technologies in half over the first 2 decades, which is far from the common perception that green hydrogen energy systems are climate neutral. However, over a 100-year period, climate impacts could be reduced by around 80 %. On the other hand, lower-end emissions (1 %) could yield limited impacts on the climate over all timescales. For blue hydrogen, associated methane emissions can make hydrogen applications worse for the climate than fossil fuel technologies for several decades if emissions are high for both gases; however, blue hydrogen yields climate benefits over a 100-year period. While more work is needed to evaluate the warming impact of hydrogen emissions for specific end-use cases and value-chain pathways, it is clear that hydrogen emissions matter for the climate and warrant further attention from scientists, industry, and governments. This is critical to informing where and how to deploy hydrogen effectively in the emerging decarbonized global economy. [ABSTRACT FROM AUTHOR]

The Nordic Centre of Excellence CRAICC (Cryosphere–Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011–2016, is the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual centre with the objectives of identifying and quantifying the major processes controlling Arctic warming and related feedback mechanisms, outlining strategies to mitigate Arctic warming, and developing Nordic Earth system modelling with a focus on short-lived climate forcers (SLCFs), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special issue of the journal Atmospheric Chemistry and Physics. This paper presents an overview of the main scientific topics investigated in the centre and provides the reader with a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Faced with a vast amount of scientific discovery, we do not claim to completely summarize the results from CRAICC within this paper, but rather concentrate here on the main results which are related to feedback loops in climate change–cryosphere interactions that affect Arctic amplification. [ABSTRACT FROM AUTHOR]

Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, the relative contributions of the world's major source regions to the global dust cycle remain poorly constrained. This problem hinders accounting for the potentially large impact of regional differences in dust properties on clouds, the Earth's energy balance, and terrestrial and marine biogeochemical cycles. Here, we constrain the contribution of each of the world's main dust source regions to the global dust cycle. We use an analytical framework that integrates an ensemble of global aerosol model simulations with observationally informed constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth (DAOD). We obtain a dataset that constrains the relative contribution of nine major source regions to size-resolved dust emission, atmospheric loading, DAOD, concentration, and deposition flux. We find that the 22–29 Tg (1 standard error range) global loading of dust with a geometric diameter up to 20 µ m is partitioned as follows: North African source regions contribute ∼ 50 % (11–15 Tg), Asian source regions contribute ∼ 40 % (8–13 Tg), and North American and Southern Hemisphere regions contribute ∼ 10 % (1.8–3.2 Tg). These results suggest that current models on average overestimate the contribution of North African sources to atmospheric dust loading at ∼ 65 %, while underestimating the contribution of Asian dust at ∼ 30 %. Our results further show that each source region's dust loading peaks in local spring and summer, which is partially driven by increased dust lifetime in those seasons. We also quantify the dust deposition flux to the Amazon rainforest to be ∼ 10 Tg yr -1 , which is a factor of 2–3 less than inferred from satellite data by previous work that likely overestimated dust deposition by underestimating the dust mass extinction efficiency. The data obtained in this paper can be used to obtain improved constraints on dust impacts on clouds, climate, biogeochemical cycles, and other parts of the Earth system. [ABSTRACT FROM AUTHOR]

According to current estimates, atmospheric new particle formation (NPF) produces a large fraction of aerosol particles and cloud condensation nuclei in the Earth's atmosphere, which have implications for health and climate. Despite recent advances, atmospheric NPF is still insufficiently understood in the lower troposphere, especially above the mixed layer (ML). This paper presents new results from co-located airborne and ground-based measurements in a boreal forest environment, showing that many NPF events (∼42 %) appear to start in the topmost part of the residual layer (RL). The freshly formed particles may be entrained into the growing mixed layer (ML) where they continue to grow in size, similar to the aerosol particles formed within the ML. The results suggest that in the boreal forest environment, NPF in the upper RL has an important contribution to the aerosol load in the boundary layer (BL). [ABSTRACT FROM AUTHOR]

Atmospheric inversions have been used for the past two decades to derive large-scale constraints on the sources and sinks of CO2 into the atmosphere. The development of dense in situ surface observation networks, such as ICOS in Europe, enables in theory inversions at a resolution close to the country scale in Europe. This has led to the development of many regional inversion systems capable of assimilating these high-resolution data, in Europe and elsewhere. The EUROCOM (European atmospheric transport inversion comparison) project is a collaboration between seven European research institutes, which aims at producing a collective assessment of the net carbon flux between the terrestrial ecosystems and the atmosphere in Europe for the period 2006–2015. It aims in particular at investigating the capacity of the inversions to deliver consistent flux estimates from the country scale up to the continental scale. The project participants were provided with a common database of in situ-observed CO2 concentrations (including the observation sites that are now part of the ICOS network) and were tasked with providing their best estimate of the net terrestrial carbon flux for that period, and for a large domain covering the entire European Union. The inversion systems differ by the transport model, the inversion approach, and the choice of observation and prior constraints, enabling us to widely explore the space of uncertainties. This paper describes the intercomparison protocol and the participating systems, and it presents the first results from a reference set of inversions, at the continental scale and in four large regions. At the continental scale, the regional inversions support the assumption that European ecosystems are a relatively small sink (-0.21±0.2 Pg C yr -1). We find that the convergence of the regional inversions at this scale is not better than that obtained in state-of-the-art global inversions. However, more robust results are obtained for sub-regions within Europe, and in these areas with dense observational coverage, the objective of delivering robust country-scale flux estimates appears achievable in the near future. [ABSTRACT FROM AUTHOR]

The interactions that occur between aerosols and a mixed-phase cloud system, and the subsequent alteration of the microphysical state of such clouds, are a problem that has yet to be well constrained. Advancing our understanding of aerosol--ice processes is necessary to determine the impact of natural and anthropogenic emissions on Earth's climate and to improve our capability to predict future climate states. This paper deals specifically with how aerosols influence ice mass production in low-level Arctic mixed-phase clouds. In this study, a 9-year record of aerosol, cloud and atmospheric state properties is used to quantify aerosol influence on ice production in mixed-phase clouds. It is found that mixed-phase clouds present in a clean aerosol state have higher ice water content (IWC) by a factor of 1.22 to 1.63 at cloud base than do similar clouds in cases with higher aerosol loading. We additionally analyze radar-derived mean Doppler velocities to better understand the drivers behind this relationship, and we conclude that aerosol induced reduction of the ice crystal nucleation rate, together with decreased riming rates in polluted clouds, are likely influences on the observed reductions in IWC. [ABSTRACT FROM AUTHOR]

Understanding the role atmospheric aerosols play in the Earth-atmosphere system is limited by uncertainties in the knowledge of their distribution, composition and sources. In this paper, we use the GEOS-Chem based inverse modelling framework for retrieving desert dust (DD), black carbon (BC) and organic carbon (OC) aerosol emissions simultaneously. Aerosol optical depth (AOD) and aerosol absorption optical depth (AAOD) retrieved from the multi-angular and polarimetric POLDER/PARASOL measurements generated by the GRASP algorithm (hereafter PARASOL/GRASP) have been assimilated. First, the inversion framework is validated in a series of numerical tests conducted with synthetic PARASOL-like data. These tests show that the framework allows for retrieval of the distribution and strength of aerosol emissions. The uncertainty of retrieved daily emissions in error free conditions is below 25.8% for DD, 5.9% for BC and 26.9% for OC. In addition, the BC emission retrieval is sensitive to BC refractive index, which could produce an additional factor of 1.8 differences for total BC emissions. The approach is then applied to 1 year (December 2007 to November 2008) of data over the African and Arabian Peninsula region using PARASOL/GRASP spectral AOD and AAOD at six wavelengths (443, 490, 565, 670, 865 and 1020 nm). Analysis of the resulting retrieved emissions indicates 1.8 times overestimation of the prior DD online mobilization and entrainment model. For total BC and OC, the retrieved emissions show a significant increase of 209.9%-271.8% in comparison to the prior carbonaceous aerosol emissions. The model posterior simulation with retrieved emissions shows good agreement with both the AOD and AAOD PARASOL/GRASP products used in the inversion. The fidelity of the results is evaluated by comparison of posterior simulations with measurements from AERONET that are completely independent measurements and more temporally frequent than PARASOL observations. To further test the robustness of our posterior emissions constrained using PARASOL/GRASP, the posterior emissions are implemented in the GEOS-5/GOCART model and the consistency of simulated AOD and AAOD with other independent measurements (MODIS and OMI) demonstrates promise in applying this database for modelling studies. [ABSTRACT FROM AUTHOR]

In this paper, we present ship-based Multi- Axis Differential Optical Absorption Spectroscopy (MAXDOAS) measurements of tropospheric trace gases' distribution along the Yangtze River during winter 2015. The measurements were performed along the Yangtze River between Shanghai andWuhan, covering major industrial areas in eastern China. Tropospheric vertical column densities (VCDs) of nitrogen dioxide (NO2), sulfur dioxide (SO2), and formaldehyde (HCHO) were retrieved using the air mass factor calculated by the radiative transfer model. Enhanced tropospheric NO2 and SO2 VCDs were detected over downwind areas of industrial zones over the Yangtze River. In addition, spatial distributions of atmospheric pollutants are strongly affected by meteorological conditions; i.e., positive correlations were found between concentration of pollutants and wind speed over these areas, indicating strong influence of transportation of pollutants from high-emission upwind areas along the Yangtze River. Comparison of tropospheric NO2 VCDs between ship-based MAX-DOAS and Ozone Monitoring Instrument (OMI) satellite observations shows good agreement with each other, with a Pearson correlation coefficient (R) of 0.82. In this study, the NO2 / S± ratio was used to estimate the relative contributions of industrial sources and vehicle emissions to ambient NO2 levels. Analysis results of the NO2 / SO2 ratio show a higher contribution of industrial industrial NO2 emissions in Jiangsu Province, while NO2 levels in Jiangxi and Hubei provinces are mainly related to vehicle emissions. These results indicate that different pollution control strategies should be applied in different provinces. In addition, multiple linear regression analysis of ambient carbon monoxide (CO) and odd oxygen (Ox) indicated that the primary emission and secondary formation of HCHO contribute 54.4±3.7% and 39.3±4.3% to the ambient HCHO, respectively. The largest contribution from primary emissions in winter suggested that photochemically induced secondary formation of HCHO is reduced due to lower solar irradiance in winter. Our findings provide an improved understanding of major pollution sources along the eastern part of the Yangtze River which are useful for designing specific air pollution control policies. [ABSTRACT FROM AUTHOR]

Ozonesondes reaching the tropical tropopause layer (TTL) over the west Pacific have occasionally measured layers of very low ozone concentrations - less than 15 ppbv - raising the question of how prevalent such layers are and how they are formed. In this paper, we examine aircraft measurements from the Airborne Tropical Tropopause Experiment (ATTREX), the Coordinated Airborne Studies in the Tropics (CAST) and the Convective Transport of Active Species in the Tropics (CONTRAST) experiment campaigns based in Guam in January-March 2014 for evidence of very low ozone concentrations and their relation to deep convection. The study builds on results from the ozonesonde campaign conducted from Manus Island, Papua New Guinea, as part of CAST, where ozone concentrations as low as 12 ppbv were observed between 100 and 150 hPa downwind of a deep convective complex. TTL measurements from the Global Hawk unmanned aircraft show a marked contrast between the hemispheres, with mean ozone concentrations in profiles in the Southern Hemisphere between 100 and 150 hPa of between 10.7 and 15.2 ppbv. By contrast, the mean ozone concentrations in profiles in the Northern Hemisphere were always above 15.4 ppbv and normally above 20 ppbv at these altitudes. The CAST and CONTRAST aircraft sampled the atmosphere between the surface and 120 hPa, finding very low ozone concentrations only between the surface and 700 hPa; mixing ratios as low as 7 ppbv were regularly measured in the boundary layer, whereas in the free troposphere above 200 hPa concentrations were generally well in excess of 15 ppbv. These results are consistent with uplift of almost-unmixed boundary-layer air to the TTL in deep convection. An interhemispheric difference was found in the TTL ozone concentrations, with values <15 ppbv measured extensively in the Southern Hemisphere but seldom in the Northern Hemisphere. This is consistent with a similar contrast in the lowlevel ozone between the two hemispheres found by previous measurement campaigns. Further evidence of a boundarylayer origin for the uplifted air is provided by the anticorrelation between ozone and halogenated hydrocarbons of marine origin observed by the three aircraft. [ABSTRACT FROM AUTHOR]

The escalating climate crisis requires rapid action to reduce the concentrations of atmospheric greenhouse gases and lower global surface temperatures. Methane will play a critical role in near-term warming due to its high radiative forcing and short atmospheric lifetime. Methane emissions have accelerated in recent years, and there is significant risk and uncertainty associated with the future growth in natural emissions. The largest natural sink of methane occurs through oxidation reactions with atmospheric hydroxyl and chlorine radicals. Enhanced atmospheric oxidation could be a potential approach to remove atmospheric methane. One method proposes the addition of iron salt aerosol (ISA) to the atmosphere, mimicking a natural process proposed to occur when mineral dust mixes with chloride from sea spray to form iron chlorides, which are photolyzed by sunlight to produce chlorine radicals. Under the right conditions, lofting ISA into the atmosphere could potentially reduce atmospheric methane concentrations and lower global surface temperatures. Recognizing that potential atmospheric methane removal must only be considered an additive measure – in addition to, not replacing, crucial anthropogenic greenhouse gas emission reductions and carbon dioxide removal – roadmaps can be a valuable tool to organize and streamline interdisciplinary and multifaceted research to efficiently move towards understanding whether an approach may be viable and socially acceptable or if it is nonviable and further research should be deprioritized. Here we present a 5-year research roadmap to explore whether ISA enhancement of the chlorine radical sink could be a viable and socially acceptable atmospheric methane removal approach. [ABSTRACT FROM AUTHOR]

Nitrous acid (HONO) is a key atmospheric component, acting as a major source of the hydroxyl radical (OH), the primary oxidant in the Earth's atmosphere. However, understanding its spatial and temporal variability remains a significant challenge. Recent TROPOspheric Monitoring Instrument (TROPOMI)/Sentinel-5 Precursor (S5P) ultraviolet–visible (UV–Vis) measurements of fresh fire plumes shed light on the impact of global pyrogenic HONO emissions. Here, we leverage Infrared Atmospheric Sounding Interferometer (IASI)/MetOp's global infrared satellite measurements, complementing midday TROPOMI observations with morning and evening overpasses, to detect and retrieve pyrogenic HONO in 2007–2023. Employing a sensitive detection method, we identify HONO enhancements within concentrated fire plumes worldwide. Most detections are in the Northern Hemisphere (NH) mid- and high latitudes, where intense wildfires and high injection heights favour HONO detection. IASI's nighttime measurements yield 10-fold more HONO detections than daytime measurements, emphasizing HONO 's extended lifetime in the absence of photolysis during the night. The annual detection count increases by at least 3–4 times throughout the IASI time series, mirroring the recent surge in intense wildfires at these latitudes. Additionally, we employ a neural-network-based algorithm for retrieving pyrogenic HONO total columns from IASI and compare them with TROPOMI in the same fire plumes. The results demonstrate TROPOMI's efficacy in capturing HONO enhancements in smaller fire plumes and in proximity to fire sources, while IASI's morning and evening overpasses enable HONO measurements further downwind, highlighting the survival of HONO or its secondary formation along long-range transport in smoke plumes. [ABSTRACT FROM AUTHOR]

Dry deposition of ozone (O 3) to the ocean surface and the ozonolysis of organics in the sea surface microlayer (SSML) are potential sources of volatile organic compounds (VOCs) to the marine atmosphere. We use a gas chromatography system coupled to a Vocus proton-transfer-reaction time-of-flight mass spectrometer to determine the chemical composition and product yield of select VOCs formed from ozonolysis of coastal seawater collected from Scripps Pier in La Jolla, California. Laboratory-derived results are interpreted in the context of direct VOC vertical flux measurements made at Scripps Pier. The dominant products of laboratory ozonolysis experiments and the largest non-sulfur emission fluxes measured in the field correspond to Vocus C x H y+ and C x H y O z+ ions. Gas chromatography (GC) analysis suggests that C 5 –C 11 oxygenated VOCs, primarily aldehydes, are the largest contributors to these ion signals. In the laboratory, using a flow reactor experiment, we determine a VOC yield of 0.43–0.62. In the field at Scripps Pier, we determine a maximum VOC yield of 0.04–0.06. Scaling the field and lab VOC yields for an average O 3 deposition flux and an average VOC structure results in an emission source of 10.7 to 167 Tg C yr -1 , competitive with the DMS source of approximately 20.3 Tg C yr -1. This study reveals that O 3 reactivity to dissolved organic carbon can be a significant carbon source to the marine atmosphere and warrants further investigation into the speciated VOC composition from different seawater samples and the reactivities and secondary organic aerosol (SOA) yields of these molecules in marine-relevant, low NO x conditions. [ABSTRACT FROM AUTHOR]

Atmospheric remote sounding from satellites is an essential component of the observational strategy deployed to monitor atmospheric pollution and changing composition. The IASI nadir looking thermal infrared sounder onboard MetOp will provide 15 years of global scale observations for a series of key atmospheric species, with unprecedented spatial sampling and coverage. This paper gives an overview of the instrument's capability for measuring atmospheric composition in the perspective of chemistry and air quality. The assessment is made in terms of species, accuracy and vertical information. Global distributions are presented for CO, CH4, O3 (total and tropospheric), HNO3, NH3, and volcanic SO2. Local distributions of organic species measured during fire events, such as C2H4, CH3OH, HCOOH, and PAN are also shown. For each species or process, the link is made to specialized papers in this issue. [ABSTRACT FROM AUTHOR]

The knowledge of the lightning-induced nitrogen oxides (LNOx) source is important for understanding and predicting the nitrogen oxides and ozone distributions in the troposphere and their trends, the oxidising capacity of the atmosphere, and the lifetime of trace gases destroyed by reactions with OH. This knowledge is further required for the assessment of other important NOx sources, in particular from aviation emissions, the stratosphere, and from surface sources, and for understanding the possible feedback between climate changes and lightning. This paper reviews more than 3 decades of research. The review includes laboratory studies as well as surface, airborne and satellite-based observations of lightning and of NOx and related species in the atmosphere. Relevant data available from measurements in regions with strong LNOx influence are identified, including recent observations at midlatitudes and over tropical continents where most lightning occurs. Various methods to model LNOx at cloud scales or globally are described. Previous estimates are re-evaluated using the global annual mean flash frequency of 44±5 s-1 reported from OTD satellite data. From the review, mainly of airborne measurements near thunderstorms and cloud-resolving models, we conclude that a "typical" thunderstorm flash produces 15 (2-40)x1025 NO molecules per flash, equivalent to 250 mol NOx or 3.5 kg of N mass per flash with uncertainty factor from 0.13 to 2.7. Mainly as a result of global model studies for various LNOx parameterisations tested with related observations, the best estimate of the annual global LNOx nitrogen mass source and its uncertainty range is (5±3) Tg a-1 in this study. In spite of a smaller global flash rate, the best estimate is essentially the same as in some earlier reviews, implying larger flash-specific NOx emissions. The paper estimates the LNOx accuracy required for various applications and lays out strategies for improving estimates in the future. An accuracy of about 1 Tg a-1 or 20%, as necessary in particular for understanding tropical tropospheric chemistry, is still a challenging goal. [ABSTRACT FROM AUTHOR]

This paper discusses the highlights of the EU-funded "Assimilation of Envisat data" (ASSET) project, which has involved assimilation of Envisat atmospheric constituent and temperature data into systems based on Numerical Weather Prediction (NWP) models and chemical transport models (CTMs). Envisat was launched in 2002 and is one of the largest Earth Observation (EO) satellites ever built. It carries several sophisticated EO instruments providing in-sights into chemistry and dynamics of the atmosphere. In this paper we focus on the assimilation of temperature and constituents from Envisat. The overarching theme of the ASSET project has been to bring together experts from all aspects of the data assimilation problem. This has allowed ASSET to address several themes comprehensively: enhancement of NWP analyses by assimilation of research satellite data; studies of the distribution of stratospheric chemical species by assimilation of research satellite data into CTM systems; objective assessment of the quality of ozone analyses; studies of the spatial and temporal evolution of tropospheric pollutants; enhanced retrievals of Envisat data; and data archival and dissemination. [ABSTRACT FROM AUTHOR]

Previous studies have presented clear evidence that the Northern Hemisphere total ozone field can be separated into distinct regimes (tropical, midlatitude, polar, and arctic) the boundaries of which are associated with the subtropical and polar upper troposphere fronts, and in the winter, the polar vortex. This paper presents a study of total ozone variability within these regimes, from 1979-2003, using data from the TOMS instruments. The change in ozone within each regime for the period January 1979-May 1991, a period of rapid total ozone change, was studied in detail. Previous studies had observed a zonal linear trend of -3.15% per decade for the latitude band 25°-60° N. When the ozone field is separated by regime, linear trends of -1.4%, 2.3%, and 3.0%, per decade for the tropical, midlatitude, and polar regimes, respectively, are observed. The changes in the relative areas of the regimes were also derived from the ozone data. The relative area of the polar regime decreased by about 20%; the tropical regime increased by about 10% over this period. No significant change was detected for the midlatitude regime. From the trends in the relative area and total ozone it is deduced that 35% of the trend between 25° and 60° N, from January 1979-May 1991 is due to movement of the upper troposphere fronts. The changes in the relative areas can be associated with a change in the mean latitude of the subtropical and polar fronts within the latitude interval 25° to 60° N. Over the period from January 1979 to May 1991, both fronts moved northward by 1.1±0.2 degrees per decade. Over the entire period of the study, 1979-2003, the subtropical front moved northward at a rate of 1.1± 0.1 degrees per decade, while the polar front moved by 0.5±0.1 degrees per decade. [ABSTRACT FROM AUTHOR]

The MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) instrument has been operating on-board the ENVISAT satellite since March 2002. In the first two years, it acquired in a nearly continuous manner high resolution (0.025 cm-1 unapodized) emission spectra of the Earth's atmosphere at limb in the middle infrared region. This paper describes the level 2 near real-time (NRT) and offline (OL) ESA processors that have been used to derive level 2 geophysical products from the calibrated and geolocated level 1b spectra. The design of the code and the analysis methodology have been driven by the requirements for NRT processing. This paper reviews the performance of the optimized retrieval strategy that has been implemented to achieve these requirements and provides estimated error budgets for the target products: pressure, temperature, O3, H2O, CH4, HNO3, N2O and NO2, in the altitude measurement range from 6 to 68 km. From application to real MIPAS data, it was found that no change was needed in the developed code although an external algorithm was introduced to identify clouds with high opacity and to exclude affected spectra from the analysis. In addition, a number of updates were made to the set-up parameters and to auxiliary data. In particular, a new version of the MIPAS dedicated spectroscopic database was used and, in the OL analysis, the retrieval range was extended to reduce errors due to uncertainties in extrapolation of the profile outside the retrieval range and more stringent convergence criteria were implemented. A statistical analysis on the x² values obtained in one year of measurements shows good agreement with the a priori estimate of the forward model errors. On the basis of the first two years of MIPAS measurements the estimates of the forward model and instrument errors are in general found to be conservative with excellent performance demonstrated for frequency calibration. It is noted that the total retrieval error is limited by forward model errors which make effectless a further reduction of random errors. However, such a reduction is within the capabilities of MIPAS measurements, which contain many more spectral signatures of the target species than what has currently been used. Further work is needed to reduce the amplitude of the forward model errors, so that the random error and the total error budget can be reduced accordingly. The importance of the Averaging kernels for a full characterization of the target products is underlined and the equations are provided for their practical applications. [ABSTRACT FROM AUTHOR]

A high-order modelling approach to interpret "continental-type" particle formation bursts in the anthropogenically influenced convective boundary layer (CBL) is proposed. The model considers third-order closure for planetary boundary layer turbulence, sulphur and ammonia chemistry as well as aerosol dynamics. In Paper I of four papers, previous observations of ultrafine particle evolution are reviewed, model equations are derived, the model setup for a conceptual study on binary and ternary homogeneous nucleation is defined and shortcomings of process parameterisation are discussed. In the subsequent Papers II, III and IV simulation results, obtained within the framework of a conceptual study on the CBL evolution and new particle formation (NPF), will be presented and compared with observational findings. [ABSTRACT FROM AUTHOR]

In spite of impressive advances in recent years, our present understanding of organic aerosol (OA) composition, physical and chemical properties, sources and transformation characteristics is still rather limited, and their environmental effects remain highly uncertain. This paper discusses and prioritizes issues related to organic aerosols and their effects on atmospheric processes and climate, providing a basis for future activities in the field. Four main topical areas are addressed: i) sources of OA; ii) formation transformation and removal of OA; iii) physical, chemical and mixing state of OA; iv) atmospheric modelling of OA. Key questions and research priorities regarding these four areas are synthesized in this paper, and outstanding issues for future research are presented for each topical area. In addition, an effort is made to formulate a basic set of consistent and universally applicable terms and definitions for coherent description of atmospheric OA across different scales and disciplines. [ABSTRACT FROM AUTHOR]

In the past, differential optical absorption spectroscopy (DOAS) has mostly been employed for atmospheric trace gas retrieval in the UV/Vis spectral region. New spectrometers such as SCIAMACHY onboard ENVISAT also provide near infrared channels and thus allow for the detection of greenhouse gases like CH4, CO2, or N2O. However, modifications of the classical DOAS algorithm are necessary to account for the idiosyncrasies of this spectral region, i.e. the temperature and pressure dependence of the high resolution absorption lines. Furthermore, understanding the sensitivity of the measurement of these high resolution, strong absorption lines by means of a non-ideal device, i.e. having finite spectral resolution, is of special importance. This applies not only in the NIR, but can also prove to be an issue for the UV/Vis spectral region. This paper presents a modified iterative maximum a posteriori-DOAS (IMAP-DOAS) algorithm based on optimal estimation theory introduced to the remote sensing community by Rodgers (1976). This method directly iterates the vertical column densities of the absorbers of interest until the modeled total optical density fits the measurement. Although the discussion in this paper lays emphasis on satellite retrieval, the basic principles of the algorithm also hold for arbitrary measurement geometries. This new approach is applied to modeled spectra based on a comprehensive set of atmospheric temperature and pressure profiles. This analysis reveals that the sensitivity of measurement strongly depends on the prevailing pressure-height. The IMAP-DOAS algorithm properly accounts for the sensitivity of measurement on pressure due to pressure broadening of the absorption lines. Thus, biases in the retrieved vertical columns thaet would arise in classical algorithms, are obviated. Here, we analyse and quantify these systematic biases as well as errors due to variations in the temperature and pressure profiles, which is indispensable for the understanding of measurement precision and accuracy in the near infrared as well as for future intercomparisons of retrieval algorithms. [ABSTRACT FROM AUTHOR]

The measurement of atmospheric concentrations by a monitoring network is a promising tool for the identification of the widespread sources of trace species. The paper addresses the case of the species scattered linearly by a known meteorology. The question is classical: what can be said about the source from a set of measurements? Is it possible to guess from the values observed by the measurements that the source is spread close to the detectors, or that the tracer comes from a remote region? And, if the source was a point source, would it be possible to understand it by just considering these values? A part of the answers is a matter of practical sense: the resolution with which an emission can be retrieved will always be limited and probably lower for a remote region, even if the detectors and dispersion model are error free. The paper proposes a linear strategy of inference: to any set of values taken by the observed concentrations is associated linearly an estimate of the source. Doubled values lead to a doubled estimate. The method, based on adjoint techniques, is intended to optimise the resolution by quantifying, with the concept of illumination, which regions are well, poorly or not seen at all. The illumination tied to ordinary adjoint functions becomes excessive close to the detectors thus leading to inversion artefacts. This may be corrected by attributing each point of the space time domain a geometric and statistical weight. The adjoint functions are transformed. The choice of this renormalising function is constrained by an unambiguous entropic criterion preventing any overestimation of the available information that would lead to artefacts. It amounts to evenly distribute the information between the points organised with their weights as a "known domain". The theory is illustrated by calculations performed with the experimental source ETEX1. [ABSTRACT FROM AUTHOR]

Biogenic volatile organic compounds (BVOCs) are continuously emitted from terrestrial vegetation into the atmosphere and react with various atmospheric oxidants, with ozone being an important one. The reaction between BVOCs and ozone can lead to low volatile organic compounds, other pollutants, and the formation of secondary organic aerosols. To understand the chemical and physical processes taking place in the atmosphere, a complete picture of the BVOCs emitted is necessary. However, the large pool of BVOCs present makes it difficult to detect every compound. The total ozone reactivity method can help understand the ozone reactive potential of all BVOCs emitted into the atmosphere and also help determine whether current analytical techniques can measure the total BVOC budget. In this study, we measured the total ozone reactivity of emissions (TOZRE) from a Norway spruce tree in Hyytiälä in late summer using the total ozone reactivity monitor (TORM) built at the Finnish Meteorological Institute (FMI). Additionally, we conducted comprehensive chemical characterisation and quantification of BVOC emissions using a gas chromatograph coupled with a mass spectrometer (GC–MS), enabling us to estimate the calculated reactivity of emissions (COZRE). TOZRE reached up to 7.4×10-9 m 3 s -2 g -1 , which corresponds to 65 µ g g -1 h -1 of α -pinene. Stress-related sesquiterpenes, such as β -farnesene and α -farnesene, and an unidentified sesquiterpene contributed the most to the observed emissions. However, COZRE made up only 35 % of the TOZRE, with sesquiterpenes being the most important sink for ozone. High TOZRE values were especially seen during high-temperature periods, with up to 95 % of TOZRE remaining unexplained. Emissions of unidentified stress-related compounds could be the reason for the high fraction of missing reactivity. [ABSTRACT FROM AUTHOR]

Tropical deep convective clouds, particularly their large cirrus outflows, play an important role in modulating the energy balance of the Earth's atmosphere. Whilst the cores of these deep convective clouds have a significant short-wave (SW) cooling effect, they dissipate quickly. Conversely, the thin cirrus that flow from these cores can persist for days after the core has dissipated, reaching hundreds of kilometres in extent. These thin cirrus have a potential for large warming in the tropics. Understanding the evolution of air parcels from deep convection, clouds along these trajectories, and how they change in response to anthropogenic emissions is therefore important to understand past and future climate change. This work uses a novel approach to investigate the evolution of tropical convective clouds by introducing the concept of "time since convection" (TSC). This is used to build a composite picture of the lifecycle of air parcels from deep convection. Cloud properties are a strong function of TSC, showing decreases in the optical thickness, cloud-top height, and cloud fraction over time, thereby driving the latitudinal structure of cloudiness. After an initial dissipation of the convective core, changes in thin cirrus cloud amount were seen beyond 200 h from convection. Changes in cloud are shown to be a strong function of TSC and not simply reflective of latitudinal changes as air moves from the tropics to the extratropics. Finally, in the initial stages of convection there was a large net negative cloud radiative effect (CRE). However, once the convective core had dissipated, the sign of the CRE flipped and there was a sustained net warming CRE beyond 120 h from the convective event. Changes are present in the cloud properties long after the main convective activities have dissipated, signalling the need to continue further analysis at longer timescales than previously studied. [ABSTRACT FROM AUTHOR]

Hydrogen is expected to play a key role in the global energy transition to net zero emissions in many scenarios. However, fugitive emissions of hydrogen into the atmosphere during its production, storage, distribution and use could reduce the climate benefit and also have implications for air quality. Here, we explore the atmospheric composition and climate impacts of increases in atmospheric hydrogen abundance using the UK Earth System Model (UKESM1) chemistry–climate model. Increases in hydrogen result in increases in methane, tropospheric ozone and stratospheric water vapour, resulting in a positive radiative forcing. However, some of the impacts of hydrogen leakage are partially offset by potential reductions in emissions of methane, carbon monoxide, nitrogen oxides and volatile organic compounds from the consumption of fossil fuels. We derive a refined methodology for determining indirect global warming potentials (GWPs) from parameters derived from steady-state simulations, which is applicable to both shorter-lived species and those with intermediate and longer lifetimes, such as hydrogen. Using this methodology, we determine a 100-year global warming potential for hydrogen of 12 ± 6. Based on this GWP and hydrogen leakage rates of 1 % and 10 %, we find that hydrogen leakage offsets approximately 0.4 % and 4 % respectively of total equivalent CO 2 emission reductions in our global hydrogen economy scenario. To maximise the benefit of hydrogen as an energy source, emissions associated with hydrogen leakage and emissions of the ozone precursor gases need to be minimised. [ABSTRACT FROM AUTHOR]

Observations collected during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) provide a detailed description of the impact of thermodynamic and kinematic forcings on atmospheric boundary layer (ABL) stability in the central Arctic. This study reveals that the Arctic ABL is stable and near-neutral with similar frequencies, and strong stability is the most persistent of all stability regimes. MOSAiC radiosonde observations, in conjunction with observations from additional measurement platforms, including a 10 m meteorological tower, ceilometer, microwave radiometer, and radiation station, provide insight into the relationships between atmospheric stability and various atmospheric thermodynamic and kinematic forcings of ABL turbulence and how these relationships differ by season. We found that stronger stability largely occurs in low-wind (i.e., wind speeds are slow), low-radiation (i.e., surface radiative fluxes are minimal) environments; a very shallow mixed ABL forms in low-wind, high-radiation environments; weak stability occurs in high-wind, moderate-radiation environments; and a near-neutral ABL forms in high-wind, high-radiation environments. Surface pressure (a proxy for synoptic staging) partially explains the observed wind speeds for different stability regimes. Cloud frequency and atmospheric moisture contribute to the observed surface radiation budget. Unique to summer, stronger stability may also form when moist air is advected from over the warmer open ocean to over the colder sea ice surface, which decouples the colder near-surface atmosphere from the advected layer, and is identifiable through observations of fog and atmospheric moisture. [ABSTRACT FROM AUTHOR]

Solar coronal mass ejections can accelerate charged particles, mostly protons, to high energies, causing solar proton events (SPEs). Such energetic particles can precipitate upon the Earth's atmosphere, mostly in polar regions because of geomagnetic shielding. Here, SPE-induced chlorine activation due to ion chemistry can occur, and the activated chlorine depletes ozone in the polar middle atmosphere. We use the state-of-the-art 1D stacked-box Exoplanetary Terrestrial Ion Chemistry (ExoTIC) model of atmospheric ion and neutral composition to investigate such events in the Northern Hemisphere (NH). The Halloween SPE that occurred in late October 2003 is used as a test field for our study. This event has been extensively studied before using different 3D models and satellite observations. Our main purpose is to use such a large event that has been recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on the Environmental Satellite (ENVISAT) to evaluate the performance of the ion chemistry model. Sensitivity tests were carried out for different model settings with a focus on the chlorine species of HOCl and ClONO 2 as well as O 3 and reactive nitrogen, NO y. The model simulations were performed in the Northern Hemisphere at a high latitude of 67.5 ∘ N, inside the polar cap. Comparison of the simulated effects against MIPAS observations for the Halloween SPE revealed rather good temporal agreement, also in terms of altitude range for HOCl, O 3 and NO y. For ClONO 2 , good agreement was found in terms of altitude range. The model showed ClONO 2 enhancements after the peak of the event. The best model setting was the one with full ion chemistry where O(1 D) was set to photo-chemical equilibrium. HOCl and ozone changes are very well reproduced by the model, especially for nighttime. HOCl was found to be the main active chlorine species under nighttime conditions, resulting in an increase of more than 0.2 ppbv. Further, ClONO 2 enhancements of 0.2–0.3 ppbv have been observed during both daytime and nighttime. Model settings that compared best with MIPAS observations were applied to an extreme solar event that occurred in AD 775, presumably once in a 1000-year event. With the model applied to this scenario, an assessment can be made about what is to be expected at worst for the effects of a SPE on the middle atmosphere, concentrating on the effects of ion chemistry compared to crude parameterizations. Here, a systematic analysis comparing the impact of the Halloween SPE and the extreme event on the Earth's middle atmosphere is presented. As seen from the model simulations, both events were able to perturb the polar stratosphere and mesosphere with a high production of NO y and HO x. Longer-lasting and stronger stratospheric ozone loss was seen for the extreme event. A qualitative difference between the two events and a long-lasting impact on HOCl and HCl for the extreme event were found. Chlorine ion chemistry contributed to stratospheric ozone losses of 2.4 % for daytime and 10 % for nighttime during the Halloween SPE, as seen with time-dependent ionization rates applied to the model. Furthermore, while comparing the Halloween SPE and the extreme scenario, with ionization rate profiles applied just for the event day, the inclusion of chlorine ion chemistry added ozone losses of 10 % and 20 % respectively. [ABSTRACT FROM AUTHOR]

Aerosols are one of the most important pollutants in the atmosphere and have been monitored for the past few decades by remote sensing and in situ observation platforms to assess the effectiveness of government-managed reduction emission policies and assess their impact on the radiative budget of the Earth's atmosphere. In fact, aerosols can directly modulate incoming short-wave solar radiation and outgoing long-wave radiation and indirectly influence cloud formation, lifetime, and precipitation. In this study, we quantitatively evaluated long-term temporal trends and seasonal variability from a climatological point of view of the optical and microphysical properties of atmospheric particulate matter at the Universitat Politècnica de Catalunya (UPC), Barcelona, Spain, over the past 17 years, through a synergy of lidar, sun photometer, and in situ concentration measurements. Interannual temporal changes in aerosol optical and microphysical properties are evaluated through the seasonal Mann–Kendall test. Long-term trends in the optical depth of the recovered aerosol; the Ångström exponent (AE); and the concentrations of PM 10 , PM 2.5 , and PM 1 reveal that emission reduction policies implemented in the past decades were effective in improving air quality, with consistent drops in PM concentrations and optical depth of aerosols. The seasonal analysis of the 17-year average vertically resolved aerosol profiles obtained from lidar observations shows that during summer the aerosol layer can be found up to an altitude of 5 km, after a sharp decay in the first kilometer. In contrast, during the other seasons, the backscatter profiles fit a pronounced exponential decay well with a well-defined scale height. Long-range transport, especially dust outbreaks from the Sahara, is likely to occur throughout the year. During winter, the dust aerosol layers are floating above the boundary layer, while during the other seasons they can penetrate the layer. The analysis also revealed that intense, short-duration pollution events during winter, associated with dust outbreaks, have become more frequent and intense since 2016. This study sheds some light on the meteorological processes and conditions that can lead to the formation of haze and helps decision makers adopt mitigation strategies to preserve large metropolitan areas in the Mediterranean basin. [ABSTRACT FROM AUTHOR]

The influence of the Madden–Julian oscillation (MJO) on the middle atmosphere (MA) and particularly on MA temperature is of interest for both the understanding of MJO-induced teleconnections and research on the variability of the MA. We analyze statistically the connection of the MJO and the MA zonal mean temperature based on observations by the Microwave Limb Sounder (MLS) satellite instrument. We consider all eight MJO phases, different seasons and the state of the quasi-biennial oscillation (QBO). We show that MA temperature anomalies are significantly related to the MJO and its temporal development. The MJO signal in the zonal mean MA temperature is characterized by a particular spatial pattern in the MA, which we link to the interhemispheric coupling (IHC) mechanism, as a major outcome of this study. The signal with the largest magnitude is found in the polar MA during boreal winter with temperature deviations on the order of ±10K when the QBO at 50 hPa is in its easterly phase. Other atmospheric conditions and locations also exhibit temperature signals, which are, however, weaker or noisier. We also analyze the change in the temperature signal while the MJO progresses from one phase to the next. We find a gradual altitude shift in parts of the IHC pattern, which can be seen more or less clearly depending on the atmospheric conditions. The statistical link between the MJO and the MA temperature highlights illustratively the far-reaching connections across different atmospheric layers and geographical regions in the atmosphere. Additionally, it highlights close linkages of known dynamical features of the atmosphere, particularly the MJO, the IHC, the QBO and sudden stratospheric warmings (SSWs). Because of the wide coverage of atmospheric regions and included dynamical features, the results might help to further constrain the underlying dynamical mechanisms and could be used as a benchmark for the representation of atmospheric couplings on the intraseasonal timescale in atmospheric models. [ABSTRACT FROM AUTHOR]

Carbonyl sulfide (OCS), the most abundant sulfur gas in the Earth's atmosphere, is a greenhouse gas, a precursor to stratospheric sulfate aerosol, and a proxy for terrestrial CO 2 uptake. Estimates of important OCS sources and sinks still have significant uncertainties and the global budget is not considered closed. One particularly uncertain source term, the OCS production during the atmospheric oxidation of dimethyl sulfide (DMS) emitted by the oceans, is addressed by a series of experiments in the atmospheric simulation chamber SAPHIR in conditions comparable to the remote marine atmosphere. DMS oxidation was initiated with OH and/or Cl radicals and DMS, OCS, and several oxidation products and intermediates were measured, including hydroperoxymethyl thioformate (HPMTF), which was recently found to play a key role in DMS oxidation in the marine atmosphere. One important finding is that the onset of HPMTF and OCS formation occurred faster than expected from the current chemical mechanisms. In agreement with other recent studies, OCS yields between 9 % and 12 % were observed in our experiments. Such yields are substantially higher than the 0.7 % yield measured in laboratory experiments in the 1990s, which is generally used to estimate the indirect OCS source from DMS in global budget estimates. However, we do not expect the higher yields found in our experiments to directly translate into a substantially higher OCS source from DMS oxidation in the real atmosphere, where conditions are highly variable, and, as pointed out in recent work, heterogeneous HPMTF loss is expected to effectively limit OCS production via this pathway. Together with other experimental studies, our results will be helpful to further elucidate the DMS oxidation chemical mechanism and in particular the paths leading to OCS formation. [ABSTRACT FROM AUTHOR]

Atmospheric age reflects how long particles have been suspended in the atmosphere, which is closely associated with the evolution of air pollutants. Severe regional haze events occur frequently in China, influencing air quality, human health, and regional climate. Previous studies have explored the characteristics of mass concentrations and compositions of fine particulate matter (PM 2.5) during haze events, but the evolution of atmospheric age remains unclear. In this study, the age-resolved University of California, Davis/California Institute of Technology (UCD/CIT) model was developed and applied to simulate the concentration and age distribution of PM 2.5 during a severe regional haze episode in eastern China. The results indicated that PM 2.5 concentrations in the North China Plain (NCP) gradually accumulated due to stagnant weather conditions during the beginning stage of the haze event. Accordingly, the atmospheric age of elemental carbon (EC), primary organic aerosol (POA), sulfate (SO42-), and secondary organic aerosol (SOA) gradually increased. The subsequent PM 2.5 concentration growth was driven by the local chemical formation of nitrate (NO3-) under high relative humidity. The newly formed NO3- particles led to a decrease in the mean atmospheric age of NO3- particles. During the regional transport stage, aged particles from the NCP moved to the downwind Yangtze River Delta (YRD) region, leading to a sharp increase in PM 2.5 concentrations and the average age of EC, POA, SO42- , and SOA in YRD. In contrast, the average age of NO3- and ammonium remained unchanged or even slightly decreased due to continuous local formation in the YRD region. Different evolution of the atmospheric age among these components provides a unique perspective on the formation of PM 2.5 components during the regional haze event. The information can also be used for designing effective control strategies for different components of PM 2.5. [ABSTRACT FROM AUTHOR]

Global monitoring of aerosols is required to analyse the impacts of aerosols on air quality and to understand their role in modulating the climate variability. The Copernicus Atmosphere Monitoring Service (CAMS) provides near-real-time forecasts and reanalyses of aerosols using the ECMWF Integrated Forecasting System (IFS), constrained by the assimilation of MODIS and Polar Multi-Sensor Aerosol Optical Properties (PMAp) aerosol optical depth (AOD). Given the potential end of lifetime of MODIS AOD, implementing new AOD observations in the CAMS operational suite is a priority to ensure the continuity of the CAMS forecast performances. The objective of this work is to test the assimilation of the NOAA VIIRS AOD product from S-NPP and NOAA20 satellites in the IFS model. Simulation experiments assimilating VIIRS on top or in place of MODIS were carried out from June 2021 to November 2021 to evaluate the impacts on the AOD analysis. For maritime aerosol background, the assimilation of VIIRS and the use of VIIRS from NOAA20 as an anchor reduce the analysis AOD values compared to MODIS-based experiments, in which the analysis values were too high due to the positive bias of MODIS/Terra over ocean. Over land, the assimilation of VIIRS induces a large increase in the analysis over biomass burning regions where VIIRS shows larger AOD than MODIS due to differences in the aerosol models and cloud filtering between MODIS and VIIRS retrieval algorithms. For dust source regions, the analysis is reduced when VIIRS is assimilated on top of or in place of MODIS, particularly over the Sahara, the Arabian Peninsula and a few places in Asia in the July–August period. The assimilation of VIIRS leads to an overall reduction of the bias in AOD analysis evaluated against AERONET measurements, with the largest bias reduction over Europe and desert and maritime sites. [ABSTRACT FROM AUTHOR]

Cyclones are expected to increase the vertical transport of sea spray aerosols (SSAs), which may significantly impact the climate by increasing the population of cloud condensation nuclei (CCN) and the cloud droplet number concentration (Nd). In this study, a high-time-resolution (1 h) aerosol monitoring was carried out in the middle and high Southern Hemisphere from 23 February to 4 March 2018. The characteristics of SSAs during three cyclones were observed during the cruise. The results showed that SSA level in the low atmosphere did not increase with the wind speed during cyclone processes, which was different from the anticipated scenario that SSA concentration would increase with wind speed. However, the size of SSA particles during cyclones was larger than that in the no-cyclone periods. It seems that the generation of SSAs was enhanced during cyclones, but SSA concentration near the sea surface increased scarcely. The upward-transport proportion was calculated according to the wind stress and sea salt flux between cyclone and non-cyclone periods. It indicated that more than 23.4 % of the SSAs were transported upwards by cyclone processes during event 1, and 36.2 % and 38.9 % were transported upwards in event 2 and event 3, respectively. The upward transport of SSAs was the main reason why SSA concentration did not increase in the low atmosphere. The transport of SSAs to the high atmosphere during cyclones may additionally increase the CCN burden in the marine boundary layer, which may affect the regional climate. This study highlights the importance of SSA transport to the high atmosphere by cyclones and extends the knowledge of SSA generation and the impact factor during the cyclone period in marine atmosphere. [ABSTRACT FROM AUTHOR]

Current process-based research mainly uses box models to evaluate photochemical ozone production and destruction rates, and it is unclear to what extent the photochemical reaction mechanisms are elucidated. Here, we modified and improved a net photochemical ozone production rate (NPOPR, P (O 3) net) detection system based on the current dual-channel reaction chamber technique, which makes the instrument applicable to different ambient environments, and its various operating indicators were characterized, i.e., "airtightness", light transmittance, wall losses of the reaction and reference chambers, conversion rate of O 3 to NO 2 , air residence time, and performance of the reaction and reference chambers. The limits of detection of the NPOPR detection system were determined to be 0.07, 1.4, and 2.3 ppbv h -1 at sampling flow rates of 1.3, 3, and 5 L min -1 , respectively. We further applied the NPOPR detection system to field observations at an urban site in the Pearl River Delta (China). During the observation period, the maximum value of P (O 3) net was 34.1 ppbv h -1 , which was ∼ 0 ppbv h -1 at night within the system detection error and peaked at approximately noon local time. The daytime (from 06:00–18:00 LT) average value of P (O 3) net was 12.8 (± 5.5) ppbv h -1. We investigated the detailed photochemical O 3 formation mechanism in the reaction and reference chambers of the NPOPR detection system using a zero-dimensional box model. We found that the photochemical reactions in the reaction chamber were very close to those in ambient air, but there was not zero chemistry in the reference chamber because the reaction related to the production and destruction of RO 2 (= HO 2 + RO 2) continued in the reference chamber, which led to a small amount of P (O 3) net. Therefore, the P (O 3) net measured here can be regarded as the lower limit of the real P (O 3) net in the atmosphere; however, the measured P (O 3) net was still ∼ 7.5 to 9.3 ppbv h -1 higher than the modeled P (O 3) net value depending on different modeling methods, which may be due to the inaccurate estimation of HO 2 / RO 2 radicals in the modeling study. Short-lived intermediate measurements coupled with direct P (O 3) net measurements are needed in the future to better understand O 3 photochemistry. Our results show that the NPOPR detection system can achieve high temporal resolution and continuous field observations, which helps us to better understand photochemical O 3 formation and provides a key scientific basis for continuous improvement of air quality in China. [ABSTRACT FROM AUTHOR]

Interpretation of observed diurnal carbon dioxide (CO2) mixing ratios near the surface requires knowledge of the local dynamics of the planetary boundary layer. In this paper, we study the relationship between the boundary layer dynamics and the CO2 budget in convective conditions through a newly derived set of analytical equations. From these equations, we are able to quantify how uncertainties in boundary layer dynamical variables or in the morning CO2 distribution in the mixed-layer or in the free atmosphere (FA) influence the bulk CO2 mixing ratio. We find that the largest uncertainty incurred on the midday CO2 mixing ratio comes from the prescribed early morning CO2 mixing ratios in the stable boundary layer, and in the free atmosphere. Errors in these values influence CO2 mixing ratios inversely proportional to the boundary layer depth (h), just like uncertainties in the assumed initial boundary layer depth and surface CO2 flux. The influence of uncertainties in the boundary layer depth itself is one order of magnitude smaller. If we "invert" the problem and calculate CO2 surface exchange from observed or simulated CO2 mixing ratios, the sensitivities to errors in boundary layer dynamics also invert: they become linearly proportional to the boundary layer depth. We demonstrate these relations for a typical well characterized situation at the Cabauw site in The Netherlands, and conclude that knowledge of the temperature and carbon dioxide profiles of the atmosphere in the early morning are of vital importance to correctly interpret observed CO2 mixing ratios during midday. [ABSTRACT FROM AUTHOR]

This paper presents a first statistical validation of tropospheric ozone products derived from measurements of the IASI satellite instrument. Since the end of 2006, IASI (Infrared Atmospheric Sounding Interferometer) aboard the polar orbiter Metop-A measures infrared spectra of the Earth's atmosphere in nadir geometry. This validation covers the northern mid-latitudes and the period from July 2007 to August 2008. Retrieval results from four different sources are presented: three are from scientific products (LATMOS, LISA, LPMAA) and the fourth one is the pre-operational product distributed by EUMETSAT (version 4.2). The different products are derived from different algorithms with different approaches. The difference and their implications for the retrieved products are discussed. In order to evaluate the quality and the performance of each product, comparisons with the vertical ozone concentration profiles measured by balloon sondes are performed and lead to estimates of the systematic and random errors in the IASI ozone products (profiles and partial columns). A first comparison is performed on the given profiles; a second comparison takes into account the altitude dependent sensitivity of the retrievals. Tropospheric columnar amounts are compared to the sonde for a lower tropospheric column (surface to about 6 km) and a "total" tropospheric column (surface to about 11 km). On average both tropospheric columns have small biases for the scientific products, less than 2 Dobson Units (DU) for the lower troposphere and less than 1DU for the total troposphere. The comparison of the still preoperational EUMETSAT columns shows higher mean differences of about 5 DU. [ABSTRACT FROM AUTHOR]

Bacteria are constantly being transported through the atmosphere, which may have implications for human health, agriculture, cloud formation, and the dispersal of bacterial species. We simulate the global transport of bacteria, represented as 1μm and 3μm diameter spherical solid particle tracers in a general circulation model. We investigate factors influencing residence time and distribution of the particles, including emission region, cloud condensation nucleus activity and removal by ice-phase precipitation. The global distribution depends strongly on the assumptions made about uptake into cloud droplets and ice. The transport is also affected, to a lesser extent, by the emission region, particulate diameter, and season. We find that the seasonal variation in atmospheric residence time is insufficient to explain by itself the observed seasonal variation in concentrations of particulate airborne culturable bacteria, indicating that this variability is mainly driven by seasonal variations in culturability and/or emission strength. We examine the potential for exchange of bacteria between ecosystems and obtain rough estimates of the flux from each ecosystem by using a maximum likelihood estimation technique, together with a new compilation of available observations described in a companion paper. Globally, we estimate the total emissions of bacteria-containing particles to the atmosphere to be 7.6×1023-3.5×1024 a-1, originating mainly from grasslands, shrubs and crops. We estimate the mass of emitted bacteria- to be 40-1800 Gg a-1, depending on the mass fraction of bacterial cells in the particles. In order to improve understanding of this topic, more measurements of the bacterial content of the air and of the rate of surface-atmosphere exchange of bacteria will be necessary. Future observations in wetlands, hot deserts, tundra, remote glacial and coastal regions and over oceans will be of particular interest. [ABSTRACT FROM AUTHOR]

Although the global methane (CH4) concentration has more than doubled since pre-industrial times, local emission sources are still poorly identified and quantified. Instruments onboard satellites can improve our knowledge about the methane global distribution owing to their very good spatial coverage. The IASI (Infrared Atmospheric Sounding Interferometer) instrument launched on the European MetOp-A platform is a Fourier transform spectrometer which measures the thermal infrared radiation emitted by the Earth and its atmosphere. In this paper, we present the first global distribution of methane total columns (mostly sensitive to the middle troposphere) from the IASI spectra using the methane v4 absorption band. The retrieval spectral range was set in order to minimize possible spectroscopic issues. Results are discussed in terms of error budget and vertical sensitivity. In addition, we study the gain of information on surface methane concentrations provided by using the v3 band, which is partly covered by IASI on the short-wave end of the spectra (extending to 2760 cm-1), where solar reflection contributes significantly. [ABSTRACT FROM AUTHOR]

Two 40-year meteorological datasets are used to drive the Model of Ozone and Related Tracers chemical transport model, version 2 (MOZART2) in hindcast simulations. One dataset is from the National Center for Environmental Prediction/National Center for Atmospheric Research (NCEP/NCAR) reanalysis, the second dataset uses meteorology from the Community Atmosphere Model (CAM3) forced with observed interannually varying sea surface temperatures. All emissions, except those from lightning are annually constant. Analysis of these simulations focuses on the period between 1979-1999, due to meteorological discontinuities in the NCEP reanalysis during the 1970s. The meteorology using CAM3 captures observed trends in temperature and water vapor; the simulation using NCEP meteorology does not. This paper examines the regional and global interannual variability of various chemical and meteorological fields: CO, OH, O3 and HNO3, the surface photolysis rate of NO2 (as a proxy for overhead cloudiness), lightning NO emissions, water vapor, planetary boundary layer height, and temperature. The variability due to changes in emissions is not considered in this analysis. In both the NCEP and CAM3 simulations the relative variability of CO, OH, O3 and HNO3 are qualitatively similar, with variability maxima both in the tropics and the high latitudes. Locally, relative variability generally ranges between 3 and 10%; globally the tropospheric variability generally ranges from half to one percent, but can be higher. For most fields the leading global Empirical Orthogonal Function explains approximately 10% of the variability and correlates significantly with El Niño. In both simulations the first principal component of a multiple tracer, globally averaged analysis shows a strong coupling between surface temperature, measures of the hydrological cycle, CO and OH, but is not correlated with El Niño. In both simulations we examine the global response of the selected variables to changes in global surface temperature, and compare with a climate simulation over the 21st century. [ABSTRACT FROM AUTHOR]

This paper presents results from the first detailed intercomparison of stratosphere-lower mesosphere water vapour analyses; it builds on earlier results from the EU funded framework V "Assimilation of ENVISAT Data" (ASSET) project. Stratospheric water vapour plays an important role in many key atmospheric processes and therefore an improved understanding of its daily variability is desirable. With the availability of high resolution, good quality Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) water vapour profiles, the ability of four different atmospheric models to assimilate these data is tested. MIPAS data have been assimilated over September 2003 into the models of the European Centre for Medium Range Weather Forecasts (ECMWF), the Belgian Institute for Space and Aeronomy (BIRA-IASB), the French Service d'Aéronomie (SA-IPSL) and the UK Met Office. The resultant middle atmosphere humidity analyses are compared against independent satellite data from the Halogen Occultation Experiment (HALOE), the Polar Ozone and Aerosol Measurement (POAM III) and the Stratospheric Aerosol and Gas Experiment (SAGE II). The MIPAS water vapour profiles are generally well assimilated in the ECMWF, BIRA-IASB and SA systems, producing stratosphere-mesosphere water vapour fields where the main features compare favourably with the independent observations. However, the models are less capable of assimilating the MIPAS data where water vapour values are locally extreme or in regions of strong humidity gradients, such as the southern hemisphere lower stratosphere polar vortex. Differences in the analyses can be attributed to the choice of humidity control variable, how the background error covariance matrix is generated, the model resolution and its complexity, the degree of quality control of the observations and the use of observations near the model boundaries. Due to the poor performance of the Met Office analyses the results are not included in the intercomparison, but are discussed separately. The Met Office results highlight the pitfalls in humidity assimilation, and provide lessons that should be learnt by developers of stratospheric humidity assimilation systems. In particular, they underline the importance of the background error covariances in generating a realistic troposphere to mesosphere water vapour analysis. [ABSTRACT FROM AUTHOR]

Equatorial planetary scale wave modes such as Kelvin waves or Rossby-gravity waves are excited by convective processes in the troposphere. In this paper an analysis for these and other equatorial wave modes is carried out with special focus on the stratosphere using temperature data from the SABER satellite instrument as well as ECMWF temperatures. Space-time spectra of symmetric and antisymmetric spectral power are derived to separate the different equatorial wave types and the contribution of gravity waves is determined from the spectral background of the space-time spectra. Both gravity waves and equatorial planetary scale wave modes are main drivers of the quasi-biennial oscillation (QBO) in the stratosphere. Temperature variances attributed to the different wave types are calculated for the period from February 2002 until March 2006 and compared to previous findings. A comparison between SABER and ECMWF wave analyses shows that in the lower stratosphere SABER and ECMWF spectra and temperature variances agree remarkably well while in the upper stratosphere ECMWF tends to overestimate Kelvin wave components. Gravity wave variances are partly reproduced by ECMWF but have a significant low-bias. For the examples of a QBO westerly phase (October-December 2004) and a QBO easterly phase (November/December 2005, period of the SCOUT-O3 tropical aircraft campaign in Darwin/Australia) in the lower stratosphere we find qualitatively good agreement between SABER and ECMWF in the longitude-time distribution of Kelvin, Rossby (n=1), and Rossby-gravity waves. [ABSTRACT FROM AUTHOR]

In radiative transfer simulations the simplification of cloud top structure by homogeneous assumptions can cause mistakes in comparison to realistic heterogeneous cloud top structures. This paper examines the influence of cloud top heterogeneity on the radiation at the top of the atmosphere. The use of cloud top measurements with a high temporal resolution allows the analysis of small spatial cloud top heterogeneities by using the frozen turbulence assumption for the time -- space conversion. Radiative observations are often based on satellite measurements, whereas small spatial structures are not considered in such treatments. A spectral analysis of the cloud top measurements showed slopes of power spectra between -1.8 and -2.0, these values are larger than the spectra of -5/3 which is often applied to generate cloud field variability. The comparison of 3-D radiative transfer results from cloud fields with homogeneous and heterogeneous tops has been done for a single wavelength of 0.6µm. The radiative transfer calculations result in lower albedos for heterogeneous cloud tops. The differences of albedos between heterogeneous and homogeneous cloud top decrease with increasing solar zenith angle. The influence of cloud top variability on radiances is shown. The reflectances for heterogeneous tops are explicitly larger in forward direction, in backward direction lower. The largest difference of the mean reflectances (mean over cloud field) between homogeneous and heterogeneous cloud top is approximately 0.3, which is 30% of illumination. [ABSTRACT FROM AUTHOR]

This paper gives an overview of the MIPAS Level 1B (L1B) processor whose main objective is to calibrate atmospheric measurements radiometrically, spectrally and geo-located. It presents also the results of instrument characterization done on ground and during the first years in-flight. An accurate calibration is mandatory for high quality atmospheric retrievals. MIPAS has shown very good performance and stability. The noise equivalent spectral radiance ranges from 3 to 50 nW/(cm² sr cm-1) and is well within the requirements over nearly the whole spetral range. The systematic radiometric error is estimated to be within 1 or 2% in most situations. [ABSTRACT FROM AUTHOR]

Ions, which are generated in the atmosphere by galactic cosmic rays and other ionization sources, may play an important role in the formation of atmospheric aerosols. In the paper, a new second-generation ion-mediated nucleation (IMN) model is presented. The new model explicitly treats the evaporation of neutral and charged clusters and it describes the evolution of the size spectra and composition of both charged and neutral clusters/particles ranging from small clusters of few molecules to large particles of several micrometers in diameter. Schemes used to calculate the evaporation coefficients for small neutral and charged clusters are consistent with the experimental data within the uncertainty range. The present IMN model, which is size-, composition-, and type-resolved, is a powerful tool for investigating the dominant mechanisms and key parameters controlling the formation and subsequent growth of nanoparticles in the atmosphere. This model can be used to analyze simultaneous measurements of the ion-mobility spectra and particle size distributions, which became available only recently. General features of the spectra for ions smaller than the critical size, size-dependent fractions of charged nanoparticles, and asymmetrical charging of freshly nucleated particles predicted by the new IMN model are consistent with recent measurements. Results obtained using the second generation IMN model, in which the most recent thermodynamic data for neutral and charged H2SO4-H2O clusters were used, suggest that ion-mediated nucleation of H2SO4-H2O can lead to a significant production of new particles in the lower atmosphere (including the boundary layer) under favorable conditions. It has been shown that freshly nucleated particles of few nanometers in size can grow by the condensation of low volatile organic compounds to the size of cloud condensation nuclei. In such cases, the chemical composition of nucleated particles larger than ∼10 nm is dominated by organics. [ABSTRACT FROM AUTHOR]

Ions, which are generated in the atmosphere by galactic cosmic rays and other ionization sources, may play an important role in the formation of atmospheric aerosols. In the paper, a new second-generation ion-mediated nucleation (IMN) model is presented. The new model explicitly treats the evaporation of neutral and charged clusters and it describes the evolution of the size spectra and composition of both charged and neutral clusters/particles ranging from small clusters of few molecules to large particles of several micrometers in diameter. Schemes used to calculate the evaporation coefficients for small neutral and charged clusters are consistent with the experimental data within the uncertainty range. The present IMN model, which is size-, composition-, and type-resolved, is a powerful tool for investigating the dominant mechanisms and key parameters controlling the formation and subsequent growth of nanoparticles in the atmosphere. This model can be used to analyze simultaneous measurements of the ion-mobility spectra and particle size distributions, which became available only recently. General features of the spectra for ions smaller than the critical size, size-dependent fractions of charged nanoparticles, and asymmetrical charging of freshly nucleated particles predicted by the new IMN model are consistent with recent measurements. Results obtained using the second generation IMN model, in which the most recent thermodynamic data for neutral and charged H2SO4-H2O clusters were used, suggest that ion-mediated nucleation of H2SO4H2O can lead to a significant production of new particles in the lower atmosphere (including the boundary layer) under favorable conditions. It has been shown that freshly nucleated particles of few nanometers in size can grow by the condensation of low volatile organic compounds to the size of cloud condensation nuclei. In such cases, the chemical composition of nucleated particles larger than ∼10 nm is dominated by organics. [ABSTRACT FROM AUTHOR]

Recent laboratory experiments showed that at conditions resembling those near the tropopause region, small ice particles can be coated by a liquid H2SO4/H2O over-layer formed after the freezing of diluted sulfuric acid/water aerosol drops. Here, idealized radiative transfer tests are conducted to evaluate the impact that such an over-layer would have on the radiative effects produced by sub-visible cirrus clouds (SVCs). Spherical particle shape is assumed to keep the problem tractable. The calculations show that the over-layer increases both the shortwave (SW) and longwave (LW) cloud radiative effects (CRE), but the impact is small: ∼0.02W m-2, or even less, for the total (LW+SW) CRE at the top of the atmosphere. For the smallest ice particles, for which the over-layer is thickest, the fractional change in CRE can, however, reach ∼20% for the SW CRE and over 50% for the LWCRE. The dependence of LW and SW CRE on particle size is also studied in the paper. Calculations for spherical and spheroidal uncoated ice particles show that even for high, optically thin cirrus, the total CRE can be negative, if the diameter of the particles is smaller than about 3-4µm. Apart from the SVCs, this result could be relevant for contrail cirrus clouds, which are believed to consist of large numbers of very small ice particles. [ABSTRACT FROM AUTHOR]

This paper summarizes and classifies the various approaches to validation of remote measurements of atmospheric state variables, and tries to recommend a clear and unambiguous terminology. The following approaches have been identified: Intercomparison of individual profiles for accuracy validation; statistical comparison of matched pairs of measurements with respect to bias determination and precision validation; statistical intercomparison of randomly sampled measurements by two instruments, and comparison of a single measurement to an ensemble of measurements. Applicable statistics are shortly reviewed, and recipes for evaluation of the co-incidence error due to less than perfect coincidences are presented. An approach is suggested to quantitatively validate profile measurements when full covariance matrices are unavailable. [ABSTRACT FROM AUTHOR]

This paper summarizes and classifies the various approaches to validation of remote measurements of atmospheric state variables, and tries to recommend a clear and unambiguous terminology. The following approaches have been identified: Intercomparison of individual profiles for accuracy validation; statistical comparison of matched pairs of measurements with respect to bias determination and precision validation; statistical intercomparison of randomly sampled measurements by two instruments, and comparison of a single measurement to an ensemble of measurements. Applicable statistics are shortly reviewed, and recipes for evaluation of the co-incidence error due to less than perfect coincidences are presented. An approach is suggested to quantitatively validate profile measurements when full covariance matrices are unavailable. [ABSTRACT FROM AUTHOR]