Atmospheric Chemistry Model Research Articles

Global 3D rocket launch and re-entry air pollutant and CO2 emissions at the onset of the megaconstellation era

Satellite megaconstellation (SMC) missions are spurring rapid growth in rocket launches and anthropogenic re-entries. These events inject pollutants and carbon dioxide (CO2) in all atmospheric layers, affecting climate and stratospheric ozone. Quantification of these and other environmental impacts requires reliable inventories of emissions. We present a global, hourly, 3D, multi-year inventory of air pollutant emissions and CO2 from rocket launches and object re-entries spanning the inception and growth of SMCs (2020–2022). We use multiple reliable sources to compile information needed to build the inventory and conduct rigorous and innovative cross-checks and validations against launch livestreams and past studies. Our inventory accounts for rocket plume afterburning effects, applies object-specific ablation profiles to re-entering objects, and quantifies unablated mass of objects returning to Earth. We also identify all launches and objects associated with SMC missions, accounting for 37–41% of emissions of black carbon particles, carbon monoxide, and CO2 by 2022. The data are provided in formats for ease-of-use in atmospheric chemistry and climate models to inform regulation and space sustainability policies.

Greenhouse gas column observations from a portable spectrometer in Uganda

Abstract. The extensive terrestrial ecosystems of tropical Africa are a significant store of carbon and play a key but uncertain role in the atmospheric budgets of carbon dioxide and methane. As ground-based observations in the tropics are scarce compared with other parts of the world, recent studies have instead made use of satellite observations assimilated into atmospheric chemistry and transport models to conclude that methane emissions from this geographical region have increased since 2010 as a result of increased wetland extent, accounting for up to a third of global methane growth, and that the tropical Africa region dominates net carbon emission across the tropics. These studies critically rely on the accuracy of satellite datasets, such as those from the Orbiting Carbon Observatory-2 (OCO-2), the Greenhouse gases Observing SATellite (GOSAT), and the Sentinel-5 Precursor TROPOspheric Monitoring Instrument (TROPOMI), along with results from atmospheric transport models, over a geographical region where there are little independent data to test the robustness of published results. In this paper we present the first ground-based observations of greenhouse gas column concentrations over East Africa, obtained using a portable Bruker EM27/SUN Fourier transform infrared (FTIR) spectrometer during a deployment covering the first few months of 2020 in Jinja, Uganda. We operated the instrument near autonomously by way of an automated weatherproof enclosure and observed total atmospheric column concentrations of the greenhouse gases carbon dioxide and methane, as well as carbon monoxide, a useful proxy for emissions from incomplete combustion processes in the region. We discuss the performance of the combined enclosure and spectrometer system that we deployed in Jinja to obtain these data and show comparisons of our ground-based observations with satellite datasets from OCO-2 and Orbiting Carbon Observatory-3 (OCO-3) for carbon dioxide and TROPOMI for methane and carbon monoxide, whilst also comparing our results with concentration data from the GEOS-Chem and Copernicus Atmosphere Monitoring Service (CAMS) atmospheric inversions that provide a means of increasing spatial and temporal coverage where satellite data are not available. For our measurement period, we find mean differences in XCO2 between OCO-2 and the EM27/SUN of −0.29 % and between OCO-3 and the EM27/SUN of −0.28 %. In the case of TROPOMI, the mean difference in XCH4 that we find between TROPOMI and the EM27/SUN is −0.44 %, whilst for XCO the mean difference is −5.65 %. In each of these cases, the mean difference observed between the satellite and ground-based column concentrations is either close to or within the precision and accuracy requirements for the respective missions. With regard to the model and reanalysis comparisons with the EM27/SUN column concentrations, we see mean differences from the EM27/SUN of a global GEOS-Chem inversion for XCO2 of −0.08 %, a regional high-resolution GEOS-Chem inversion for XCH4 of −0.22 %, and the CAMS global reanalysis for XCO of −9.79 %. Our results demonstrate the value of ground-based observations of total column concentrations and show that the combined EM27/SUN and enclosure system employed would be suitable for acquisition of the longer-term observations needed to rigorously evaluate satellite observations and model and reanalysis calculations over tropical Africa.

The co-benefits of a low-carbon future for PM2.5 and O3 air pollution in Europe

Abstract. There is considerable academic interest in the potential for air quality improvement as a co-benefit of climate change mitigation. Few studies use regional air quality models for simulating future co-benefits, but many use global chemistry–climate model output. Using regional atmospheric chemistry could provide a better representation of air quality changes than global chemistry–climate models, especially by improving the representation of elevated urban concentrations. We use a detailed regional atmospheric-chemistry model (WRF-Chem v4.2) to model European air quality in 2050 compared to 2014 following three climate change mitigation scenarios. We represent different climate futures by using air pollutant emissions and chemical boundary conditions (from CESM2-WACCM output) for three shared socioeconomic pathways (SSP1-2.6, SSP2-4.5 and SSP3-7.0: high-, medium- and low-mitigation pathways respectively). We find that in 2050, following SSP1-2.6, mean population-weighted PM2.5 concentrations across European countries are reduced by 52 % compared to 2014. Under SSP2-4.5, this average reduction is 34%. The smallest average reduction is 18 %, achieved following SSP3-7.0. Maximum 6-monthly-mean daily-maximum 8 h (6mDM8h) ozone (O3) is reduced across Europe by 15 % following SSP1-2.6 and by 3 % following SSP2-4.5, but it increases by 13 % following SSP3-7.0. This demonstrates clear co-benefits of climate mitigation. The additional resolution allows us to analyse regional differences and identify key sectors. We find that the mitigation of agricultural emissions will be key for attaining meaningful co-benefits of mitigation policies, as evidenced by the importance of changes in NO3 aerosol mass to future PM2.5 air quality and changes in CH4 emissions to future O3 air quality.

Diversity of ammonia sources in Tianjin: nitrogen isotope analyses and simulations of aerosol ammonium

Environmental context Atmospheric particulate NH4+, primarily produced from the reaction of NH3 and acids, is an important component of PM2.5. In this study, nitrogen stable isotope analyses and an atmospheric chemistry model were used to estimate the contribution of major NH3 sources to particulate NH4+ in Tianjin, a megacity in North China Plain (NCP). Our research has implications for investigations of NH3 emission sources and relevant pollution control in Tianjin and NCP. Rationale The North China Plain (NCP) has been identified as an NH3 emission hotspot. Source apportionment of NH3 is a prerequisite for controlling NH3 or NH4+ pollution. Nitrogen stable isotope (δ15N) analysis is a promising method for NH3 source apportionment but its accuracy is still in question. Methodology In this study, daytime and nighttime PM2.5 samples were collected from two sites in Tianjin, NCP, in autumn. Concentrations and δ15N of particulate NH4+ were then measured. Nitrogen stable isotope analyses and isotope mixing model (MixSIAR), and an atmospheric chemistry model (WRF-CMAQ-ISAM) were used to estimate the sources of NH3 in Tianjin. Results Results from the MixSIAR and WRF-CMAQ-ISAM models suggested that all the sources including livestock breeding, N-fertiliser application, fossil fuels, NH3 slip (especially from traffic), human waste and biomass burning (mostly from bioapplication) were non-negligible to NH3 and NH4+ in Tianjin. This high complexity is due to significant agricultural and industrial production and residential life in Tianjin and the surrounding regions. Our results indicate all NH3 sources need to be considered if we want to reduce NH4+ pollution in Tianjin in autumn.

Earth's Mesosphere During Possible Encounters With Massive Interstellar Clouds 2 and 7 Million Years Ago

AbstractOur solar system's path has recently been shown to potentially intersect dense interstellar clouds 2 and 7 million years ago: the Local Lynx of Cold Cloud and the edge of the Local Bubble. These clouds compressed the heliosphere, directly exposing Earth to the interstellar medium. Previous studies that examined climate effects of these encounters argued for an induced ice age due to the formation of global noctilucent clouds (NLCs). Here, we revisit such studies with a modern 2D atmospheric chemistry model using parameters of global heliospheric magnetohydrodynamic models as input. We show that NLCs remain confined to polar latitudes and short seasonal lifetimes during these dense cloud crossings lasting ∼105 years. Polar mesospheric ozone becomes significantly depleted, but the total ozone column broadly increases. Furthermore, we show that the densest NLCs lessen the amount of sunlight reaching the surface instantaneously by up to 7% while halving outgoing longwave radiation.

Substantial nitrogen abatement accompanying decarbonization suppresses terrestrial carbon sinks in China

China faces challenges in reaching its carbon neutrality goal by the year 2060 to meet the Paris Agreement and improving air quality simultaneously. Dramatic nitrogen emission reductions will be brought by this ambitious target, yet their impact on the natural ecosystem is not clear. Here, by combining two atmospheric chemistry models and two process-based terrestrial ecosystem models constrained using nationwide measurements, we show that atmospheric nitrogen deposition in China’s terrestrial land will decrease by 44–57% following two emission control scenarios including one aiming at carbon neutrality. They consequently result in a pronounced shrinkage in terrestrial net ecosystem production, by 11–20% depending on models and emission scenarios. Our results indicate that the nitrogen emission reductions accompanying decarbonization would undermine natural carbon sinks and in turn set back progress toward carbon neutrality. This unintended impact calls for great concern about the trade-offs between nitrogen management and carbon neutrality.

Reporting of gridded ammonia emission and assessment of hotspots across India: A comprehensive study of 24 anthropogenic sources

Ammonia (NH3) acts as a key precursor of the particulate matter, could reduce visibility, deplete stratospheric ozone, and trigger perturbation in ecosystems. Being an agrarian country with a large livestock population and uncontrolled fertilizer application, India could be accountable as a major stakeholder of global NH3 emissions. This study developed a comprehensive gridded (0.1° x 0.1°) ammonia inventory for India considering 24 types of sources. The total NH3 emission is estimated to be 10.54 Tg/yr in 2022, where synthetic fertilizer application accounts for ∼47 % followed by livestock (∼34 %). Minor unattended sectors such as biomass burning, agricultural soil, human excrement, waste disposal, etc. contribute 0.68 Tg/yr, 0.32 Tg/yr, 0.3 Tg/yr, and 0.14 Tg/yr, respectively. The overall uncertainty of the inventory ranges around ± 55 %. These emission datasets are essential for atmospheric chemistry models and could be a crucial tool for policymakers to combat ammonia pollution.

The impact of energy sector pollution on human development and inequality amidst climate change

Abstract The provision of energy is a primary contributor to climate change and environmental pollution, the latter including air pollution from aerosol emissions and a broad range of other human health effects and ecosystem damages. At the same time, aerosol emissions also reduce radiative forcing, leading to a masking of part of the warming due to rising CO$_2$ concentrations and temporarily reducing the adverse impacts of climate change. Using an energy-economy-climate model linked to atmospheric chemistry, health impact and life cycle assessment models, we show that the societal costs of the health impacts of environmental pollution substantially exceed the economic benefits from masked warming. We further highlight the unequal burden of these issues on developing countries and explore the implications for human development, global inequality and international climate policy.

An Improved CH4 Profile Retrieving Method for Ground-Based Differential Absorption Lidar

Range-resolved CH4 concentration measurement is important prior data for atmospheric physical and chemical models. Ground-based differential absorption lidar (DIAL) can measure the vertical distribution of CH4 concentration in the atmosphere. The traditional method uses lidar observational data and the lidar equation to calculate profiles, but the inversion accuracy is greatly affected by noise. Although some denoising methods can improve accuracy at low altitudes, the low signal-to-noise ratio caused by the effect of aerosol Mie scattering and lower aerosol concentrations at high altitudes cannot be solved. Here, an improved cubic smoothing spline fitting CH4 concentration profile inversion method is proposed to address this challenge. By adding a penalty term of the second derivative of the conventional cubic spline function to the objective function, this penalty term acts to smooth the fitting, allowing the fitting function to avoid necessarily passing through those noisy sampling points. This avoids the large fluctuations caused by noisy sampling points, effectively suppresses noise, captures signals with lower noise levels, and thereby enhances the inversion accuracy of the profiles. Simulations and case studies demonstrated the superiority of the proposed method. Compared with the traditional method, cubic smoothing spline fitting can reduce the mean error of the whole CH4 profile by 85.54%. The standard deviation of CH4 concentration retrieved is 3.59 ppb–90.29 ppb and 0.01 ppb–6.75 ppb smaller than the traditional method and Chebyshev fitting, respectively. Three real cases also indicate that the CH4 concentration retrieved by cubic smoothing spline fitting is more consistent with in-situ measurements. In addition, long-term DIAL observations have also revealed notable diurnal and seasonal trends in CH4 concentration at observation sites.

Updating the radiation infrastructure in MESSy (based on MESSy version 2.55)

Abstract. The calculation of the radiative transfer is a key component of global circulation models. In this article, we describe the most recent updates of the radiation infrastructure in the Modular Earth Submodel System (MESSy). These updates include the implementation of the PSrad radiation scheme within the RAD submodel. Furthermore, the radiation-related submodels CLOUDOPT (for the calculation of cloud optical properties) and AEROPT (for the calculation of aerosol optical properties) have been updated and are now more flexible in order to deal with different sets of shortwave and longwave bands of radiation schemes. In the wake of these updates, a new submodel (ALBEDO), which features solar-zenith-angle-dependent albedos and a new satellite-based background (white sky) albedo, was created. All of these developments are backward compatible, and previous features of the MESSy radiation infrastructure remain available. Moreover, these developments mark an important step in the use of the ECHAM/MESSy Atmospheric Chemistry (EMAC) model, as the update of the radiation scheme was a key aspect in the development of the sixth generation of the European Centre for Medium-Range Weather Forecasts – HAMburg (ECHAM6) model from ECHAM5. The developments presented here are also aimed towards using the MESSy infrastructure with the ICOsahedral Non-hydrostatic (ICON) model as a base model. The improved infrastructure will also aid in the implementation of additional radiation schemes once this should be needed. We have optimized the set of free parameters for two general circulation model-type (GCM-type) setups for pre-industrial and present-day conditions: one with the radiation scheme that was used to date (i.e. the radiation scheme of ECHAM5) and one with the newly implemented PSrad radiation scheme. After this parameter optimization, we performed four model simulations and evaluated the corresponding model results using reanalysis and observational data. The most apparent improvements related to the updated radiation scheme are the reduced cold biases in the tropical upper troposphere and lower stratosphere and the extratropical lower stratosphere and a strengthened polar vortex. The former is also related to improved stratospheric humidity and its variability if the new radiation scheme is employed. Using the multiple radiation call capability of MESSy, we have applied the two model configurations to calculate instantaneous and stratospheric-adjusted radiative forcings related to changes in greenhouse gases. Overall, we find that for many forcing experiments the simulations with the new radiation scheme show improved radiative forcing values. This is in particular the case for methane radiative forcings, which are considerably higher when assessed with the new radiation scheme and thus in better agreement with reference values.

How Nonpolar CO2 Aggregates on Cycloalkenes: A Case Study with Cyclopentene-(CO2)1-3 Clusters.

This study explores the molecular clusters of cyclopentene (CPE) with one to three CO2 molecules (CPE-(CO2)1-3) through their jet-cooled rotational spectra using Fourier transform microwave spectroscopy with supplementary quantum chemical calculations. The assembly of CPE-(CO2)1-3 clusters is predominantly driven by tetrel bonding networks, notably C···π(C═C) and C···O interactions, with additional stabilization from weak C─H(CH2)···C═O hydrogen bonds. Critically, the dispersive forces play a pivotal role in stabilizing CO2 aggregation on CPE, eclipsing the effects of electrostatic and orbital interactions. This highlights the complex balance of forces that govern the formation and stabilization of these molecular clusters. Our findings offer precise insights into noncovalent interactions that could enhance atmospheric chemistry models and sustain climate science through informed environmental chemistry strategies.

Evaluation of the coupling of EMACv2.55 to the land surface and vegetation model JSBACHv4

Abstract. We present the coupling of the Jena Scheme for Biosphere–Atmosphere Coupling in Hamburg version 4 (JSBACHv4) to the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. With JSBACH, the soil water bucket model in EMAC is replaced by a diffusive hydrological transport model for soil water that includes water storage and infiltration in five soil layers, preventing soil from drying too rapidly and reducing biases in soil temperature and moisture. A three-layer soil scheme is implemented, and phase changes in water in the soil are considered. The leaf area index (LAI) climatology in EMAC has been substituted with a phenology module calculating the LAI. Multiple land cover types are included to provide a state-dependent surface albedo, which accounts for the absorption of solar radiation by vegetation. Plant net primary productivity, leaf area index and surface roughness are calculated according to the plant functional types. This paper provides a detailed evaluation of the new coupled model based on observations and reanalysis data, including ERA5/ERA5-Land datasets, Global Precipitation Climatology Project (GPCP) data and Moderate Resolution Imaging Spectroradiometer (MODIS) satellite data. Land surface temperature (LST), terrestrial water storage (TWS), surface albedo (α), net top-of-atmosphere radiation flux (RadTOA), precipitation (precip), leaf area index (LAI), fraction of absorbed photosynthetic active radiation (FAPAR) and gross primary productivity (GPP) are evaluated in particular. The strongest correlation (r) between reanalysis data and the newly coupled model is found for LST (r=0.985, with an average global bias of −1.546 K), α (r=0.947, with an average global bias of −0.015) and RadTOA (r=0.907, with an average global bias of 3.56 W m−2). Precipitation exhibits a correlation with the GPCP dataset of 0.523 and an average global bias of 0.042 mm d−1. The LAI optimisation yields a correlation of 0.637 with observations and a global mean deviation of −0.212. FAPAR and GPP exemplify two of the many additional variables made available through JSBACH in EMAC. FAPAR and observations show a correlation of 0.663, with an average global difference of −0.223, while the correlation for GPP and observations is 0.564 and the average global difference is −0.001 kg carbon km−1. Benefiting from the numerous added features within the simulated land system, the representation of soil moisture is improved, which is critical for vegetation modelling. This improvement can be attributed to a general increase in soil moisture and water storage in deeper soil layers and a closer alignment of simulated TWS with observations, mitigating the previously widespread problem of soil drought. We show that the numerous newly added components strongly improve the land surface, e.g. soil moisture, TWS and LAI, while surface parameters, such as LST, surface albedo or RadTOA, which were mostly prescribed according to climatologies, remain similar. The coupling of JSBACH brings EMAC a step closer towards a holistic comprehensive Earth system model and extends its versatility.

The influence of plant water stress on vegetation–atmosphere exchanges: implications for ozone modelling

Abstract. Evapotranspiration is important for Earth's water and energy cycles as it strongly affects air temperature, cloud cover, and precipitation. Leaf stomata are the conduit of transpiration, and their opening is sensitive to weather and climate conditions. This feedback can exacerbate heat waves and can play a role in their spatiotemporal propagation. Sustained high temperatures strongly favour high ozone levels, with significant negative impacts on air quality and thus on human health. Our study evaluates the process representation of evapotranspiration in the atmospheric chemistry–climate European Centre for Medium-Range Weather Forecasts – Hamburg(ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry model. Different water stress parameterizations are implemented in a stomatal model based on CO2 assimilation. The stress factors depend on either soil moisture or leaf water potential, which act on photosynthetic activity, and mesophyll and stomatal conductance. The new functionalities reduce the initial overestimation of evapotranspiration in the model globally by more than an order of magnitude, which is most important in the Southern Hemisphere. The intensity of simulated warm spells over continents is significantly improved. For ozone, we find that a realistic model representation of plant water stress suppresses uptake by vegetation and enhances photochemical production in the troposphere. These effects lead to an overall increase in simulated ground-level ozone, which is most pronounced in the Southern Hemisphere over the continents. More sophisticated land surface models with multi-layer soil schemes could address the uncertainties in representing plant dynamics representation due to too-shallow roots. In regions with low evaporative loss, the representation of precipitation remains the largest uncertainty.

Unique impacts of strong and westward-extended western Pacific subtropical high on ozone pollution over eastern China

As a subtropical anticyclonic high-pressure system that typically forms over the northwestern Pacific Ocean in summer, the Western Pacific subtropical high (WPSH) affects meteorological conditions and ozone pollution in China. The relationship between maximum daily 8-h average ozone (MDA8 O3) concentrations and the extremely strong and westward-extended WPSH occurred in 2022 is investigated using observations, reanalysis data and atmospheric chemistry model simulations. During July–August 2022, a significant positive relationship existed between the intensity of the WPSH and MDA8 O3 over southern China, with a correlation coefficient of +0.44, but the correlation is negative (−0.40) in northern China. During the strong WPSH days, MDA8 O3 increased by 16.5 μg m−3 (16.4% relative to July–August average) over southern China and decreased by 19.0 μg m−3 (14.5%) in northern China compared to the weak WPSH days. The unique dipole pattern in the relationship between ozone levels and the WPSH in 2022 exhibited a contrast to that during 2015–2021. The difference is primarily due to the extremely strong WPSH intensity and its unusual westward expansion in 2022. In this case, an anomalous anticyclone at 500 hPa dominates over southern China, which creates conditions conducive for ozone formation and accumulation. The anticyclone weakened horizontal winds and reduced the dispersion of ozone, alongside a high temperature and low relative humidity, which favored the chemical production of ozone. In contrast, abnormal northerly winds enhanced ozone diffusion in northern China and the low temperature reduced ozone chemical production. This study reveals the mechanism for the significant impact of strong and westward-extended WPSH on ozone concentrations over China, emphasizing the role of the WPSH location in modulating meteorology and ozone levels.

Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe

Abstract. Atmospheric volatile organic compounds (VOCs) constitute a wide range of species, acting as precursors to ozone and aerosol formation. Atmospheric chemistry and transport models (CTMs) are crucial to understanding the emissions, distribution, and impacts of VOCs. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West (EMEP MSC-W) CTM to evaluate emission inventories in Europe. Here we undertake the first intensive model–measurement comparison of VOCs in 2 decades. The modelled surface concentrations are evaluated both spatially and temporally, using measurements from the regular EMEP monitoring network in 2018 and 2019, as well as a 2022 campaign. To achieve this, we utilised the UK National Atmospheric Emissions Inventory to derive explicit emission profiles for individual species and employed a tracer method to produce pure concentrations that are directly comparable to observations. The degree to which the modelled and measured VOCs agree varies depending on the specific species. The model successfully captures the overall spatial and temporal variations of major alkanes (e.g. ethane, n-butane) and unsaturated species (e.g. ethene, benzene) but less so for propane, i-butane, and ethyne. This discrepancy underscores potential issues in the boundary conditions for the latter species and in their primary emissions from, in particular, the solvent and road transport sectors. Specifically, potential missing propane emissions and issues with its boundary conditions are highlighted by large model underestimations and smaller propane-to-ethane ratios compared to the measurement. Meanwhile, both the model and measurements show strong linear correlations among butane isomers and among pentane isomers, indicating common sources for these pairs of isomers. However, modelled ratios of i-butane to n-butane and i-pentane to n-pentane are approximately one-third of the measured ratios, which is largely driven by significant emissions of n-butane and n-pentane from the solvent sector. This suggests issues with the speciation profile of the solvent sector, underrepresented contributions from transport and fuel evaporation sectors in current inventories, or both. Furthermore, the modelled ethene-to-ethyne and benzene-to-ethyne ratios differ significantly from measured ratios. The different model performance strongly points to shortcomings in the spatial and temporal patterns and magnitudes of ethyne emissions, especially during winter. For OVOCs, the modelled and measured concentrations of methanal and methylglyoxal show a good agreement, despite a moderate underestimation by the model in summer. This discrepancy could be attributed to an underestimation of contributions from biogenic sources or possibly a model overestimation of their photolytic loss in summer. However, the insufficiency of suitable measurements limits the evaluation of other OVOCs. Finally, model simulations employing the CAMS inventory show slightly better agreements with measurements than those using the Centre on Emission Inventories and Projections (CEIP) inventory. This enhancement is likely due to the CAMS inventory's detailed segmentation of the road transport sector, including its associated sub-sector-specific emission profiles. Given this improvement, alongside the previously mentioned concerns about the model's biased estimations of various VOC ratios, future efforts should focus on a more detailed breakdown of dominant emission sectors (e.g. solvents) and the refinement of their speciation profiles to improve model accuracy.

Nonlinear and Non‐Gaussian Ensemble Assimilation of MOPITT CO

AbstractSatellite retrievals of carbon monoxide (CO) are routinely assimilated in atmospheric chemistry models to improve air quality forecasts, produce reanalyzes and to estimate emissions. This study applies the quantile‐conserving ensemble filter framework, a novel assimilation algorithm that can deal with non‐Gaussian and modestly nonlinear distributions. Instead of assuming normal distributions like the Ensemble Adjustments Kalman Filter (EAKF), we now apply a bounded normal rank histogram (BNRH) distribution for the prior. The goal is to efficiently estimate bounded quantities such as CO atmospheric mixing ratios and emission fluxes while maintaining the good performance achieved by the EAKF. We contrast assimilating meteorological and MOPITT (Measurement of Pollution in the Troposphere) observations for May 2018. We evaluate the results with the fourth deployment of the NASA Atmospheric Tomography Mission (ATom‐4) airborne field campaign. We also compare simulations with CO tropospheric columns from the network for the detection of atmospheric composition change and surface in‐situ observations from NOAA carbon cycle greenhouse gases. While the differences remain small, the BNRH approach clearly works better than the EAKF in comparison to all observation data sets.

Impacts of stratosphere-to-troposphere transport on tropospheric ozone in southeastern China: insights from ozonesonde observations

Tropospheric ozone pollution poses a major environmental challenge in China. As its primary natural source, Stratosphere-to-Troposphere Transport (STT) has been recognized as a significant contributor to tropospheric ozone in western, northeastern, and eastern China. However, the extent of STT’s influence on southeastern China has been less studied due to data limitations. Using a recently available one-year dataset of ozonesonde observations from a regional background station, we find that STT contributes significantly to tropospheric and surface ozone elevation in southeastern China. Our results show that STT plays a more substantial role in shaping tropospheric ozone during spring than previously believed, accounting for over 30% of ozone concentrations above 4 km. Without the stratospheric contribution, the spring seasonal peak almost disappears. STT can also significantly influence ozone concentrations at the surface. For example, a distinct ozone profile was observed on 4 May 2022, with a notable increase in tropospheric ozone. This tropospheric ozone increase was caused by a STT event triggered by a robust horizontal trough and subsequent southward movement of subtropical jets in the upper troposphere. According to a stratospheric tracer derived from an atmospheric chemistry model, this STT event contributed to 25%–30% of the surface ozone increase. Overall, this study highlights the important role of STT in driving tropospheric ozone variations, even in regions with comparatively lower ozone levels in southeastern China.

Projecting Changes in the Frequency and Magnitude of Ozone Pollution Events Under Uncertain Climate Sensitivity

AbstractClimate change is projected to worsen ozone pollution over many populated regions, with larger impacts at higher concentrations. More intense and frequent ozone episodes risk setbacks to human health and environmental policy achievements. However, assessing these changes is complicated by uncertain climate sensitivity, closely related to climate model response, and internal variability in simulations projecting climate's influence on air quality. Here, leveraging a global modeling framework that one‐way couples a human activity model, an Earth system model of intermediate complexity, and an atmospheric chemistry model, we investigate the role of climate sensitivity in climate‐induced changes to high ozone pollution episodes in the United States using multiple greenhouse gas emissions scenarios, representations of climate sensitivity, and initial condition members. We bias correct and evaluate historical model simulations, identifying modeled and observed O3 episodes using extreme value theory, and extend the approach to projections of mid‐ and end‐century climate impacts. Results show that the influence of climate sensitivity can be as significant as that of greenhouse gas emissions scenario absent precursor emissions changes. Climate change is projected to increase the magnitude of the highest annually occurring O3 concentrations by over 2.3 ppb on average across the U.S. at mid‐century under a high climate sensitivity and moderate emissions scenario, but the increase is limited to less than 0.3 ppb under lower climate sensitivity. Further, we show that areas in the U.S. currently meeting air quality standards risk being pushed into non‐compliance due to a climate‐induced increase in frequency of high ozone days.

The Design of a Parameterization Scheme for 137Cs Based on the WRF-Chem Model and Its Application in Simulating the Fukushima Nuclear Accident

Based on the Weather Research and Forecasting Model Coupled with Chemistry (WRF-Chem) atmospheric chemistry model, a parameterization scheme for the radioactive isotope caesium (137Cs), considering processes such as advection, turbulent diffusion, dry deposition, and wet deposition, was constructed, enabling the spatial distribution simulation of the concentration and deposition of 137Cs. The experimental simulation studies were carried out during the high emission period of the Fukushima nuclear accident (from 11 to 17 March 2011). Two sets of comparison experiments, with or without deposition, were designed, the effects of wind field and precipitation on the spatial transport and ground deposition of 137Cs were analyzed, and the influence of wind field and precipitation on 137Cs vertical transport was analyzed in detail. The results indicate that the model can accurately simulate the meteorological and 137Cs variables. On 15 March, 137Cs dispersed towards the Kanto Plain in Japan under the influence of northeastern winds. In comparison to the experiment without deposition, the concentration of 137Cs in the Fukushima area decreased by approximately 286 Bq·m−3 in the deposition experiment. Under the influence of updrafts in the non-deposition experiment, a 137Cs cloud spread upward to a maximum height of 6 km, whereas in the deposition experiment, the highest dispersion of the 137Cs cloud only reach a height of 4 km. Affected by the wind field, dry deposition is mainly distributed in Fukushima, the Kanto Plain, and their eastern ocean areas, with a maximum dry deposition of 5004.5 kBq·m−2. Wet deposition is mainly influenced by the wind field and precipitation, distributed in the surrounding areas of Fukushima, with a maximum wet deposition of 725.3 kBq·m−2. The single-station test results from the deposition experiment were better than those for the non-deposition experiment: the percentage deviations of the Tokyo, Chiba, Maebashi, and Naraha stations decreased by 61%, 69%, 46%, and 51%, respectively, and the percentage root mean square error decreased by 46%, 25%, 38%, and 48%, respectively.

Decision-making strategies implemented in SolFinder 1.0 to identify eco-efficient aircraft trajectories: application study in AirTraf 3.0

Abstract. The optimization of aircraft trajectories involves balancing operating costs and climate impact, which are often conflicting objectives. To achieve compromised optimal solutions, higher-level information such as preferences of decision-makers must be taken into account. This paper introduces the SolFinder 1.0 module, a decision-making tool designed to identify eco-efficient aircraft trajectories, which allow for the reduction of the flight's climate impact with limited cost penalties compared to cost-optimal solutions. SolFinder 1.0 offers flexible decision-making options that allow users to select trade-offs between different objective functions, including fuel use, flight time, NOx emissions, contrail distance, and climate impact. The module is included in the AirTraf 3.0 submodel, which optimizes trajectories under atmospheric conditions simulated by the ECHAM/MESSy Atmospheric Chemistry model. This paper focuses on the ability of the module to identify eco-efficient trajectories while solving a bi-objective optimization problem that minimizes climate impact and operating costs. SolFinder 1.0 enables users to explore trajectory properties at varying locations of the Pareto fronts without prior knowledge of the problem results and to identify solutions that limit the cost of reducing the climate impact of a single flight.