Chemistry-climate Model Research Articles

Radiative impact of improved global parameterisations of oceanic dry deposition of ozone and lightning-generated NOx

Abstract. We investigated the radiative impact of recent process-based improvements to oceanic ozone (O3) dry deposition parameterisation and empirical improvements to lightning-generated oxides of nitrogen (LNOx) parameterisation by conducting a 5-year simulation of the Australian Community Climate and Earth System Simulator – United Kingdom Chemistry and Aerosol (ACCESS-UKCA) global chemistry–climate model, with radiative effects of O3, methane (CH4) and aerosol included. Compared to the base parameterisations, the global consequences of the two improved parameterisations on atmospheric composition are dominated by the LNOx change (which increases the LNOx production from 4.8 to 6.9 Tg N yr−1) and include (a) an increase in the O3 column of 3.75 DU, and this O3 change is centred on the tropical upper troposphere where O3 is most effective as a radiative forcer; (b) a decrease of 0.64 years in the atmospheric lifetime of CH4 due to an increase in hydroxyl radical, which corresponds to a decrease of 0.31 years in the CH4 lifetime per Tg N yr−1 change in LNOx; (c) an increase of 6.7 % in the column integrated condensation nuclei concentration; and (d) a slight increase in high-level cloud cover. The two combined parameterisation changes cause an increase of 86.3 mW m−2 in the globally-averaged all-sky net downward top-of-atmosphere (TOA) radiative flux (which is akin to instantaneous radiative forcing), and only 5 % of which is due to the dry deposition parameterisation change. Other global radiative changes from the use of the two parameterisations together include an increase in the downward longwave radiation and a decrease in the downward shortwave radiation at the earth's surface. The indirect effect of LNOx on aerosol and cloud cover can at least partly explain the differences in the downward shortwave flux at the surface. It is demonstrated that although the total global LNOx production may be the same, how LNOx is distributed spatially makes a difference to radiative transfer. We estimate that for a reported uncertainty range of 5±3 Tg N yr−1 in global estimates of LNOx, the uncertainty in the net downward TOA radiation is ±119 mW m−2. The corresponding uncertainly in the atmospheric methane lifetime is ±0.92 years. Thus, the value of LNOx used within a model will influence the effective radiative forcing (ERF) and global warming potential (GWP) of anthropogenic CH4, and influence the results of climate scenario modelling.

Ozone, DNA-active UV radiation, and cloud changes for the near-global mean and at high latitudes due to enhanced greenhouse gas concentrations

Abstract. This study analyses the variability and trends of ultraviolet-B (UV-B, wavelength 280–320 nm) radiation that can cause DNA damage. The variability and trends caused by climate change due to enhanced greenhouse gas (GHG) concentrations. The analysis is based on DNA-active irradiance, total ozone, total cloud cover, and surface albedo calculations with the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) chemistry–climate model (CCM) free-running simulations following the RCP 6.0 climate scenario for the period 1960–2100. The model output is evaluated with DNA-active irradiance ground-based measurements, satellite SBUV (v8.7) total-ozone measurements, and satellite MODerate-resolution Imaging Spectroradiometer (MODIS) Terra cloud cover data. The results show that the model reproduces the observed variability and change in total ozone, DNA-active irradiance, and cloud cover for the period 2000–2018 quite well according to the statistical comparisons. Between 50∘ N–50∘ S, the DNA-damaging UV radiation is expected to decrease until 2050 and to increase thereafter, as was shown previously by Eleftheratos et al. (2020). This change is associated with decreases in the model total cloud cover and negative trends in total ozone after about 2050 due to increasing GHGs. The new study confirms the previous work by adding more stations over low latitudes and mid-latitudes (13 instead of 5 stations). In addition, we include estimates from high-latitude stations with long-term measurements of UV irradiance (three stations in the northern high latitudes and four stations in the southern high latitudes greater than 55∘). In contrast to the predictions for 50∘ N–50∘ S, it is shown that DNA-active irradiance will continue to decrease after the year 2050 over high latitudes because of upward ozone trends. At latitudes poleward of 55∘ N, we estimate that DNA-active irradiance will decrease by 8.2 %±3.8 % from 2050 to 2100. Similarly, at latitudes poleward of 55∘ S, DNA-active irradiance will decrease by 4.8 % ± 2.9 % after 2050. The results for the high latitudes refer to the summer period and not to the seasons when ozone depletion occurs, i.e. in late winter and spring. The contributions of ozone, cloud, and albedo trends to the DNA-active irradiance trends are estimated and discussed.

Atmospheric concentrations and sources of black carbon over tropical Australian waters

Black carbon (BC) aerosols significantly contribute to radiative budgets globally, however their actual contributions remain poorly constrained in many under-sampled ocean regions. The tropical waters north of Australia are a part of the Indo-Pacific warm pool, regarded as a heat engine of global climate, and are in proximity to large terrestrial sources of BC aerosols such as fossil fuel emissions, and biomass burning emissions from northern Australia. Despite this, measurements of marine aerosols, especially BC remain elusive, leading to large uncertainties and discrepancies in current chemistry-climate models for this region. Here, we report the first comprehensive measurements of aerosol properties collected over the tropical warm pool in Australian waters during a voyage in late 2019. The non-marine related aerosol emissions observed in the Arafura Sea region were more intense than in the Timor Sea marine region, as the Arafura Sea was subject to greater continental outflows. The median equivalent BC (eBC) concentration in the Arafura Sea (0.66 μg m−3) was slightly higher than that in the Timor Sea (0.49 μg m−3). Source apportionment modelling and back trajectory analysis and tracer studies consistently suggest fossil fuel combustion eBC (eBCff) was the dominant contributor to eBC across the entire voyage region, with biomass burning eBC (eBCbb) making significant additional contributions to eBC in the Arafura Sea. eBCff (possibly from ship emissions or oil and gas rigs and their associated activities) and cloud condensation nuclei (CCN) were robustly correlated in the Timor Sea data, whereas eBCbb positively correlated to CCN in the Arafura Sea, suggesting different sources and atmospheric processing pathways occurred in these two regions. This work demonstrates the substantial impact that fossil fuel and biomass burning emissions can have on the composition of aerosols and cloud processes in the remote tropical marine atmosphere, and their potentially significant contribution to the radiative balance of the rapidly warming Indo-Pacific warm pool.

Air quality and health implications of transitioning 30% of the US Midwest heavy-duty transport fleet from diesel to electric power

BackgroundTransitioning to an electric vehicle fleet is an ongoing climate change mitigation action that will reduce tailpipe emissions but increase the energy demand for charging. The subsequent impact this would have on air quality is poorly understood. In this work, we study the effect of transitioning 30% of the heavy-duty fleet in the US Midwest to electric and analyse the corresponding effects on air pollution concentrations and their associated health impacts. MethodsWe scaled tailpipe, refuelling, and idling emissions from heavy-duty vehicles (HDVs) by 30% and estimated the additional energy demand needed for charging. The two-way coupled Weather Research Forecast and Community Multiscale Air Quality chemistry-climate model was used to simulate air pollution concentrations after these emission changes. Monthly simulations for each season were run at a 1·3-km resolution. We estimated the associated health impacts of resultant pollutant concentrations using concentrations response functions derived from epidemiological studies. FindingsCompared with a baseline scenario, we estimate that annual NO2 and PM2·5 concentrations will decrease by up to 4·91 parts per billion and 0·49 μg/m3, respectively, across the study domain. By contrast, differences in annual daily maximum 8-h running mean O3 (MDA8O3) concentrations are spatially heterogenous, with increases along major road networks and metropolitan areas (up to 1·45 parts per billion) and small decreases in less populated regions. We estimate that these changes will lead to a substantial number of NO2 and PM2·5-related avoided deaths and marginal increases in MDA8O3-related health effects. InterpretationOur results highlight the overall beneficial effect of electrifying HDVs on air quality and human health, despite an increase in energy demand. However, policies aimed to transition to an electric vehicle fleet should consider air quality changes with a focus on areas that could experience MDA8O3 increases, leading to adverse health effects. FundingUS National Science Foundation, Ubben Program for Carbon and Climate Science, and Northwestern University.

Estimating the burden of disease attributable to ambient air pollution (ambient PM2.5 and ambient ozone) in South Africa for 2000, 2006 and 2012.

Globally, a growing body of research has shown that ambient air pollution is one of the most critical environmental issues, especially in relation to human health. Exposure to ambient air pollution leads to serious health conditions such as lower respiratory infections, cancers, diabetes mellitus type 2, ischaemic heart disease, stroke and chronic obstructive pulmonary disease. To estimate the burden of disease attributable to ambient air pollution in South Africa (SA) for the years 2000, 2006 and 2012. Comparative risk assessment method was used to determine the burden of disease due to two pollutants (particulate matter (PM2.5) and ambient ozone). Regionally optimised fully coupled climate chemistry models and surface air pollution observations were used to generate concentrations of PM2.5 and ozone for each SA Census Small Area Level, for the year 2012. For 2000 and 2006, population-weighted PM2.5and ozone were estimated, based on the 2012 results. Following the identification of disease outcomes associated with particulate matter with aerodynamic diameter <2.5 μm (PM2.5) and ozone exposure, the attributable burden of disease was estimated for 2000, 2006 and 2012. Furthermore, for the year 2012, the burden of disease attributable to ambient air pollution exposure was computed at provincial levels. In 2012, approximately 97.6% of people in SA were exposed to PM2.5 at levels above the 2005 World Health Organization guideline: 10 μg/m3 annual mean. From 2000 to 2012, population-weighted annual average PM2.5 increased from 26.6 μg/m3 to 29.7 μg/m3, and ozone 6-month high 8-hour daily maximum increased from 64.4 parts per billion (ppb) to 72.1 ppb. At a national scale, in the year 2000, 15 619 (95% uncertainty interval (UI) 8 958 - 21 849) deaths were attributed to PM2.5 exposure, while 1 326 (95% UI 534 - 1 885) deaths were attributed to ozone. In 2006, an estimated 19 672 deaths (95% UI 11 526 - 27 086) were attributed to PM2.5, and a further 1 591 deaths (95% UI 651 - 2 236) to ozone exposure. In 2012, deaths attributed to PM2.5 were 19 507 (95% UI 11 318 - 27 111), and to ozone 1 734 (95% UI 727 - 2 399). Additionally, population-weighted provincial scale analysis showed that Gauteng Province had the highest number of attributable deaths due to both PM2.5 and ozone in 2012. The study showed that ambient air pollution exposure is an important health risk in SA, requiring both short- and long-term intervention. In the short term, the SA Ambient Air Quality Standards and industrial minimum emissions standards need to be enforced. In the longer term, to reduce air pollution and the associated disease burden, the combustion of fossil fuels as a source of energy for power generation and transportation, as well as industrial and domestic uses, needs to be replaced with clean renewable energy sources. In addition to local measures, when the southern African prevalent anticyclonic air dynamics that transport regionally emitted pollutants into SA (especially from biomass burning) are considered, it is also advisable to establish long-term regional co-operation in reducing air pollution.

Correcting ozone biases in a global chemistry–climate model: implications for future ozone

Abstract. Weaknesses in process representation in chemistry–climate models lead to biases in simulating surface ozone and to uncertainty in projections of future ozone change. We here develop a deep learning model to demonstrate the feasibility of ozone bias correction in a global chemistry–climate model. We apply this approach to identify the key factors causing ozone biases and to correct projections of future surface ozone. Temperature and the related geographic variables latitude and month show the strongest relationship with ozone biases. This indicates that ozone biases are sensitive to temperature and suggests weaknesses in representation of temperature-sensitive physical or chemical processes. Photolysis rates are also an important factor, highlighting the sensitivity of biases to simulated cloud cover and insolation. Atmospheric chemical species such as the hydroxyl radical, nitric acid and peroxyacyl nitrate show strong positive relationships with ozone biases on a regional scale. These relationships reveal the conditions under which ozone biases occur, although they reflect association rather than direct causation. We correct model projections of future ozone under different climate and emission scenarios following the shared socio-economic pathways. We find that changes in seasonal ozone mixing ratios from the present day to the future are generally smaller than those simulated without bias correction, especially in high-emission regions. This suggests that the ozone sensitivity to changing emissions and climate may be overestimated with chemistry–climate models. Given the uncertainty in simulating future ozone, we show that deep learning approaches can provide improved assessment of the impacts of climate and emission changes on future air quality, along with valuable information to guide future model development.

Lightning-induced chemistry on tidally-locked Earth-like exoplanets

ABSTRACT Determining the habitability and interpreting atmospheric spectra of exoplanets requires understanding their atmospheric physics and chemistry. We use a 3-D coupled climate-chemistry model, the Met Office Unified Model with the UK Chemistry and Aerosols framework, to study the emergence of lightning and its chemical impact on tidally-locked Earth-like exoplanets. We simulate the atmosphere of Proxima Centauri b orbiting in the Habitable Zone of its M-dwarf star, but the results apply to similar M-dwarf orbiting planets. Our chemical network includes the Chapman ozone reactions and hydrogen oxide (HOx = H + OH + HO2) and nitrogen oxide (NOx = NO + NO2) catalytic cycles. We find that photochemistry driven by stellar radiation (177–850 nm) supports a global ozone layer between 20–50 km. We parametrize lightning flashes as a function of cloud-top height and the resulting production of nitric oxide (NO) from the thermal decomposition of N2 and O2. Rapid dayside convection over and around the substellar point results in lightning flash rates of up to 0.16 flashes km−2 yr−1, enriching the dayside atmosphere below altitudes of 20 km in NOx. Changes in dayside ozone are determined mainly by UV irradiance and the HOx catalytic cycle. ∼45 per cent of the planetary dayside surface remains at habitable temperatures (Tsurf &amp;gt; 273.15K), and the ozone layer reduces surface UV radiation levels to 15 per cent. Dayside–nightside thermal gradients result in strong winds that subsequently advect NOx towards the nightside, where the absence of photochemistry allows NOx chemistry to involve reservoir species. Our study also emphasizes the need for accurate UV stellar spectra to understand the atmospheric chemistry of exoplanets.

Dynamical perturbation of the stratosphere by a pyrocumulonimbus injection of carbonaceous aerosols

Abstract. The Pacific Northwest Pyrocumulonimbus Event (PNE) took place in British Columbia during the evening and nighttime hours between 12 and 13 August 2017. Several pyroconvective clouds erupted on this occasion, and released in the upper troposphere and lower stratosphere unprecedented amounts of carbonaceous aerosols (300 ktn). Only a few years later, an even larger pyrocumulonimbus (pyroCb) injection took place over Australia. This event, named “the Australian New Year (ANY) event”, injected up to 1100 ktn of aerosol between 29 December 2019 and 4 January 2020. Such large injections of carbonaceous aerosol modify the stratospheric radiative budgets, locally perturbing stratospheric temperatures and winds. In this study, we use the Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) to study the perturbations on the stratospheric meteorology induced by an aerosol injection of the magnitude of the PNE. Our simulations include the radiative interactions of aerosols, so that their impact on temperatures and winds are explicitly simulated. We show how the presence of the carbonaceous aerosols from the pyroCb causes the formation and maintenance of a synoptic-scale stratospheric anticyclone. We follow this disturbance considering the potential vorticity anomaly and the brown carbon aerosol loading and we describe its dynamical and thermodynamical structure and its evolution in time. The analysis presented here shows that the simulated anticyclone undergoes daily expansion–compression cycles governed by the radiative heating, which are directly related to the vertical motion of the plume, and that the aerosol radiative heating is essential in maintaining the anticyclone itself.

Abrupt emission reduction during COVID-19 intensified the spring 2020 rainfall over India

The high level of aerosol pollution in South Asia has a measurable impact on clouds, radiation, and precipitation. Here, exploring multiple observational data sets and simulations of the state-of-the-art ECHAM6-HAMMOZ chemistry-climate model, we report that the reduction in anthropogenic emissions during the COVID-19 lockdown period has enhanced precipitation by 5–25% over India. This precipitation enhancement is the result of the combined effect of an enhancement in cloud cover, a reduction in aerosol induced cloud invigoration and dynamical changes. We observed that the increase in cloud cover was associated with a reduction in cloud base height and an increase in the effective radius of cloud particles which led to an increase in cloud water content. In response to sudden emission reduction, an anomalous northward moisture transport was observed adding convection and precipitation over the Indian region. Importantly, we show that there is an advantage of anthropogenic pollution reduction for water availability in addition to benefits of air quality, human health, and crop yield.

Atmospheric impacts of chlorinated very short-lived substances over the recent past – Part 1: Stratospheric chlorine budget and the role of transport

Abstract. Impacts of chlorinated very short-lived substances (Cl-VSLS) on stratospheric chlorine budget over the first two decades of the 21st century are assessed using the Met Office’s Unified Model coupled to the United Kingdom Chemistry and Aerosol (UM-UKCA) chemistry–climate model; this constitutes the most up-to-date assessment and the first study to simulate Cl-VSLS impacts using a whole atmosphere chemistry–climate model. We examine the Cl-VSLS responses using a small ensemble of free-running simulations and two pairs of integrations where the meteorology was “nudged” to either ERA5 or ERA-Interim reanalysis. The stratospheric chlorine source gas injection due to Cl-VSLS estimated from the free-running integrations doubled from ∼40 ppt Cl injected into the stratosphere in 2000 to ∼80 ppt Cl injected in 2019. Combined with chlorine product gas injection, the integrations showed a total of ∼130 ppt Cl injected into the stratosphere in 2019 due to Cl-VSLS. The use of the nudged model significantly increased the abundance of Cl-VSLS simulated in the lower stratosphere relative to the free-running model. Averaged over 2010–2018, simulations nudged to ERAI-Interim and ERA5 showed 20 ppt (i.e. a factor of 2) and 10 ppt (i.e. ∼50 %) more Cl, respectively, in the tropical lower stratosphere at 20 km in the form of Cl-VSLS source gases compared to the free-running case. These differences can be explained by the corresponding differences in the speed of the large-scale circulation. The results illustrate the strong dependence of the simulated stratospheric Cl-VSLS levels on the model dynamical fields. In UM-UKCA, this corresponds to the choice between free-running versus nudged set-up, and to the reanalysis dataset used for nudging. Temporal changes in Cl-VSLS are found to have significantly impacted recent HCl and COCl2 trends in the model. In the tropical lower stratosphere, the inclusion of Cl-VSLS reduced the magnitude of the negative HCl and COCl2 trends (e.g. from ∼-8%(HCl)/decade and ∼-4 ppt(COCl2)/decade at ∼20 km to ∼-6%(HCl)/decade and ∼ −2 ppt(COCl2)/decade in the free running simulations) and gave rise to positive tropospheric trends in both tracers. In the tropics, both the free-running and nudged integrations with Cl-VSLS included compared much better to the observed trends from the ACE-FTS satellite record than the analogous simulations without Cl-VSLS. Since observed HCl trends provide information on the evolution of total stratospheric chlorine and, thus, the effectiveness of the Montreal Protocol, our results demonstrate that Cl-VSLS are a confounding factor in the interpretation of such data and should be factored into future analysis. Unlike the nudged model runs, the ensemble mean free-running integrations did not reproduce the hemispheric asymmetry in the observed mid-latitude HCl and COCl2 trends related to short-term dynamical variability. The individual ensemble members also showed a considerable spread of the diagnosed tracer trends, illustrating the role of natural interannual variability in modulating the diagnosed responses and the need for caution when interpreting both model and observed tracer trends derived over a relatively short time period.

A machine learning methodology for the generation of a parameterization of the hydroxyl radical

Abstract. We present a methodology that uses gradient-boosted regression trees (a machine learning technique) and a full-chemistry simulation (i.e., training dataset) from a chemistry–climate model (CCM) to efficiently generate a parameterization of tropospheric hydroxyl radical (OH) that is a function of chemical, dynamical, and solar irradiance variables. This surrogate model of OH is designed to be integrated into a CCM and allow for computationally efficient simulation of nonlinear feedbacks between OH and tropospheric constituents that have loss by reaction with OH as their primary sinks (e.g., carbon monoxide (CO), methane (CH4), volatile organic compounds (VOCs)). Such a model framework is advantageous for studies that require multi-decadal simulations of CH4 or multi-year sensitivity simulations to understand the causes of trends and variations of CO and CH4. To allow the user to easily target the training dataset towards a desired application, we are outlining a methodology to generate a parameterization of OH and not presenting an “off-the-shelf” version of a parameterization to be incorporated into a CCM. This provides for the relatively easy creation of a new parameterization in response to, for example, changes in research goals or the underlying CCM chemistry and/or dynamics schemes. We show that a sample parameterization of OH generated from a CCM simulation is able to reproduce OH concentrations with a normalized root-mean-square error of approximately 5 % and capture the global mean methane lifetime within approximately 1 %. Our calculated accuracy of the parameterization assumes inputs being within the bounds of the training dataset. Large excursions from these bounds will likely decrease the overall accuracy. However, we show that the sample parameterization predicts large deviations in OH for an El Niño event that was not part of the training dataset and that the spatial distribution and strength of these deviations are consistent with the event. This result gives confidence in the fidelity of a parameterization developed with our methodology to simulate the spatial and temporal responses of OH to perturbations from large variations in the chemical, dynamical, and solar irradiance drivers of OH. In addition, we discuss how two machine learning metrics, Gain feature importance and Shapley additive explanations values, indicate that the behavior of a parameterization of OH generally accords with our understanding of OH chemistry, even though there are no physics- or chemistry-based constraints on the parameterization.

Updated Simulation of Tropospheric Ozone and Its Radiative Forcing over the Globe and China Based on a Newly Developed Chemistry-Climate Model

Updated Simulation of Tropospheric Ozone and Its Radiative Forcing over the Globe and China Based on a Newly Developed Chemistry-Climate Model

A mini-chemical scheme with net reactions for 3D general circulation models

Context. Growing evidence has indicated that the global composition distribution plays an indisputable role in interpreting observational data. Three-dimensional general circulation models (GCMs) with a reliable treatment of chemistry and clouds are particularly crucial in preparing for upcoming observations. In attempts to achieve 3D chemistry-climate modeling, the challenge mainly lies in the expensive computing power required for treating a large number of chemical species and reactions. Aims. Motivated by the need for a robust and computationally efficient chemical scheme, we devise a mini-chemical network with a minimal number of species and reactions for H2-dominated atmospheres. Methods. We apply a novel technique to simplify the chemical network from a full kinetics model, VULCAN, by replacing a large number of intermediate reactions with net reactions. The number of chemical species is cut down from 67 to 12, with the major species of thermal and observational importance retained, including H2O, CH4, CO, CO2, C2H2, NH3, and HCN. The size of the total reactions is also greatly reduced, from ~800 to 20. We validated the mini-chemical scheme by verifying the temporal evolution and benchmarking the predicted compositions in four exoplanet atmospheres (GJ 1214b, GJ 436b, HD 189733b, and HD 209458b) against the full kinetics of VULCAN. Results. The mini-network reproduces the chemical timescales and composition distributions of the full kinetics well within an order of magnitude for the major species in the pressure range of 1 bar–0.1 mbar across various metallicities and carbon-to-oxygen (C/O) ratios. Conclusions. We have developed and validated a mini-chemical scheme using net reactions to significantly simplify a large chemical network. The small scale of the mini-chemical scheme permits simple use and fast computation, which is optimal for implementation in a 3D GCM or a retrieval framework. We focus on the thermochemical kinetics of net reactions in this paper and address photochemistry in a follow-up paper.

TransClim (v1.0): a chemistry–climate response model for assessing the effect of mitigation strategies for road traffic on ozone

Abstract. Road traffic emits not only carbon dioxide (CO2) and particulate matter, but also other pollutants such as nitrogen oxides (NOx), volatile organic compounds (VOCs) and carbon monoxide (CO). These chemical species influence the atmospheric chemistry and produce ozone (O3) in the troposphere. Ozone acts as a greenhouse gas and thus contributes to anthropogenic global warming. Technological trends and political decisions can help to reduce the O3 effect of road traffic emissions on climate. In order to assess the O3 response of such mitigation options on climate, we developed a chemistry–climate response model called TransClim (Modelling the effect of surface Transportation on Climate). The current version considers road traffic emissions of NOx, VOC and CO and determines the O3 change and its corresponding stratosphere-adjusted radiative forcing. Using a tagging method, TransClim is further able to quantify the contribution of road traffic emissions to the O3 concentration. Thus, TransClim determines the contribution to O3 as well as the change in total tropospheric O3 of a road traffic emission scenario. Both quantities are essential when assessing mitigation strategies. The response model is based on lookup tables which are generated by a set of emission variation simulations performed with the global chemistry–climate model EMAC (ECHAM5 v5.3.02, MESSy v2.53.0). Evaluating TransClim against independent EMAC simulations reveals low deviations of all considered species (0.01 %–10 %). Hence, TransClim is able to reproduce the results of an EMAC simulation very well. Moreover, TransClim is about 6000 times faster in computing the climate effect of an emission scenario than the complex chemistry–climate model. This makes TransClim a suitable tool to efficiently assess the climate effect of a broad range of mitigation options for road traffic or to analyse uncertainty ranges by employing Monte Carlo simulations.

Introducing new lightning schemes into the CHASER (MIROC) chemistry–climate model

Abstract. The formation of nitrogen oxides (NOx) associated with lightning activities (hereinafter designated as LNOx) is a major source of NOx. In fact, it is regarded as the dominant NOx source in the middle to upper troposphere. Therefore, improving the prediction accuracy of lightning and LNOx in chemical climate models is crucially important. This study implemented three new lightning schemes with the CHASER (MIROC) global chemical transport and climate model. The first lightning scheme is based on upward cloud ice flux (ICEFLUX scheme). The second one (the original ECMWF scheme), also adopted in the European Centre for Medium-Range Weather Forecasts (ECMWF) forecasting system, calculates lightning flash rates as a function of QR (a quantity intended to represent the charging rate of collisions between graupel and other types of hydrometeors inside the charge separation region), convective available potential energy (CAPE), and convective cloud-base height. For the original ECMWF scheme, by tuning the equations and adjustment factors for land and ocean, a new lightning scheme called the ECMWF-McCAUL scheme was also tested in CHASER. The ECMWF-McCAUL scheme calculates lightning flash rates as a function of CAPE and column precipitating ice. In the original version of CHASER (MIROC), lightning is initially parameterized with the widely used cloud-top height scheme (CTH scheme). Model evaluations with lightning observations conducted using the Lightning Imaging Sensor (LIS) and Optical Transient Detector (OTD) indicate that both the ICEFLUX and ECMWF schemes simulate the spatial distribution of lightning more accurately on a global scale than the CTH scheme does. The ECMWF-McCAUL scheme showed the highest prediction accuracy for the global distribution of lightning. Evaluation by atmospheric tomography (ATom) aircraft observations (NO) and tropospheric monitoring instrument (TROPOMI) satellite observations (NO2) shows that the newly implemented lightning schemes partially facilitated the reduction of model biases (NO and NO2), typically within the regions where LNOx is the major source of NOx, when compared to using the CTH scheme. Although the newly implemented lightning schemes have a minor effect on the tropospheric mean oxidation capacity compared to the CTH scheme, they led to marked changes in oxidation capacity in different regions of the troposphere. Historical trend analyses of flash and surface temperatures predicted using CHASER (2001–2020) show that lightning schemes predicted increasing trends of lightning or no significant trends, except for one case of the ICEFLUX scheme, which predicted a decreasing trend of lightning. The global lightning rates of increase during 2001–2020 predicted by the CTH scheme were 17.69 % ∘C−1 and 2.50 % ∘C−1, respectively, with and without meteorological nudging. The un-nudged runs also included the short-term surface warming but without the application of meteorological nudging. Furthermore, the ECMWF schemes predicted a larger increasing trend of lightning flash rates under the short-term surface warming by a factor of 4 (ECMWF-McCAUL scheme) and 5 (original ECMWF scheme) compared to the CTH scheme without nudging. In conclusion, the three new lightning schemes improved global lightning prediction in the CHASER model. However, further research is needed to assess the reproducibility of trends of lightning over longer periods.

3‐D Atmospheric Modeling of the Global Budget of N2O and Its Isotopologues for 1980–2019: The Impact of Anthropogenic Emissions

AbstractNitrous oxide (N2O) is the third most important anthropogenic greenhouse gas and a major ozone‐depleting substance. Its main sources include anthropogenic activities (mostly agriculture) and natural emissions from ocean and soils. However, emission estimates for individual sources are highly variable due to uncertainties in N2O lifetime estimates and partitioning among sources. We derive annual global N2O emissions for 1990–2019 using NOAA Global Monitoring Laboratory (GML) surface N2O observations and the N2O lifetime calculated in the NASA GEOS‐5 chemistry climate model. The inferred global mean N2O emissions has gradually increased from ∼15.8 TgN/yr in the early 1990s to ∼17.8 TgN/yr in the 2010s. This implies that anthropogenic N2O emissions have grown rapidly from ∼6.7 TgN/yr in the 1990s to about ∼8.7 TgN/yr in the 2010s, a ∼30% increase. With specially designed N2O isotopic tracers in 3‐D GEOSCCM, we estimate that, on global average, stratospheric enrichment contributes about +7.7‰/yr, +7.6‰/yr, +8.0‰/yr to tropospheric δ15Nα, δ15Nβ, and δ18O budget, respectively. To balance the global mean isotopic signature for pre‐industrial terrestrial sources of δ15Nα ∼ 6.7‰, δ15Nβ ∼ −12.6‰, δ18O ∼ 35.4‰, our 3‐dimensional isotopic budget simulation using the GEOSCCM suggests global mean anthropogenic isotopic signatures in the recent decades are δ15Nα ∼ −18‰, δ15Nβ ∼ −20‰, δ18O ∼ 19‰. These anthropogenic isotopic estimates are significantly lighter than results from one‐box atmospheric model‐based estimates with the largest difference seen for δ15Nβ. More surface isotopic measurements are needed to better quantify the N2O isotopic signatures.

Springtime arctic ozone depletion forces northern hemisphere climate anomalies

Large-scale chemical depletion of ozone due to anthropogenic emissions occurs over Antarctica as well as, to a lesser degree, the Arctic. Surface climate predictability in the Northern Hemisphere might be improved due to a previously proposed, albeit uncertain, link to springtime ozone depletion in the Arctic. Here we use observations and targeted chemistry–climate experiments from two models to isolate the surface impacts of ozone depletion from complex downward dynamical influences. We find that springtime stratospheric ozone depletion is consistently followed by surface temperature and precipitation anomalies with signs consistent with a positive Arctic Oscillation, namely, warm and dry conditions over southern Europe and Eurasia and moistening over northern Europe. Notably, we show that these anomalies, affecting large portions of the Northern Hemisphere, are driven substantially by the loss of stratospheric ozone. This is due to ozone depletion leading to a reduction in short-wave radiation absorption, when in turn causing persistent negative temperature anomalies in the lower stratosphere and a delayed break-up of the polar vortex. These results indicate that the inclusion of interactive ozone chemistry in atmospheric models can considerably improve the predictability of Northern Hemisphere surface climate on seasonal timescales. Ozone depletion in the Arctic stratosphere consistently disrupts surface temperature and precipitation patterns across the Northern Hemisphere, according to atmospheric chemistry–climate modelling and observations.

Studies of the Effect of Seasonal Cycle on the Equatorial Quasi-Biennial Oscillation with a Chemistry-Climate Model

The effect of the seasonal cycle on the quasi-biennial oscillation (QBO) in the equatorial stratosphere was investigated using a chemistry-climate model (CCM) by fixing the seasonal cycle in CCM simulations. The CCM realistically reproduced the QBO in wind and ozone fields of a 30-month period in a climatological simulation (control run) under annually repeating sea surface temperature (SST) with a seasonal cycle. For the control run, four experimental simulations (perpetual runs) were made by fixing solar declination and SST on the 15th of January, April, July, and October, respectively, for about 20 years. In the three perpetual runs of January, July, and October, the QBO was maintained and persisted throughout the 20-year integration in spite of some small differences in period and amplitude among the three runs. On the other hand, the QBO in the perpetual April run began to weaken after about 15 years and the downward propagation of westerly wind stopped at about 20 hPa, resulting in the QBO’s ceasing. The cause of this QBO disappearance is related to the evolution of the background mean flow in the lower stratosphere, which filtered out the parameterized gravity waves propagating upwards farther.

A New Chemistry-Climate Model GRIMs-CCM: Model Evaluation of Interactive Chemistry-Meteorology Simulations

We describe a new chemistry-climate model, Global/Regional Integrated Model system Chemistry Climate Model (GRIMs-CCM), developed by coupling the chemistry modules of the GEOS-Chem chemical transport model to the GRIMs general circulation model. The GRIMs-CCM is driven by meteorological variables simulated by the GRIMs and uses simulated gas and aerosol concentrations to calculate the radiative transfer equations at each time step. The model is evaluated by comparing ozone and aerosol concentrations with respective observations from the surface networks and the satellite datasets. It is found that the GRIMs-CCM successfully reproduces the observed spatial distributions of annual-mean aerosol optical depth and captures the seasonal and latitudinal variations of total column ozone. The evaluation of simulated aerosols in surface air against the observations reveals that the model reproduces the observed temporal and spatial variations but shows biases in soil dust aerosols. We also estimate the climatic impact of aerosols by conducting two sets of 10-year simulations for the preindustrial and present conditions. The GRIMs-CCM shows the aerosol radiative forcing of − 0.30 W m−2 from the preindustrial to present-day climates, comparable to the values from other climate model intercomparison projects. These results suggest that the GRIMs-CCM is suitable for studying chemistry-climate interactions and their changes over time.

Modeling the Transport and Deposition of 10Be Produced by the Strongest Solar Proton Event During the Holocene

AbstractProminent excursions in the number of cosmogenic nuclides (e.g., 10Be) around 774 CE/775 document the most severe solar proton event (SPE) throughout the Holocene. Its manifestation in ice cores is valuable for geochronology, but also for solar‐terrestrial physics and climate modeling. Using the ECHAM/MESSy Atmospheric Chemistry (EMAC) climate model in combination with the Warning System for Aviation Exposure to SEP (WASAVIES), we investigate the transport, mixing, and deposition of the cosmogenic nuclide 10Be produced by the 774 CE/775 SPE. By comparing the model results to the reconstructed 10Be time series from four ice core records, we study the atmospheric pathways of 10Be from its stratospheric source to its sink at Earth's surface. The reconstructed post‐SPE evolution of the 10Be surface fluxes at the ice core sites is well captured by the model. The downward transport of the 10Be atoms is controlled by the Brewer‐Dobson circulation in the stratosphere and cross‐tropopause transport via tropopause folds or large‐scale sinking. Clear hemispheric differences in the transport and deposition processes are identified. In both polar regions the 10Be surface fluxes peak in summertime, with a larger influence of wet deposition on the seasonal 10Be surface flux in Greenland than in Antarctica. Differences in the peak 10Be surface flux following the 774 CE/775 SPE at the drilling sites are explained by specific meteorological conditions depending on the geographic locations of the sites.