Coupled Chemistry Climate Model Research Articles

Empirical Model of SSUSI‐Derived Auroral Ionization Rates

AbstractWe present an empirical model for auroral (90–150 km) electron–ion pair production rates, ionization rates for short, derived from Special Sensor Ultraviolet Spectrographic Imager electron energy and flux data. Using the Fang et al. (2010, https://doi.org/10.1029/2010gl045406) parametrization for mono‐energetic electrons, and the NRLMSISE‐00 neutral atmosphere model (Picone et al., 2002, https://doi.org/10.1029/2002ja009430), the calculated ionization rate profiles are binned in 2‐hr magnetic local time and 3.6°geomagnetic latitude to yield time series of ionization rates at 5‐km altitude steps. We fit each of these time series to the geomagnetic indices Kp, PC, and Ap, the 81‐day averaged solar radio flux index, and a constant term. The resulting empirical model can easily be incorporated into coupled chemistry–climate models to include particle precipitation effects.

Impact of Infrared Atmospheric Sounding Interferometer (IASI) thermal infrared measurements on global ozone reanalyses

Abstract. The information content of thermal infrared measurements for tropospheric ozone (O3) estimation has already been well demonstrated. However, the impact of such measurements to constrain modelled O3 distributions within global assimilation systems is not yet unequivocal. A new tropospheric O3 reanalysis is computed for the year 2010 by means of assimilating measurements from the Infrared Atmospheric Sounding Interferometer (IASI) within the MOdéle pour la Chimie Á Grande Echelle (MOCAGE) chemical transport model. The objective is to evaluate the impact of recent methodological improvements of the data assimilation scheme on the O3 distribution. The new O3 reanalysis (named IASI-r) and its precursor (IASI-a) have been validated against ozonesondes, and compared to independent estimations of tropospheric O3 and to results from two state-of-the-art products based on detailed tropospheric chemistry (the Goddard Earth Observing System with a coupled chemistry–climate model, GEOS-CCM, and the Copernicus Atmosphere Monitoring Service, CAMS, reanalysis). The main difference between IASI-r and IASI-a concerns the treatment of IASI observations, with radiances being assimilated directly in IASI-r instead of intermediate Level 2 O3 retrievals. IASI-r is found to correct major issues with IASI-a, such as the neutral or negative impact of IASI assimilation in the extra-tropics and the presence of residual biases in the tropics. IASI-r also compares relatively well to the CAMS reanalysis, which is based on a more comprehensive chemical mechanism and the assimilation of several ultraviolet (UV) and microwave measurements.

Persistence of flare-driven atmospheric chemistry on rocky habitable zone worlds

Low-mass stars show evidence of vigorous magnetic activity in the form of large flares and coronal mass ejections. Such space weather events may have important ramifications for the habitability and observational fingerprints of exoplanetary atmospheres. Here, using a suite of three-dimensional coupled chemistry–climate model simulations, we explore effects of time-dependent stellar activity on rocky planet atmospheres orbiting G, K and M dwarf stars. We employ observed data from the MUSCLES campaign and the Transiting Exoplanet Survey Satellite and test a range of rotation period, magnetic field strength and flare frequency assumptions. We find that recurring flares drive the atmospheres of planets around K and M dwarfs into chemical equilibria that substantially deviate from their pre-flare regimes, whereas the atmospheres of G dwarf planets quickly return to their baseline states. Interestingly, simulated O2-poor and O2-rich atmospheres experiencing flares produce similar mesospheric nitric oxide abundances, suggesting that stellar flares can highlight otherwise undetectable chemical species. Applying a radiative transfer model to our chemistry–climate model results, we find that flare-driven transmission features of bio-indicating chemical species, such as nitrogen dioxide, nitrous oxide and nitric acid, show particular promise for detection by future instruments.

Correcting model biases of CO in East Asia: impact on oxidant distributions during KORUS-AQ

Global coupled chemistry-climate models underestimate carbon monoxide (CO) in the Northern Hemisphere, exhibiting a pervasive negative bias against measurements peaking in late winter and early spring. While this bias has been commonly attributed to underestimation of direct anthropogenic and biomass burning emissions, chemical production and loss via OH reaction from emissions of anthropogenic and biogenic volatile organic compounds (VOCs) play an important role. Here we investigate the reasons for this underestimation using aircraft measurements taken in May and June 2016 from the Korea-United States Air Quality (KORUS-AQ) experiment in South Korea and the Air Chemistry Research in Asia (ARIAs) in the North China Plain (NCP). For reference, multispectral CO retrievals (V8J) from the Measurements of Pollution in the Troposphere (MOPITT) are jointly assimilated with meteorological observations using an ensemble adjustment Kalman filter (EAKF) within the global Community Atmosphere Model with Chemistry (CAM-Chem) and the Data Assimilation Research Testbed (DART). With regard to KORUS-AQ data, CO is underestimated by 42% in the control run and by 12% with the MOPITT assimilation run. The inversion suggests an underestimation of anthropogenic CO sources in many regions, by up to 80% for northern China, with large increments over the Liaoning Province and the North China Plain (NCP). Yet, an often-overlooked aspect of these inversions is that correcting the underestimation in anthropogenic CO emissions also improves the comparison with observational O3 datasets and observationally constrained box model simulations of OH and HO2. Running a CAM-Chem simulation with the updated emissions of anthropogenic CO reduces the bias by 29% for CO, 18% for ozone, 11% for HO2, and 27% for OH. Longer-lived anthropogenic VOCs whose model errors are correlated with CO are also improved, while short-lived VOCs, including formaldehyde, are difficult to constrain solely by assimilating satellite retrievals of CO. During an anticyclonic episode, better simulation of O3, with an average underestimation of 5.5 ppbv, and a reduction in the bias of surface formaldehyde and oxygenated VOCs can be achieved by separately increasing by a factor of 2 the modeled biogenic emissions for the plant functional types found in Korea. Results also suggest that controlling VOC and CO emissions, in addition to widespread NO x controls, can improve ozone pollution over East Asia.

Extending the Modular Earth Submodel System (MESSy v2.54) model hierarchy: the ECHAM/MESSy IdeaLized (EMIL) model setup

Abstract. As models of the Earth system grow in complexity, a need emerges to connect them with simplified systems through model hierarchies in order to improve process understanding. The Modular Earth Submodel System (MESSy) was developed to incorporate chemical processes into an Earth System model. It provides an environment to allow for model configurations and setups of varying complexity, and as of now the hierarchy ranges from a chemical box model to a fully coupled chemistry–climate model. Here, we present a newly implemented dry dynamical core model setup within the MESSy framework, denoted as ECHAM/MESSy IdeaLized (EMIL) model setup. EMIL is developed with the aim to provide an easily accessible idealized model setup that is consistently integrated in the MESSy model hierarchy. The implementation in MESSy further enables the utilization of diagnostic chemical tracers. The setup is achieved by the implementation of a new submodel for relaxation of temperature and horizontal winds to given background values, which replaces all other “physics” submodels in the EMIL setup. The submodel incorporates options to set the needed parameters (e.g., equilibrium temperature, relaxation time and damping coefficient) to functions used frequently in the past. This study consists of three parts. In the first part, test simulations with the EMIL model setup are shown to reproduce benchmarks provided by earlier dry dynamical core studies. In the second part, the sensitivity of the coupled troposphere–stratosphere dynamics to various modifications of the setup is studied. We find a non-linear response of the polar vortex strength to the prescribed meridional temperature gradient in the extratropical stratosphere that is indicative of a regime transition. In agreement with earlier studies, we find that the tropospheric jet moves poleward in response to the increase in the polar vortex strength but at a rate that strongly depends on the specifics of the setup. When replacing the idealized topography to generate planetary waves by mid-tropospheric wave-like heating, the response of the tropospheric jet to changes in the polar vortex is strongly damped in the free troposphere. However, near the surface, the jet shifts poleward at a higher rate than in the topographically forced simulations. Those results indicate that the wave-like heating might have to be used with care when studying troposphere–stratosphere coupling. In the third part, examples for possible applications of the model system are presented. The first example involves simulations with simplified chemistry to study the impact of dynamical variability and idealized changes on tracer transport, and the second example involves simulations of idealized monsoon circulations forced by localized heating. The ability to incorporate passive and chemically active tracers in the EMIL setup demonstrates the potential for future studies of tracer transport in the idealized dynamical model.

Impacts of Stratospheric Ozone Extremes on Arctic High Cloud

AbstractStratospheric ozone depletion in the Antarctic is well known to cause changes in Southern Hemisphere tropospheric climate; however, because of its smaller magnitude in the Arctic, the effects of stratospheric ozone depletion on Northern Hemisphere tropospheric climate are not as obvious or well understood. Recent research using both global climate models and observational data has determined that the impact of ozone depletion on ozone extremes can affect interannual variability in tropospheric circulation in the Northern Hemisphere in spring. To further this work, we use a coupled chemistry–climate model to examine the difference in high cloud between years with anomalously low and high Arctic stratospheric ozone concentrations. We find that low ozone extremes during the late twentieth century, when ozone-depleting substances (ODS) emissions are higher, are related to a decrease in upper tropospheric stability and an increase in high cloud fraction, which may contribute to enhanced Arctic surface warming in spring through a positive longwave cloud radiative effect. A better understanding of how Arctic climate is affected by ODS emissions, ozone depletion, and ozone extremes will lead to improved predictions of Arctic climate and its associated feedbacks with atmospheric fields as ozone levels recover.

Added Value of Aerosol-Cloud Interactions for Representing Aerosol Optical Depth in an Online Coupled Climate-Chemistry Model over Europe

Aerosol-cloud interactions (ACI) represent one of the most important sources of uncertainties in climate modelling. In this sense, realistic simulations of ACI are needed for a better understanding of the complex interactions between air pollution and the climate system. This work quantifies the added value of including ACI in an online coupled climate/chemistry model (WRF-Chem, 0.44 ∘ horizontal resolution, years 2003 to 2010) in order to assess whether there is an improvement in the representation of aerosol optical depth (AOD). Modelling results for each species have been evaluated against the Copernicus Atmosphere Monitoring Service (CAMS) reanalysis, and AOD at 675 nm has been compared to AERONET data. Results indicate that the improvements of the monthly biases are around 8% for total AOD550 when including ACI, reaching 20% for the monthly bias in AOD550 coming from dust. Moreover, the temporal representation of AOD550 largely improves (increase in the Pearson time correlation coefficients), ranging from 6% to 20% depending on the chemical species considered. The benefits from this improvement overcome the problems derived from the high computational time required in ACI simulations (eight times higher with respect to simulations not including aerosol-cloud interactions).

Local and remote mean and extreme temperature response to regional aerosol emissions reductions

Abstract. The climatic implications of regional aerosol and precursor emissions reductions implemented to protect human health are poorly understood. We investigate the mean and extreme temperature response to regional changes in aerosol emissions using three coupled chemistry–climate models: NOAA GFDL CM3, NCAR CESM1, and NASA GISS-E2. Our approach contrasts a long present-day control simulation from each model (up to 400 years with perpetual year 2000 or 2005 emissions) with 14 individual aerosol emissions perturbation simulations (160–240 years each). We perturb emissions of sulfur dioxide (SO2) and/or carbonaceous aerosol within six world regions and assess the statistical significance of mean and extreme temperature responses relative to internal variability determined by the control simulation and across the models. In all models, the global mean surface temperature response (perturbation minus control) to SO2 and/or carbonaceous aerosol is mostly positive (warming) and statistically significant and ranges from +0.17 K (Europe SO2) to −0.06 K (US BC). The warming response to SO2 reductions is strongest in the US and Europe perturbation simulations, both globally and regionally, with Arctic warming up to 1 K due to a removal of European anthropogenic SO2 emissions alone; however, even emissions from regions remote to the Arctic, such as SO2 from India, significantly warm the Arctic by up to 0.5 K. Arctic warming is the most robust response across each model and several aerosol emissions perturbations. The temperature response in the Northern Hemisphere midlatitudes is most sensitive to emissions perturbations within that region. In the tropics, however, the temperature response to emissions perturbations is roughly the same in magnitude as emissions perturbations either within or outside of the tropics. We find that climate sensitivity to regional aerosol perturbations ranges from 0.5 to 1.0 K (W m−2)−1 depending on the region and aerosol composition and is larger than the climate sensitivity to a doubling of CO2 in two of three models. We update previous estimates of regional temperature potential (RTP), a metric for estimating the regional temperature responses to a regional emissions perturbation that can facilitate assessment of climate impacts with integrated assessment models without requiring computationally demanding coupled climate model simulations. These calculations indicate a robust regional response to aerosol forcing within the Northern Hemisphere midlatitudes, regardless of where the aerosol forcing is located longitudinally. We show that regional aerosol perturbations can significantly increase extreme temperatures on the regional scale. Except in the Arctic in the summer, extreme temperature responses largely mirror mean temperature responses to regional aerosol perturbations through a shift of the temperature distributions and are mostly dominated by local rather than remote aerosol forcing.

Global ozone depletion and increase of UV radiation caused by pre-industrial tropical volcanic eruptions

Large explosive tropical volcanic eruptions inject high amounts of gases into the stratosphere, where they disperse globally through the large-scale meridional circulation. There is now increasing observational evidence that volcanic halogens can reach the upper troposphere and lower stratosphere. Here, we present the first study that combines measurement-based data of sulfur, chlorine and bromine releases from tropical volcanic eruptions with complex coupled chemistry climate model simulations taking radiative-dynamical-chemical feedbacks into account. Halogen model input parameters represent a size-time-region-wide average for the Central American eruptions over the last 200 ka ensuring a comprehensive perspective. The simulations reveal global, long-lasting impact on the ozone layer affecting atmospheric composition and circulation for a decade. Column ozone drops below 220 DU (ozone hole conditions) in the tropics, Arctic and Antarctica, increasing biologically active UV by 80 to 400%. Our model results could potentially be validated using high-resolution proxies from ice cores and pollen records.

Prescribing Zonally Asymmetric Ozone Climatologies in Climate Models: Performance Compared to a Chemistry-Climate Model.

Three different methods of specifying ozone in an atmosphere‐only version of the HadGEM3‐A global circulation model are compared to the coupled chemistry configuration of this model. These methods include a specified zonal‐mean ozone climatology, a specified 3‐D ozone climatology, and a calculated‐asymmetry scheme in which a specified zonal‐mean ozone field is adapted online to be consistent with dynamically produced zonal asymmetries. These simulations all use identical boundary conditions and, by construction, have the same climatological zonal‐mean ozone, that of the coupled chemistry configuration of the model. Prescribing ozone, regardless of scheme, results in a simulation which is 3–4 times faster than the coupled chemistry‐climate model (CCM). Prescribing climatological zonal asymmetries leads to a vortex which is the correct intensity but which is systematically displaced over regions with lower prescribed ozone. When zonal asymmetries in ozone are free to evolve interactively with model dynamics, the modeled wintertime stratospheric vortex shape and mean sea level pressure patterns closely resemble that produced by the full CCM in both hemispheres, in terms of statistically significant differences. Further, we separate out the two distinct pathways by which zonal ozone asymmetries influence modeled dynamics. We present this interactive‐ozone zonal‐asymmetry scheme as an inexpensive tool for accurately modeling the impacts of dynamically consistent ozone fields as seen in a CCM which ultimately influence mean sea level pressure and tropospheric circulation (particularly during wintertime in the Northern Hemisphere, when ozone asymmetries are generally largest), without the computational burden of simulating interactive chemistry.

Connecting regional aerosol emissions reductions to local and remote precipitation responses

Abstract. The unintended climatic implications of aerosol and precursor emission reductions implemented to protect public health are poorly understood. We investigate the precipitation response to regional changes in aerosol emissions using three coupled chemistry–climate models: NOAA Geophysical Fluid Dynamics Laboratory Coupled Model 3 (GFDL-CM3), NCAR Community Earth System Model (CESM1), and NASA Goddard Institute for Space Studies ModelE2 (GISS-E2). Our approach contrasts a long present-day control simulation from each model (up to 400 years with perpetual year 2000 or 2005 emissions) with 14 individual aerosol emissions perturbation simulations (160–240 years each). We perturb emissions of sulfur dioxide and/or carbonaceous aerosol within six world regions and assess the significance of precipitation responses relative to internal variability determined by the control simulation and across the models. Global and regional precipitation mostly increases when we reduce regional aerosol emissions in the models, with the strongest responses occurring for sulfur dioxide emissions reductions from Europe and the United States. Precipitation responses to aerosol emissions reductions are largest in the tropics and project onto the El Niño–Southern Oscillation (ENSO). Regressing precipitation onto an Indo-Pacific zonal sea level pressure gradient index (a proxy for ENSO) indicates that the ENSO component of the precipitation response to regional aerosol removal can be as large as 20 % of the total simulated response. Precipitation increases in the Sahel in response to aerosol reductions in remote regions because an anomalous interhemispheric temperature gradient alters the position of the Intertropical Convergence Zone (ITCZ). This mechanism holds across multiple aerosol reduction simulations and models.

Quantifying the effect of mixing on the mean age of air in CCMVal-2 and CCMI-1 models

Abstract. The stratospheric age of air (AoA) is a useful measure of the overall capabilities of a general circulation model (GCM) to simulate stratospheric transport. Previous studies have reported a large spread in the simulation of AoA by GCMs and coupled chemistry–climate models (CCMs). Compared to observational estimates, simulated AoA is mostly too low. Here we attempt to untangle the processes that lead to the AoA differences between the models and between models and observations. AoA is influenced by both mean transport by the residual circulation and two-way mixing; we quantify the effects of these processes using data from the CCM inter-comparison projects CCMVal-2 (Chemistry–Climate Model Validation Activity 2) and CCMI-1 (Chemistry–Climate Model Initiative, phase 1). Transport along the residual circulation is measured by the residual circulation transit time (RCTT). We interpret the difference between AoA and RCTT as additional aging by mixing. Aging by mixing thus includes mixing on both the resolved and subgrid scale. We find that the spread in AoA between the models is primarily caused by differences in the effects of mixing and only to some extent by differences in residual circulation strength. These effects are quantified by the mixing efficiency, a measure of the relative increase in AoA by mixing. The mixing efficiency varies strongly between the models from 0.24 to 1.02. We show that the mixing efficiency is not only controlled by horizontal mixing, but by vertical mixing and vertical diffusion as well. Possible causes for the differences in the models' mixing efficiencies are discussed. Differences in subgrid-scale mixing (including differences in advection schemes and model resolutions) likely contribute to the differences in mixing efficiency. However, differences in the relative contribution of resolved versus parameterized wave forcing do not appear to be related to differences in mixing efficiency or AoA.

Downward Wave Coupling between the Stratosphere and Troposphere under Future Anthropogenic Climate Change

AbstractDownward wave coupling (DWC) is an important process that characterizes the dynamical coupling between the stratosphere and troposphere via planetary wave reflection. A recent modeling study has indicated that natural forcing factors, including sea surface temperature (SST) variability and the quasi-biennial oscillation (QBO), influence DWC and the associated surface impact in the Northern Hemisphere (NH). In light of this, the authors further investigate how DWC in the NH is affected by anthropogenic forcings, using a fully coupled chemistry–climate model CESM1(WACCM). The results indicate that the occurrence of DWC is significantly suppressed in the future, starting later in the seasonal cycle, with more events concentrated in late winter (February and March). The future decrease in DWC events is associated with enhanced wave absorption in the stratosphere due to increased greenhouse gases (GHGs), which is manifest as more absorbing types of stratospheric sudden warmings (SSWs) in early winter. This early winter condition leads to a delay in the development of the upper-stratospheric reflecting surface, resulting in a shift in the seasonal cycle of DWC toward late winter in the future. The tropospheric responses to DWC events in the future exhibit different spatial patterns, compared to those of the past. In the North Atlantic sector, DWC-induced circulation changes are characterized by a poleward shift and an eastward extension of the tropospheric jet, while in the North Pacific sector, the circulation changes are characterized by a weakening of the tropospheric jet. These responses are consistent with a change in the pattern of DWC-induced synoptic-scale eddy–mean flow interaction in the future.

An assessment of aerosol optical properties from remote-sensing observations and regional chemistry–climate coupled models over Europe

Abstract. Atmospheric aerosols modify the radiative budget of the Earth due to their optical, microphysical and chemical properties, and are considered one of the most uncertain climate forcing agents. In order to characterise the uncertainties associated with satellite and modelling approaches to represent aerosol optical properties, mainly aerosol optical depth (AOD) and Ångström exponent (AE), their representation by different remote-sensing sensors and regional online coupled chemistry–climate models over Europe are evaluated. This work also characterises whether the inclusion of aerosol–radiation (ARI) or/and aerosol–cloud interactions (ACI) help improve the skills of modelling outputs.Two case studies were selected within the EuMetChem COST Action ES1004 framework when important aerosol episodes in 2010 all over Europe took place: a Russian wildfire episode and a Saharan desert dust outbreak that covered most of the Mediterranean Sea. The model data came from different regional air-quality–climate simulations performed by working group 2 of EuMetChem, which differed according to whether ARI or ACI was included or not. The remote-sensing data came from three different sensors: MODIS, OMI and SeaWIFS. The evaluation used classical statistical metrics to first compare satellite data versus the ground-based instrument network (AERONET) and then to evaluate model versus the observational data (both satellite and ground-based data).Regarding the uncertainty in the satellite representation of AOD, MODIS presented the best agreement with the AERONET observations compared to other satellite AOD observations. The differences found between remote-sensing sensors highlighted the uncertainty in the observations, which have to be taken into account when evaluating models. When modelling results were considered, a common trend for underestimating high AOD levels was observed. For the AE, models tended to underestimate its variability, except when considering a sectional approach in the aerosol representation. The modelling results showed better skills when ARI+ACI interactions were included; hence this improvement in the representation of AOD (above 30 % in the model error) and AE (between 20 and 75 %) is important to provide a better description of aerosol–radiation–cloud interactions in regional climate models.

Chemical Feedback From Decreasing Carbon Monoxide Emissions

AbstractUnderstanding changes in the burden and growth rate of atmospheric methane (CH4) has been the focus of several recent studies but still lacks scientific consensus. Here we investigate the role of decreasing anthropogenic carbon monoxide (CO) emissions since 2002 on hydroxyl radical (OH) sinks and tropospheric CH4 loss. We quantify this impact by contrasting two model simulations for 2002–2013: (1) a Measurement of the Pollution in the Troposphere (MOPITT) CO reanalysis and (2) a Control‐Run without CO assimilation. These simulations are performed with the Community Atmosphere Model with Chemistry of the Community Earth System Model fully coupled chemistry climate model with prescribed CH4 surface concentrations. The assimilation of MOPITT observations constrains the global CO burden, which significantly decreased over this period by ~20%. We find that this decrease results to (a) increase in CO chemical production, (b) higher CH4 oxidation by OH, and (c) ~8% shorter CH4 lifetime. We elucidate this coupling by a surrogate mechanism for CO‐OH‐CH4 that is quantified from the full chemistry simulations.

Efficient Isoprene Secondary Organic Aerosol Formation from a Non-IEPOX Pathway.

With a large global emission rate and high reactivity, isoprene has a profound effect upon atmospheric chemistry and composition. The atmospheric pathways by which isoprene converts to secondary organic aerosol (SOA) and how anthropogenic pollutants such as nitrogen oxides and sulfur affect this process are subjects of intense research because particles affect Earth's climate and local air quality. In the absence of both nitrogen oxides and reactive aqueous seed particles, we measure SOA mass yields from isoprene photochemical oxidation of up to 15%, which are factors of 2 or more higher than those typically used in coupled chemistry climate models. SOA yield is initially constant with the addition of increasing amounts of nitric oxide (NO) but then sharply decreases for input concentrations above 50 ppbv. Online measurements of aerosol molecular composition show that the fate of second-generation RO2 radicals is key to understanding the efficient SOA formation and the NOx-dependent yields described here and in the literature. These insights allow for improved quantitative estimates of SOA formation in the preindustrial atmosphere and in biogenic-rich regions with limited anthropogenic impacts and suggest that a more-complex representation of NOx-dependent SOA yields may be important in models.

Effect of methane emission increases in East Asia on atmospheric circulation and ozone

We used a fully coupled chemistry–climate model (version 3 of the Whole Atmosphere Community Climate Model, WACCM3) to investigate the effect of methane (CH4) emission increases, especially in East Asia and North America, on atmospheric temperature, circulation and ozone (O3). We show that CH4 emission increases strengthen westerly winds in the Northern Hemisphere midlatitudes, accelerate the Brewer–Dobson (BD) circulation, and cause an increase in the mass flux across the tropopause. However, the BD circulation in the tropics between 10°S and 10°N at 100 hPa weakens as CH4 emissions increase in East Asia and strengthens when CH4 emissions increase in North America. When CH4 emissions are increased by 50% in East Asia and 15% globally, the stratospheric temperature cools by up to 0.15 K, and the stratospheric O3 increases by 45 ppbv and 60 ppbv, respectively. A 50% increase of CH4 emissions in North America (with an amplitude of stratospheric O3 increases by 60 ppbv) has a greater influence on the stratospheric O3 than the same CH4 emissions increase in East Asia. CH4 emission increases in East Asia and North America reduce the concentration of tropospheric hydroxyl radicals (4% and 2%, respectively) and increase the concentration of mid-tropospheric O3 (5% and 4%, respectively) in the Northern Hemisphere midlatitudes. When CH4 emissions increase in East Asia, the increase in the tropospheric O3 concentration is largest in August. When CH4 emissions increase in North America, the increase in the O3 concentration is largest in July in the mid-troposphere, and in April in the upper troposphere.

Modelled and observed changes in aerosols and surface solar radiation over Europe between 1960 and 2009

Abstract. Substantial changes in anthropogenic aerosols and precursor gas emissions have occurred over recent decades due to the implementation of air pollution control legislation and economic growth. The response of atmospheric aerosols to these changes and the impact on climate are poorly constrained, particularly in studies using detailed aerosol chemistry–climate models. Here we compare the HadGEM3-UKCA (Hadley Centre Global Environment Model-United Kingdom Chemistry and Aerosols) coupled chemistry–climate model for the period 1960–2009 against extensive ground-based observations of sulfate aerosol mass (1978–2009), total suspended particle matter (SPM, 1978–1998), PM10 (1997–2009), aerosol optical depth (AOD, 2000–2009), aerosol size distributions (2008–2009) and surface solar radiation (SSR, 1960–2009) over Europe. The model underestimates observed sulfate aerosol mass (normalised mean bias factor (NMBF) = −0.4), SPM (NMBF = −0.9), PM10 (NMBF = −0.2), aerosol number concentrations (N30 NMBF = −0.85; N50 NMBF = −0.65; and N100 NMBF = −0.96) and AOD (NMBF = −0.01) but slightly overpredicts SSR (NMBF = 0.02). Trends in aerosol over the observational period are well simulated by the model, with observed (simulated) changes in sulfate of −68 % (−78 %), SPM of −42 % (−20 %), PM10 of −9 % (−8 %) and AOD of −11 % (−14 %). Discrepancies in the magnitude of simulated aerosol mass do not affect the ability of the model to reproduce the observed SSR trends. The positive change in observed European SSR (5 %) during 1990–2009 ("brightening") is better reproduced by the model when aerosol radiative effects (ARE) are included (3 %), compared to simulations where ARE are excluded (0.2 %). The simulated top-of-the-atmosphere aerosol radiative forcing over Europe under all-sky conditions increased by > 3.0 W m−2 during the period 1970–2009 in response to changes in anthropogenic emissions and aerosol concentrations.

The impact of polar stratospheric ozone loss on Southern Hemisphere stratospheric circulation and climate

Abstract. The impact of polar stratospheric ozone loss resulting from chlorine activation on polar stratospheric clouds is examined using a pair of model integrations run with the fully coupled chemistry climate model UM-UKCA. Suppressing chlorine activation through heterogeneous reactions is found to produce modelled ozone differences consistent with observed ozone differences between the present and pre-ozone hole period. Statistically significant high-latitude Southern Hemisphere (SH) ozone loss begins in August and peaks in October–November, with > 75% of ozone destroyed at 50 hPa. Associated with this ozone destruction is a > 12 K decrease of the lower polar stratospheric temperatures and an increase of > 6 K in the upper stratosphere. The heating components of this temperature change are diagnosed and it is found that the temperature dipole is the result of decreased short-wave heating in the lower stratosphere and increased dynamical heating in the upper stratosphere. The cooling of the polar lower stratosphere leads, through thermal wind balance, to an acceleration of the polar vortex and delays its breakdown by ~ 2 weeks. A link between lower stratospheric zonal wind speed, the vertical component of the Eliassen–Palm (EP) flux, Fz and the residual mean vertical circulation, w*, is identified. In November and December, increased westerly winds and a delay in the breakup of the polar vortex lead to increases in Fz, indicating increased wave activity entering the stratosphere and propagating to higher altitudes. The resulting increase in wave breaking, diagnosed by decreases to the EP flux divergence, drives enhanced downwelling over the polar cap. Many of the stratospheric signals modelled in this study propagate down to the troposphere, and lead to significant surface changes in December.

Stratospheric ozone depletion from future nitrous oxide increases

Abstract. We have investigated the impact of the assumed nitrous oxide (N2O) increases on stratospheric chemistry and dynamics using a series of idealized simulations with a coupled chemistry-climate model (CCM). In a future cooler stratosphere the net yield of NOy from N2O is shown to decrease in a reference run following the IPCC A1B scenario, but NOy can still be significantly increased by extra increases of N2O over 2001–2050. Over the last decade of simulations, 50% increases in N2O result in a maximal 6% reduction in ozone mixing ratios in the middle stratosphere at around 10 hPa and an average 2% decrease in the total ozone column (TCO) compared with the control run. This enhanced destruction could cause an ozone decline in the first half of this century in the middle stratosphere around 10 hPa, while global TCO still shows an increase at the same time. The results from a multiple linear regression analysis and sensitivity simulations with different forcings show that the chemical effect of N2O increases dominates the N2O-induced ozone depletion in the stratosphere, while the dynamical and radiative effects of N2O increases are overall insignificant. The analysis of the results reveals that the ozone depleting potential of N2O varies with the time period and is influenced by the environmental conditions. For example, carbon dioxide (CO2) increases can strongly offset the ozone depletion effect of N2O.