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We conducted global simulations of temperature change due to anthropogenic trace gas emissions, which extended from the surface, through the thermosphere and ionosphere, to the exobase. These simulations were done under solar maximum conditions, in order to compare the effect of the solar cycle on global change to previous work using solar minimum conditions. The Whole Atmosphere Community Climate Model‐eXtended was employed in this study. As in previous work, lower atmosphere warming, due to increasing anthropogenic gases, is accompanied by upper atmosphere cooling, starting in the lower stratosphere, and becoming dramatic, almost 2 K per decade for the global mean annual mean, in the thermosphere. This thermospheric cooling, and consequent reduction in density, is less than the almost 3 K per decade for solar minimum conditions calculated in previous simulations. This dependence of global change on solar activity conditions is due to solar‐driven increases in radiationally active gases other than carbon dioxide, such as nitric oxide. An ancillary result of these and previous simulations is an estimate of the solar cycle effect on temperatures as a function of altitude. These simulations used modest, five‐member, ensembles, and measured sea surface temperatures rather than a fully coupled ocean model, so any solar cycle effects were not statistically significant in the lower troposphere. Temperature change from solar minimum to maximum increased from near zero at the tropopause to about 1 K at the stratopause, to approximately 500 K in the upper thermosphere, commensurate with the empirical evidence, and previous numerical models.

An advanced aerosol treatment, with a focus on semivolatile nitrate formation, is introduced into the Community Atmosphere Model version 5 with interactive chemistry (CAM5‐chem) by coupling the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) with the 7‐mode Modal Aerosol Module (MAM7). An important feature of MOSAIC is dynamic partitioning of all condensable gases to the different fine and coarse mode aerosols, as governed by mode‐resolved thermodynamics and heterogeneous chemical reactions. Applied in the free‐running mode from 1995 to 2005 with prescribed historical climatological conditions, the model simulates global distributions of sulfate, nitrate, and ammonium in good agreement with observations and previous studies. Inclusion of nitrate resulted in ∼10% higher global average accumulation mode number concentrations, indicating enhanced growth of Aitken mode aerosols from nitrate formation. While the simulated accumulation mode nitrate burdens are high over the anthropogenic source regions, the sea‐salt and dust modes respectively constitute about 74% and 17% of the annual global average nitrate burden. Regional clear‐sky shortwave radiative cooling of up to −5 W m−2 due to nitrate is seen, with a much smaller global average cooling of −0.05 W m−2. Significant enhancements in regional cloud condensation nuclei (at 0.1% supersaturation) and cloud droplet number concentrations are also attributed to nitrate, causing an additional global average shortwave cooling of −0.8 W m−2. Taking into consideration of changes in both longwave and shortwave radiation under all‐sky conditions, the net change in the top of the atmosphere radiative fluxes induced by including nitrate aerosol is −0.7 W m−2., Key Points A modal version of the advanced aerosol chemistry module MOSAIC is developed and introduced in a climate model to simulate nitrate aerosolMOSAIC provides an accurate and efficient treatment for dynamically partitioning semivolatile gases over to entire aerosol size distributionThe modeled global distribution of nitrate is in good agreement with observations and its impact on the radiative effects is quantified

This study considers the impact of electron precipitation from Earth's radiation belts on atmospheric composition using observations from the NASA Van Allen Probes and NSF Focused Investigations of Relativistic Electron Burst Intensity, Range, and Dynamics (FIREBIRD II) CubeSats. Ratios of electron flux between the Van Allen Probes (in near-equatorial orbit in the radiation belts) and FIREBIRD II (in polar low Earth orbit) during spacecraft conjunctions (2015–2017) allow an estimate of precipitation into the atmosphere. Total Radiation Belt Electron Content, calculated from Van Allen Probes RBSP-ECT MagEIS data, identifies a sustained 10-day electron loss event in March 2013 that serves as an initial case study. Atmospheric ionization profiles, calculated by integrating monoenergetic ionization rates across the precipitating electron flux spectrum, provide input to the NCAR Whole Atmosphere Community Climate Model in order to quantify enhancements of atmospheric HOx and NOx and subsequent destruction of O3 in the middle atmosphere. Results suggest that current APEEP parameterizations of radiation belt electrons used in Coupled Model Intercomparison Project may underestimate the duration of events as well as higher energy electron contributions to atmospheric ionization and modeled NOx concentrations in the mesosphere and upper stratosphere.

We report airborne measurements of acetaldehyde (CH(3)CHO) during the first and second deployments of the National Aeronautics and Space Administration (NASA) Atmospheric Tomography Mission (ATom). The budget of CH(3)CHO is examined using the Community Atmospheric Model with chemistry (CAM-chem), with a newly-developed online air-sea exchange module. The upper limit of the global ocean net emission of CH(3)CHO is estimated to be 34 Tg a(−1) (42 Tg a(−1) if considering bubble-mediated transfer), and the ocean impacts on tropospheric CH(3)CHO are mostly confined to the marine boundary layer. Our analysis suggests that there is an unaccounted CH(3)CHO source in the remote troposphere and that organic aerosols can only provide a fraction of this missing source. We propose that peroxyacetic acid (PAA) is an ideal indicator of the rapid CH(3)CHO production in the remote troposphere. The higher-than-expected CH(3)CHO measurements represent a missing sink of hydroxyl radicals (and halogen radical) in current chemistry-climate models.

We describe here changes in stratospheric dynamics and chemistry in a first century‐long sulfate aerosol geoengineering simulation in which the mean surface temperature and the interhemispheric and equator‐to‐pole surface temperature gradients were kept near their 2020 levels despite the RCP8.5 emission scenario. Simulations were carried out with the Community Earth System Model, version 1 with the Whole Atmosphere Community Climate Model as its atmospheric component [CESM1(WACCM)] coupled to a feedback algorithm controlling the magnitude of sulfur dioxide (SO_2) injections at four injection latitudes. We find that, throughout the entire geoengineering simulation, the lower stratospheric temperatures increase by ∼0.19 K per Tg SO_2 injection per year or ∼10 K with ∼40 Tg SO_2/year total SO_2 injection. These temperature changes are associated with a strengthening of the polar jets in the stratosphere and weakening of the mean zonal wind in the lower stratosphere subtropics and throughout the troposphere, associated with weaker storm track activity. In the geoengineering simulation the quasi‐biennial oscillation of the tropical lower stratospheric winds remains close to the presently observed quasi‐biennial oscillation, even for large amounts of SO2 injection. Water vapor in the stratosphere increases substantially: by 25% with ∼20 Tg SO_2/year annual injection and by up to 90% with a ∼40 Tg SO_2/year injection. Stratospheric column ozone in the geoengineering simulation is predicted to recover to or supersede preozone hole conditions by the end of the century.

Strategically applied geoengineering is proposed to reduce some of the known side effects of stratospheric aerosol modifications. Specific climate goals could be reached depending on design choices of stratospheric sulfur injections by latitude, altitude, and magnitude. Here we explore in detail the stratospheric chemical and dynamical responses to injections at different altitudes using a fully coupled Earth System Model. Two different scenarios are explored that produce approximately the same global cooling of 2°C over the period 2042–2049, a high‐altitude injection case using 24 Tg SO_2/year at 30 hPa (≈25‐km altitude) and a low‐altitude injection case using 32 Tg SO_2/year injections at 70 hPa (between 19‐ and 20‐km altitude), with annual injections divided equally between 15°N and 15°S. Both cases result in a warming of the lower tropical stratosphere up to 10 and 15°C for the high‐ and low‐altitude injection case and in substantial increases of stratospheric water vapor of up to 2 and 4 ppm, respectively, compared to no geoengineering conditions. Polar column ozone in the Northern Hemisphere is reduced by up to 18% in March for the high‐altitude injection case and up to 8% for the low‐altitude injection case. However, for winter middle and high northern latitudes, low‐altitude injections result in greater column ozone values than without geoengineering. These changes are mostly driven by dynamics and advection. Antarctic column ozone in 2042–2049 does not recover from present‐day (2002–2009) values for both cases.

We simulated anthropogenic global change through the entire atmosphere, including the thermosphere and ionosphere, using the Whole Atmosphere Community Climate Model‐eXtended. The basic result was that even as the lower atmosphere gradually warms, the upper atmosphere rapidly cools. The simulations employed constant low solar activity conditions, to remove the effects of variable solar and geomagnetic activity. Global mean annual mean temperature increased at a rate of +0.2 K/decade at the surface and +0.4 K/decade in the upper troposphere but decreased by about −1 K/decade in the stratosphere‐mesosphere and −2.8 K/decade in the thermosphere. Near the mesopause, temperature decreases were small compared to the interannual variation, so trends in that region are uncertain. Results were similar to previous modeling confined to specific atmospheric levels and compared favorably with available measurements. These simulations demonstrate the ability of a single comprehensive numerical model to characterize global change throughout the atmosphere.

We discuss and evaluate the representation of atmospheric chemistry in the global Community Atmosphere Model (CAM) version 4, the atmospheric component of the Community Earth System Model (CESM). We present a variety of configurations for the representation of tropospheric and stratospheric chemistry, wet removal, and online and offline meteorology. Results from simulations illustrating these configurations are compared with surface, aircraft and satellite observations. Major biases include a negative bias in the high-latitude CO distribution, a positive bias in upper-tropospheric/lower-stratospheric ozone, and a positive bias in summertime surface ozone (over the United States and Europe). The tropospheric net chemical ozone production varies significantly between configurations, partly related to variations in stratosphere-troposphere exchange. Aerosol optical depth tends to be underestimated over most regions, while comparison with aerosol surface measurements over the United States indicate reasonable results for sulfate , especially in the online simulation. Other aerosol species exhibit significant biases. Overall, the model-data comparison indicates that the offline simulation driven by GEOS5 meteorological analyses provides the best simulation, possibly due in part to the increased vertical resolution (52 levels instead of 26 for online dynamics). The CAM-chem code as described in this paper, along with all the necessary datasets needed to perform the simulations described here, are available for download at www.cesm.ucar.edu.

Key developments have been made to the NCAR Whole Atmosphere Community Climate Model with thermosphere and ionosphere extension (WACCM‐X). Among them, the most important are the self‐consistent solution of global electrodynamics, and transport of O+ in the F‐region. Other ionosphere developments include time‐dependent solution of electron/ion temperatures, metastable O+ chemistry, and high‐cadence solar EUV capability. Additional developments of the thermospheric components are improvements to the momentum and energy equation solvers to account for variable mean molecular mass and specific heat, a new divergence damping scheme, and cooling by O(3P) fine structure. Simulations using this new version of WACCM‐X (2.0) have been carried out for solar maximum and minimum conditions. Thermospheric composition, density, and temperatures are in general agreement with measurements and empirical models, including the equatorial mass density anomaly and the midnight density maximum. The amplitudes and seasonal variations of atmospheric tides in the mesosphere and lower thermosphere are in good agreement with observations. Although global mean thermospheric densities are comparable with observations of the annual variation, they lack a clear semiannual variation. In the ionosphere, the low‐latitude E × B drifts agree well with observations in their magnitudes, local time dependence, seasonal, and solar activity variations. The prereversal enhancement in the equatorial region, which is associated with ionospheric irregularities, displays patterns of longitudinal and seasonal variation that are similar to observations. Ionospheric density from the model simulations reproduces the equatorial ionosphere anomaly structures and is in general agreement with observations. The model simulations also capture important ionospheric features during storms.

We investigate atomic hydrogen (H) variability from the mesopause to the upper thermosphere, on time scales of solar cycle, seasonal, and diurnal, using measurements made by the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) instrument on the Thermosphere Ionosphere Mesosphere Energetics Dynamics satellite, and simulations by the National Center for Atmospheric Research Whole Atmosphere Community Climate Model‐eXtended (WACCM‐X). In the mesopause region (85 to 95 km), the seasonal and solar cycle variations of H simulated by WACCM‐X are consistent with those from SABER observations: H density is higher in summer than in winter, and slightly higher at solar minimum than at solar maximum. However, mesopause region H density from the Mass‐Spectrometer‐Incoherent‐Scatter (National Research Laboratory Mass‐Spectrometer‐Incoherent‐Scatter 00 (NRLMSISE‐00)) empirical model has reversed seasonal variation compared to WACCM‐X and SABER. From the mesopause to the upper thermosphere, H density simulated by WACCM‐X switches its solar cycle variation twice, and seasonal dependence once, and these changes of solar cycle and seasonal variability occur in the lower thermosphere (~95 to 130 km), whereas H from NRLMSISE‐00 does not change solar cycle and seasonal dependence from the mesopause through the thermosphere. In the upper thermosphere (above 150 km), H density simulated by WACCM‐X is higher at solar minimum than at solar maximum, higher in winter than in summer, and also higher during nighttime than daytime. The amplitudes of these variations are on the order of factors of ~10, ~2, and ~2, respectively. This is consistent with NRLMSISE‐00.

The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. The main focus of this paper is to compare the performance of configurations with internally derived "free running" (FR) meteorology and "specified dynamics" (SD) against observations from surface, aircraft, and satellite, as well as understand the origin of the identified differences. We focus on the representation of aerosols and chemistry. All model configurations reproduce tropospheric ozone for most regions based on in situ and satellite observations. However, shortcomings exist in the representation of ozone precursors and aerosols. Tropospheric ozone in all model configurations agrees for the most part with ozonesondes and satellite observations in the tropics and the Northern Hemisphere within the variability of the observations. Southern hemispheric tropospheric ozone is consistently underestimated by up to 25%. Differences in convection and stratosphere to troposphere exchange processes are mostly responsible for differences in ozone in the different model configurations. Carbon monoxide (CO) and other volatile organic compounds are largely underestimated in Northern Hemisphere mid-latitudes based on satellite and aircraft observations. Nitrogen oxides (NOx) are biased low in the free tropical troposphere, whereas peroxyacetyl nitrate (PAN) is overestimated in particular in high northern latitudes. The present-day methane lifetime estimates are compared among the different model configurations. These range between 7.8 years in the SD configuration of CAM5-chem and 8.8 years in the FR configuration of CAM4-chem and are therefore underestimated compared to observational estimations. We find that differences in tropospheric aerosol surface area between CAM4 and CAM5 play an important role in controlling the burden of the tropical tropospheric hydroxyl radical (OH), which causes differences in tropical methane lifetime of about half a year between CAM4-chem and CAM5-chem. In addition, different distributions of NOx from lightning explain about half of the difference between SD and FR model versions in both CAM4-chem and CAM5-chem. Remaining differences in the tropical OH burden are due to enhanced tropical ozone burden in SD configurations compared to the FR versions, which are not only caused by differences in chemical production or loss but also by transport and mixing. For future studies, we recommend the use of CAM5-chem configurations, due to improved aerosol description and inclusion of aerosol–cloud interactions. However, smaller tropospheric surface area density in the current version of CAM5-chem compared to CAM4-chem results in larger oxidizing capacity in the troposphere and therefore a shorter methane lifetime.

The Antarctic ozone hole will continue to be observed in the next 35–50 years, although the emissions of chlorofluorocarbons (CFCs) have gradually been phased out during the last two decades. In this paper, we suggest a geo-engineering approach that will remove substantial amounts of hydrogen chloride (HCl) from the lower stratosphere in fall, and hence limit the formation of the Antarctic ozone hole in late winter and early spring. HCl will be removed by ice from the atmosphere at temperatures higher than the threshold under which polar stratospheric clouds (PSCs) are formed if sufficiently large amounts of ice are supplied to produce water saturation. A detailed chemical-climate numerical model is used to assess the expected efficiency of the proposed geo-engineering method, and specifically to calculate the removal of HCl by ice particles. The size of ice particles appears to be a key parameter: larger particles (with a radius between 10 and 100 µm) appear to be most efficient for removing HCl. Sensitivity studies lead to the conclusions that the ozone recovery is effective when ice particles are supplied during May and June in the latitude band ranging from 70°S to 90°S and in the altitude layer ranging from 10 to 26 km. It appears, therefore, that supplying ice particles to the Antarctic lower stratosphere could be effective in reducing the depth of the ozone hole. In addition, photodegradation of CFCs might be accelerated when ice is supplied due to enhanced vertical transport of this efficient greenhouse gas.

Injections of sulfur dioxide into the stratosphere are among several proposed methods of solar radiation management. Such injections could cool the Earth's climate. However, they would significantly alter the dynamics of the stratosphere. We explore here the stratospheric dynamical response to sulfur dioxide injections ∼ 5 km above the tropopause at multiple latitudes (equator, 15° S, 15° N, 30° S and 30° N) using a fully coupled Earth system model, Community Earth System Model, version 1, with the Whole Atmosphere Community Climate Model as its atmospheric component (CESM1(WACCM)). We find that in all simulations, the tropical lower stratosphere warms primarily between 30° S and 30° N, regardless of injection latitude. The quasi-biennial oscillation (QBO) of the tropical zonal wind is altered by the various sulfur dioxide injections. In a simulation with a 12 Tg yr−1 equatorial injection, and with fully interactive chemistry, the QBO period lengthens to ∼ 3.5 years, but never completely disappears. However, in a simulation with specified (or non-interactive) chemical fields, including O3 and prescribed aerosols taken from the interactive simulation, the oscillation is virtually lost. In addition we find that geoengineering does not always lengthen the QBO. We further demonstrate that the QBO period changes from 24 to 12 - 17 months in simulations with sulfur dioxide injections placed poleward of the equator. Our study points to the importance of understanding and verifying of the complex interactions between aerosols, atmospheric dynamics, and atmospheric chemistry as well as understanding the effects of sulfur dioxide injections placed away from the Equator on the QBO.

We describe the first simulations of stratospheric sulfate aerosol geoengineering using multiple injection locations to meet multiple simultaneous surface temperature objectives. Simulations were performed using CESM1(WACCM), a coupled atmosphere-ocean general circulation model with fully interactive stratospheric chemistry, dynamics (including an internally generated quasi-biennial oscillation), and a sophisticated treatment of sulfate aerosol formation, microphysical growth, and deposition. The objectives are defined as maintaining three temperature features at their 2020 levels against a background of the RCP8.5 scenario over the period 2020–2099. These objectives are met using a feedback mechanism in which the rate of sulfur dioxide injection at each of the four locations is adjusted independently every year of simulation. Even in the presence of uncertainties, nonlinearities, and variability, the objectives are met, predominantly by SO_2 injection at 30°N and 30°S. By the last year of simulation, the feedback algorithm calls for a total injection rate of 51 Tg SO_2 per year. The injections are not in the tropics, which results in a greater degree of linearity of the surface climate response with injection amount than has been found in many previous studies using injection at the equator. Because the objectives are defined in terms of annual mean temperature, the required geongineering results in “overcooling” during summer and “undercooling” during winter. The hydrological cycle is also suppressed as compared to the reference values corresponding to the year 2020. The demonstration we describe in this study is an important step toward understanding what geoengineering can do and what it cannot do.

We present new insights into the evolution and interactions of stratospheric aerosol using an updated version of the Whole Atmosphere Community Climate Model (WACCM). Improved horizontal resolution, dynamics, and chemistry now produce an internally generated quasi-biennial oscillation and significant improvements to stratospheric temperatures and ozone compared to observations. We present a validation of WACCM column ozone and climate calculations against observations. The prognostic treatment of stratospheric sulfate aerosols accurately represents the evolution of stratospheric aerosol optical depth and perturbations to solar and longwave radiation following the June 1991 eruption of Mount Pinatubo. We confirm the inclusion of interactive OH chemistry as an important factor in the formation and initial distribution of aerosol following large inputs of sulfur dioxide (SO_2) to the stratosphere. We calculate that depletion of OH levels within the dense SO_2 cloud in the first weeks following the Pinatubo eruption significantly prolonged the average initial e-folding decay time for SO_2 oxidation to 47 days. Previous observational and model studies showing a 30 day decay time have not accounted for the large (30–55%) losses of SO_2 on ash and ice within 7–9 days posteruption and have not correctly accounted for OH depletion. We examine the variability of aerosol evolution in free-running climate simulations due to meteorology, with comparison to simulations nudged with specified dynamics. We assess calculated impacts of volcanic aerosols on ozone loss with comparisons to observations. The completeness of the chemistry, dynamics, and aerosol microphysics in WACCM qualify it for studies of stratospheric sulfate aerosol geoengineering.

Injection of SO_2 into the stratosphere has been proposed as a method to, in part, counteract anthropogenic climate change. So far, most studies investigated injections at the equator or in a region in the tropics. Here we use Community Earth System Model version 1 Whole Atmosphere Community Climate Model (CESM1(WACCM)) to explore the impact of continuous single grid point SO_2 injections at seven different latitudes and two altitudes in the stratosphere on aerosol distribution and climate. For each of the 14 locations, 3 different constant SO_2 emission rates were tested to identify linearity in aerosol burden, aerosol optical depth, and climate effects. We found that injections at 15°N and 15°S and at 25 km altitude have equal or greater effect on radiation and surface temperature than injections at the equator. Nonequatorial injections transport SO_2 and sulfate aerosols more efficiently into middle and high latitudes and result in particles of smaller effective radius and larger aerosol burden in middle and high latitudes. Injections at 15°S produce the largest increase in global average aerosol optical depth and increase the change in radiative forcing per Tg SO_2/yr by about 15% compared to equatorial injections. High-altitude injections at 15°N produce the largest reduction in global average temperature of 0.2° per Tg S/yr for the last 7 years of a 10 year experiment. Injections at higher altitude are generally more efficient at reducing surface temperature, with the exception of large equatorial injections of at least 12 Tg SO_2/yr. These findings have important implications for designing a strategy to counteract global climate change.

By injecting different amounts of SO_2 at multiple different latitudes, the spatial pattern of aerosol optical depth (AOD) can be partially controlled. This leads to the ability to influence the climate response to geoengineering with stratospheric aerosols, providing the potential for design. We use simulations from the fully coupled whole-atmosphere chemistry climate model CESM1(WACCM) to demonstrate that by appropriately combining injection at just four different locations, 30°S, 15°S, 15°N, and 30°N, then three spatial degrees of freedom of AOD can be achieved: an approximately spatially uniform AOD distribution, the relative difference in AOD between Northern and Southern Hemispheres, and the relative AOD in high versus low latitudes. For forcing levels that yield 1–2°C cooling, the AOD and surface temperature response are sufficiently linear in this model so that the response to different combinations of injection at different latitudes can be estimated from single-latitude injection simulations; nonlinearities associated with both aerosol growth and changes to stratospheric circulation will be increasingly important at higher forcing levels. Optimized injection at multiple locations is predicted to improve compensation of CO_2-forced climate change relative to a case using only equatorial aerosol injection (which overcools the tropics relative to high latitudes). The additional degrees of freedom can be used, for example, to balance the interhemispheric temperature gradient and the equator to pole temperature gradient in addition to the global mean temperature. Further research is needed to better quantify the impacts of these strategies on changes to long-term temperature, precipitation, and other climate parameters.

Radiative kernels at the top of the atmosphere are useful for decomposing changes in atmospheric radiative fluxes due to feedbacks from atmosphere and surface temperature, water vapor, and surface albedo. Here we describe and validate radiative kernels calculated with the large-ensemble version of CAM5, CESM1.1.2, at the top of the atmosphere and the surface. Estimates of the radiative forcing from greenhouse gases and aerosols in RCP8.5 in the CESM large-ensemble simulations are also diagnosed. As an application, feedbacks are calculated for the CESM large ensemble. The kernels are freely available at https://doi.org/10.5065/D6F47MT6, and accompanying software can be downloaded from https://github.com/apendergrass/cam5-kernels.

The Parallel Offline Radiative Transfer (PORT) model is a stand-alone tool, driven by model-generated datasets, that can be used for any radiation calculation that the underlying radiative transfer schemes can perform, such as diagnosing radiative forcing. In its present distribution, PORT isolates the radiation code from the Community Atmosphere Model (CAM4) in the Community Earth System Model (CESM1). The current configuration focuses on CAM4 radiation with the constituents as represented in present-day conditions in CESM1, along with their optical properties. PORT includes an implementation of stratospheric temperature adjustment under the assumption of fixed dynamical heating, which is necessary to compute radiative forcing in addition to the more straightforward instantaneous radiative forcing. PORT can be extended to use radiative constituent distributions from other models or model simulations. Ultimately, PORT can be used with various radiative transfer models. As illustrations of the use of PORT, we perform the computation of radiative forcing from doubling of carbon dioxide, from the change of tropospheric ozone concentration from the year 1850 to 2000, and from present-day aerosols. The radiative forcing from tropospheric ozone (with respect to 1850) generated by a collection of model simulations under the Atmospheric Chemistry and Climate Model Intercomparison Project is found to be 0.34 (with an intermodel standard deviation of 0.07) W m−2. Present-day aerosol direct forcing (relative to no aerosols) is found to be −1.3 W m−2.

The Community Earth System Model (CESM1) CAM4-chem has been used to perform the Chemistry Climate Model Initiative (CCMI) reference and sensitivity simulations. In this model, the Community Atmospheric Model version 4 (CAM4) is fully coupled to tropospheric and stratospheric chemistry. Details and specifics of each configuration, including new developments and improvements are described. CESM1 CAM4-chem is a low-top model that reaches up to approximately 40 km and uses a horizontal resolution of 1.9° latitude and 2.5° longitude. For the specified dynamics experiments, the model is nudged to Modern-Era Retrospective Analysis for Research and Applications (MERRA) reanalysis. We summarize the performance of the three reference simulations suggested by CCMI, with a focus on the last 15 years of the simulation when most observations are available. Comparisons with selected data sets are employed to demonstrate the general performance of the model. We highlight new data sets that are suited for multi-model evaluation studies. Most important improvements of the model are the treatment of stratospheric aerosols and the corresponding adjustments for radiation and optics, the updated chemistry scheme including improved polar chemistry and stratospheric dynamics and improved dry deposition rates. These updates lead to a very good representation of tropospheric ozone within 20 % of values from available observations for most regions. In particular, the trend and magnitude of surface ozone is much improved compared to earlier versions of the model. Furthermore, stratospheric column ozone of the Southern Hemisphere in winter and spring is reasonably well represented. All experiments still underestimate CO most significantly in Northern Hemisphere spring and show a significant underestimation of hydrocarbons based on surface observations.

A modal aerosol module (MAM) has been developed for the Community Atmosphere Model version 5 (CAM5), the atmospheric component of the Community Earth System Model version 1 (CESM1). MAM is capable of simulating the aerosol size distribution and both internal and external mixing between aerosol components, treating numerous complicated aerosol processes and aerosol physical, chemical and optical properties in a physically-based manner. Two MAM versions were developed: a more complete version with seven lognormal modes (MAM7), and a version with three lognormal modes (MAM3) for the purpose of long-term (decades to centuries) simulations. In this paper a description and evaluation of the aerosol module and its two representations are provided. Sensitivity of the aerosol lifecycle to simplifications in the representation of aerosol is discussed. Simulated sulfate and secondary organic aerosol (SOA) mass concentrations are remarkably similar between MAM3 and MAM7. Differences in primary organic matter (POM) and black carbon (BC) concentrations between MAM3 and MAM7 are also small (mostly within 10%). The mineral dust global burden differs by 10% and sea salt burden by 30–40% between MAM3 and MAM7, mainly due to the different size ranges for dust and sea salt modes and different standard deviations of the log-normal size distribution for sea salt modes between MAM3 and MAM7. The model is able to qualitatively capture the observed geographical and temporal variations of aerosol mass and number concentrations, size distributions, and aerosol optical properties. However, there are noticeable biases; e.g., simulated BC concentrations are significantly lower than measurements in the Arctic. There is a low bias in modeled aerosol optical depth on the global scale, especially in the developing countries. These biases in aerosol simulations clearly indicate the need for improvements of aerosol processes (e.g., emission fluxes of anthropogenic aerosols and precursor gases in developing countries, boundary layer nucleation) and properties (e.g., primary aerosol emission size, POM hygroscopicity). In addition, the critical role of cloud properties (e.g., liquid water content, cloud fraction) responsible for the wet scavenging of aerosol is highlighted.

Solar eruptions in early 2005 led to a substantial barrage of charged particles on the Earth's atmosphere during the 16–21 January period. Proton fluxes were greatly increased during these several days and led to the production of HOx (H, OH, HO2) and NOx (N, NO, NO2), which then caused the destruction of ozone. We focus on the Northern polar region, where satellite measurements and simulations with the Whole Atmosphere Community Climate Model (WACCM3) showed large enhancements in mesospheric HOx and NOx constituents, and associated ozone reductions, due to these solar proton events (SPEs). The WACCM3 simulations show enhanced short-lived OH and HO2 concentrations throughout the mesosphere in the 60–82.5° N latitude band due to the SPEs for most days in the 16–21 January 2005 period, somewhat higher in abundance than those observed by the Aura Microwave Limb Sounder (MLS). These HOx enhancements led to huge predicted and MLS-measured ozone decreases of greater than 40 % throughout most of the northern polar mesosphere during the SPE period. Envisat Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) measurements of hydrogen peroxide (H2O2) show increases throughout the stratosphere with highest enhancements of about 60 pptv in the lowermost mesosphere over the 16–18 January 2005 period due to the solar protons. WACCM3 predictions indicate H2O2 enhancements over the same time period of about three times that amount. Measurements of nitric acid (HNO3) by both MLS and MIPAS show an increase of about 1 ppbv above background levels in the upper stratosphere during 16–29 January 2005. WACCM3 simulations show only minuscule HNO3 increases (x are computed to be greater than 50 ppbv during the SPE period due to the small loss rates during winter. Computed NOx increases, which were statistically significant at the 95 % level, lasted about a month past the SPEs. The SCISAT-1 Atmospheric Chemistry Experiment Fourier Transform Spectrometer NOx measurements and MIPAS NO2 measurements for the polar Northern Hemisphere are in reasonable agreement with these predictions. An extremely large ground level enhancement (GLE) occurred during the SPE period on 20 January 2005. We find that protons of energies 300 to 20 000 MeV, associated with this GLE, led to very small enhanced lower stratospheric odd nitrogen concentrations of less than 0.1 % and ozone decreases of less than 0.01 %.

Solar eruptions sometimes produce protons, which impact the Earth's atmosphere. These solar proton events (SPEs) generally last a few days and produce high energy particles that precipitate into the Earth's atmosphere. The protons cause ionization and dissociation processes that ultimately lead to an enhancement of odd-hydrogen and odd-nitrogen in the polar cap regions (>60° geomagnetic latitude). We have used the Whole Atmosphere Community Climate Model (WACCM3) to study the atmospheric impact of SPEs over the period 1963–2005. The very largest SPEs were found to be the most important and caused atmospheric effects that lasted several months after the events. We present the short- and medium-term (days to a few months) atmospheric influence of the four largest SPEs in the past 45 years (August 1972; October 1989; July 2000; and October–November 2003) as computed by WACCM3 and observed by satellite instruments. Polar mesospheric NOx (NO+NO2) increased by over 50 ppbv and mesospheric ozone decreased by over 30% during these very large SPEs. Changes in HNO3, N2O5, ClONO2, HOCl, and ClO were indirectly caused by the very large SPEs in October–November 2003, were simulated by WACCM3, and previously measured by Envisat Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). WACCM3 output was also represented by sampling with the MIPAS averaging kernel for a more valid comparison. Although qualitatively similar, there are discrepancies between the model and measurement with WACCM3 predicted HNO3 and ClONO2 enhancements being smaller than measured and N2O5 enhancements being larger than measured. The HOCl enhancements were fairly similar in amounts and temporal variation in WACCM3 and MIPAS. WACCM3 simulated ClO decreases below 50 km, whereas MIPAS mainly observed increases, a very perplexing difference. Upper stratospheric and lower mesospheric NOx increased by over 10 ppbv and was transported during polar night down to the middle stratosphere in several weeks past the SPE. The WACCM3 simulations confirmed the SH HALOE observations of enhanced NOx in September 2000 as a result of the July 2000 SPE and the NH SAGE II observations of enhanced NO2 in March 1990 as a result of the October 1989 SPEs.

© 2016. American Geophysical Union. All Rights Reserved. We examine in detail a 1 year global reanalysis of carbon monoxide (CO) that is based on joint assimilation of conventional meteorological observations and Measurement of Pollution in The Troposphere (MOPITT) multispectral CO retrievals in the Community Earth System Model (CESM). Our focus is to assess the impact to the chemical system when CO distribution is constrained in a coupled full chemistry-climate model like CESM. To do this, we first evaluate the joint reanalysis (MOPITT Reanalysis) against four sets of independent observations and compare its performance against a reanalysis with no MOPITT assimilation (Control Run). We then investigate the CO burden and chemical response with the aid of tagged sectoral CO tracers.We estimate the total tropospheric CO burden in 2002 (from ensemble mean and spread) to be 371 ± 12%Tg for MOPITT Reanalysis and 291 ± 9%Tg for Control Run. Our multispecies analysis of this difference suggests that (a) direct emissions of CO and hydrocarbons are too low in the inventory used in this study and (b) chemical oxidation, transport, and deposition processes are not accurately and consistently represented in the model. Increases in CO led to net reduction of OH and subsequent longer lifetime of CH4 (Control Run: 8.7 years versus MOPITT Reanalysis: 9.3 years). Yet at the same time, this increase led to 5-10% enhancement of Northern Hemisphere O3 and overall photochemical activity via HOx recycling. Such nonlinear effects further complicate the attribution to uncertainties in direct emissions alone. This has implications to chemistry-climate modeling and inversion studies of longer-lived species.

Here we describe an updated parameterization for prescribing stratospheric aerosol in the National Center for Atmospheric Research (NCAR) Community Earth System Model (CESM1). The need for a new parameterization is motivated by the poor response of the CESM1 (formerly referred to as the Community Climate System Model, version 4, CCSM4) simulations contributed to the Coupled Model Intercomparison Project 5 (CMIP5) to colossal volcanic perturbations to the stratospheric aerosol layer (such as the 1991 Pinatubo eruption or the 1883 Krakatau eruption) in comparison to observations. In particular, the scheme used in the CMIP5 simulations by CESM1 simulated a global mean surface temperature decrease that was inconsistent with the GISS Surface Temperature Analysis (GISTEMP), NOAA's National Climatic Data Center, and the Hadley Centre of the UK Met Office (HADCRUT4). The new parameterization takes advantage of recent improvements in historical stratospheric aerosol databases to allow for variations in both the mass loading and size of the prescribed aerosol. An ensemble of simulations utilizing the old and new schemes shows CESM1's improved response to the 1991 Pinatubo eruption. Most significantly, the new scheme more accurately simulates the temperature response of the stratosphere due to local aerosol heating. Results also indicate that the new scheme decreases the global mean temperature response to the 1991 Pinatubo eruption by half of the observed temperature change, and modelled climate variability precludes statements as to the significance of this change.

Atmospheric chemistry plays a key role in determining the amounts and distributions of oxidants and gaseous precursors that control the formation of secondary gaseous and aerosol pollutants; all of those species can interact with the climate system. To understand the impacts of different gas-phase mechanisms on global air quality and climate predictions, in this work, a comprehensive comparative evaluation is performed using the Community Atmosphere Model (CAM) Version 5 with comprehensive tropospheric and stratospheric chemistry (CAM5-chem) within the Community Earth System Model (CESM) with the two most commonly used gas-phase chemical mechanisms: the 2005 Carbon Bond mechanism with Global Extension (CB05_GE) and the Model of OZone and Related chemical Tracers version 4 (MOZART-4) mechanism with additional updates (MOZART-4x). MOZART-4x and CB05_GE use different approaches to represent volatile organic compounds (VOCs) and different surrogates for secondary organic aerosol (SOA) precursors. MOZART-4x includes a more detailed representation of isoprene chemistry compared to CB05_GE. CB05_GE includes additional oxidation of SO2 by O3 over the surface of dust particles, which is not included in MOZART-4x. The results show that the two CAM5-chem simulations with CB05_GE and MOZART-4x predict similar chemical profiles for major gases (e.g., O3, CO, and NOx) compared to the aircraft measurements, with generally better agreement for NOy profiles by CB05_GE than MOZART-4x. The concentrations of SOA at four sites in the continental US (CONUS) and organic carbon (OC) over the IMPROVE sites are well predicted by MOZART-4x (with normalized mean biases (NMBs) of −1.9 and 2.1 %, respectively) but moderately underpredicted by CB05_GE (with NMBs of −23.1 and −20.7 %, respectively). This is mainly due to the higher biogenic emissions and OH levels simulated with MOZART-4x than with CB05_GE. The concentrations of OC over Europe are largely underpredicted by both MOZART-4x and CB05_GE, with NMBs of −73.0 and −75.1 %, respectively, indicating the uncertainties in the emissions of precursors and primary OC and relevant model treatments such as the oxidations of VOCs and SOA formation. Uncertainties in the emissions and convection scheme can contribute to the large bias in the model predictions (e.g., SO2, CO, black carbon, and aerosol optical depth). The two simulations also have similar cloud/radiative predictions, with a slightly better performance of domain average cloud condensation nuclei (CCN) at supersaturation of 0.5 % by CB05_GE, but slightly better agreement with observed CCN (at supersaturation of 0.2 %) profile over Beijing by MOZART-4x. The two gas-phase mechanisms result in a global average difference of 0.5 W m−2 in simulated shortwave cloud radiative forcing, with significant differences (e.g., up to 13.6 W m−2) over subtropical regions.

Two periods of extremely large solar proton events (SPEs) occurred in the past 30 years, which forced significant long-term polar stratospheric changes. The August 2-10, 1972, and October 19-27, 1989, SPEs happened in stratospheres that were quite different chemically. The stratospheric chlorine levels were relatively small in 1972 (∼1.2 ppbv) and were fairly substantial in 1989 (∼3 ppbv). Although these SPEs produced both HO x and NOy constituents in the mesosphere and stratosphere, only the NOy constituents had lifetimes long enough to affect ozone for several months to years past the events. Our recently improved two-dimensional chemistry and transport atmospheric model was used to compute the effects of these gigantic SPEs in a changing stratosphere. Significant upper stratospheric ozone depletions >10% are computed to last for a few months past these SPEs. The long-lived SPE-produced NOy constituents were transported to lower levels during winter after these huge SPEs and caused impacts in the middle and lower stratosphere. During periods of high halogen loading, these impacts resulted in interference with the chlorine and bromine loss cycles for ozone destruction. This interference actually led to a predicted total ozone increase that was especially notable in the time period 1992-1994, a few years after the October 1989 SPE. The chemical state of the atmosphere, including the stratospheric sulfate aerosol density, substantially affected the predicted stratospheric influence of these extremely large SPEs.

A two-dimensional photochemical transport model which has inputs that characterize the odd nitrogen production associated with galactic cosmic rays, solar particle events (SPEs), and lower thermospheric contributions (auroral electrons and solar EUV and soft X-rays) is used to compute odd nitrogen concentrations in the polar middle atmosphere from 1 January 1970 to 31 December 1994. We are able to separate out of the total odd nitrogen budget the contributions of the energetic charged particles according to type. The SPE contributions to annual average odd nitrogen concentrations in the polar stratosphere (latitudes > 50°) are computed to be significant (>10%) only for the larger events of August 1972 and October 1989. The SPE contributions to odd nitrogen concentrations in the polar middle atmosphere are found to be asymmetric with respect to hemispheres. The computed SPE contributions to odd nitrogen concentrations at 30 km are significant more often over the South Pole than the North Pole. The thermospheric contributions to odd nitrogen concentrations in the polar middle atmosphere are asymmetric with respect to hemispheres. A stronger thermospheric influence in the stratosphere is computed over the South Pole than the North Pole. An attempt has been made to compare the modeled odd nitrogen of the polar middle atmosphere to an ultra-high resolution polar ice cap nitrate sequence to examine the hypothesis that the nitrate sequences exhibit a signal associated with energetic particles. Variations of odd nitrogen production and modeled concentrations associated with energetic particles themselves cannot explain all of the huge variations observed in the fine structure present in nitrate data from the polar ice cap nitrates, but may be able to explain parts of some of them.

The NASA/Goddard Space Flight Center two-dimensional (GSFC 2D) photochemical transport model has been used to study the influence of thermospheric NO on the chemical balance of the middle atmosphere. Lower thermospheric NO sources are included in the GSFC 2D model in addition to the sources that are relevant to the stratosphere. A time series of hemispheric auroral electron power has been used to modulate the auroral NO production in the auroral zone. A time series of the Ottawa 10.7-cm solar flux index has been used as a proxy to modulate NO production at middle and low latitudes by solar EUV and soft X-rays. An interhemispheric asymmetry is calculated for the amounts of odd nitrogen in the polar stratosphere. We compute a 508) due to thermospheric sources, whereas we compute a 508). 7 2000 Elsevier Science Ltd. All rights reserved.

The odd nitrogen source strengths associated with solar proton events (SPEs), galactic cosmic rays (GCRs), and the oxidation of nitrous oxide in the Earth's middle atmosphere from 1974 through 1993 have been compared globally, at middle and lower latitudes ( 50 o) with a two-dimensional photochemical transport model. As discovered previously, the oxidation of nitrous oxide dominates the global odd nitrogen source, while GCRs and SPEs are significant at polar latitudes. The horizontal transport of odd nitrogen, produced by the oxidation of nitrous oxide at latitudes

We discuss and evaluate the representation of atmospheric chemistry in the global Community Atmosphere Model (CAM) version 4, the atmospheric component of the Community Earth System Model (CESM). We present a variety of configurations for the representation of tropospheric and stratospheric chemistry, wet removal, and online and offline meteorology. Results from simulations illustrating these configurations are compared with surface, aircraft and satellite observations. Overall, the model indicates a good performance when compared to observations. Major biases include a negative bias in the high-latitude CO distribution and a positive bias in upper-tropospheric/lower-stratospheric ozone, especially when online meteorology is used. The CAM-chem code as described in this paper, along with all the necessary datasets needed to perform the simulations described here, are available for download at http://www.cesm.ucar.edu.

[1] We have analyzed a set of simulations aimed at understanding the mechanisms that drive observed trends in the lower stratosphere after 1970. The simulations were performed using a version of the Community Atmosphere Model version 3 (CAM3) updated with interactive tropospheric and stratospheric chemistry. Even with a relatively low model top (≈40 km), this model shows good ability at reproducing a variety of large-scale changes in climate and chemical composition in the stratosphere when forced with the observed sea-surface temperatures and surface concentrations of long-lived trace gases and ozone-depleting substances. We then used the same model framework to differentiate the role of chemically active composition (ozone, methane, and chlorofluorocarbons) and CO2 changes on observed trends in the stratosphere. Among the sensitivity factors analyzed, our simulations indicate that changes in CO2 over the simulated period do not lead to significantly different total ozone trend; however, changes in CO2 lead to important differences in ozone in the upper part of the model. On the other hand, changes in surface methane concentration are shown to play a significant role in driving changes in the globally averaged total ozone column, through a combination of changes in tropospheric and stratospheric ozone columns. We also show that the correlation between a change in tropical mean age of air and in vertical velocity breaks down above 20 hPa, in association with increased isentropic mixing above that level. Finally, we show that our model is capable of reproducing trends in the tropical age of air that were found in other studies; our simulations also indicate a significant impact of keeping methane and ozone-depleting substances at their 1970 levels, indicating the potentially important role of controlling methane emissions.