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Vitt, Francis

Publications and source records attributed to Vitt, Francis.

Development and Evaluation of Chemistry‐Aerosol‐Climate Model CAM5‐Chem‐MAM7‐MOSAIC: Global Atmospheric Distribution and Radiative Effects of Nitrate Aerosol

Abstract 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 .

54 ENVIRONMENTAL SCIENCES↗

Climate Forcing and Trends of Organic Aerosols in the Community Earth System Model (CESM2)

The Community Earth System Model version 2 (CESM2) includes three main atmospheric configurations: the Community Atmosphere Model version 6 (CAM6) with simplified chemistry and a simplified organic aerosol (OA) scheme, CAM6 with comprehensive tropospheric and stratospheric chemistry representation (CAM6-chem), and the Whole Atmosphere Community Climate Model version 6 (WACCM6). Both, CAM6-chem and WACCM6 include a more comprehensive secondary organic aerosols (SOA) approach using the volatility basis set (vbs) scheme and prognostic stratospheric aerosols. This paper describes the different OA schemes available in the different atmospheric configurations of CESM2 and discusses differences in aerosol burden and resulting climate forcings. Derived OA burden and trends differ due to differences in OA formation using the different approaches. Regional differences in Aerosol Optical Depth with larger values using the comprehensive approach occur over SOA source regions. Stronger increasing SOA trends between 1960 and 2015 in WACCM6 compared to CAM6 are due to increasing biogenic emissions aligned with increasing surface temperatures. Using the comprehensive SOA approach further leads to improved comparisons to aircraft observations and SOA formation of ˜143 Tg/yr. We further use WACCM6 to identify source contributions of OA from biogenic, fossil fuel, and biomass burning emissions, to quantify SOA amounts and trends from these sources. Increasing SOA trends between 1960 and 2015 are the result of increasing biogenic emissions aligned with increasing surface temperatures. Biogenic emissions are at least two thirds of the total SOA burden. In addition, SOA source contributions from fossil fuel emissions become more important, with largest values over Southeast Asia. The estimated total anthropogenic forcing of OA in WACCM6 for 1995–2010 conditions is -0.43 W/m2, mostly from the aerosol direct effect.

Tilmes, S↗

Comparing surface and stratospheric impacts of geoengineering with different SO2 injection strategies

Geoengineering with stratospheric sulfate aerosols can, to some extent, be designed to achieve different climate objectives. Here we use the the state-of-the-art Community Earth System Model, version 1, with the Whole Atmosphere Community Climate Model as its atmospheric component (CESM1(WACCM)), to compare surface climate and stratospheric effects of two geoengineering strategies. In one, SO2 is injected into the tropical lower stratosphere at the equator to keep global mean temperature nearly constant under an RCP8.5 scenario, as has been commonly simulated in previous studies. In another, the Geoengineering Large Ensemble (GLENS), SO2 is injected into the lower stratosphere at four different locations (30°N/S and 15°N/S) to keep global mean temperature, the interhemispheric temperature gradient, and the equator-to-pole temperature gradient nearly unchanged. Both simulations are effective at offsetting changes in global mean temperature and the interhemispheric temperature gradient that result from increased greenhouse gases, but only GLENS offsets changes in the equator-to-pole temperature gradient. GLENS results in a more even aerosol distribution, whereas equatorial injection tends to result in an aerosol peak in the tropics. Many other aspects of surface climate changes, including precipitation and sea ice coverage, also show reduced changes in GLENS as compared to equatorial injection. Stratospheric changes, including heating, circulation, and effects on the quasi-biennial oscillation are greatly reduced in GLENS as compared to equatorial injection.

Kravitz, Benjamin S.↗

Effects of Different Stratospheric SO2 Injection Altitudes on Stratospheric Chemistry and Dynamics

Strategic geoengineering has been 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 state-of-the-art climate model. Two different sce-narios are explored that produce approximately the same global cooling of 2?C over the period 2042 – 49, a high altitude injection case using 24 Tg SO2 yr-1 at 30 hPa (˜ 25km altitude), and a low altitude injection case using 32 Tg SO2 yr-1 injections at 70 hPa (˜ 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 increase of water vapor of 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 mid- and high northern latitudes, low altitude injections result in column ozone greater than without geoengineering. These changes are mostly driven by dynamics and advection. Antarctic column ozone in 2040-49 does not recover from present day values for both cases.

Tilmes, S↗

The Climate Response to Stratospheric Aerosol Geoengineering Can Be Tailored Using Multiple Injection Locations

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. In this work, 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.

54 ENVIRONMENTAL SCIENCES↗

First Simulations of Designing Stratospheric Sulfate Aerosol Geoengineering to Meet Multiple Simultaneous Climate Objectives

In this work, 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 SO2 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 SO2 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 geeongineering 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.

54 ENVIRONMENTAL SCIENCES↗

Radiative and Chemical Response to Interactive Stratospheric Sulfate Aerosols in Fully Coupled CESM1(WACCM)

We present a new version of the Community Earth System Model, version 1 (CESM1) with the Whole Atmosphere Community Climate Model (WACCM) featuring numerous improvements that are unique among earth system models. Improved horizontal resolution, dynamics, and chemistry now provide the development of an internally generated quasi-biennial oscillation, and significant improvements to temperatures and ozone throughout the stratosphere. The prognostic treatment of stratospheric sulfate aerosols is shown to represent well the evolution of stratospheric aerosol optical depth and perturbations to solar and longwave radiation following volcanic eruptions. We identify the inclusion of interactive OH chemistry as crucial to the study of aerosol formation following large inputs of SO 2 to the stratosphere. We show that depletion of OH levels within the dense SO 2 cloud in the first weeks following the June 1991 eruption of Mt. Pinatubo significantly prolonged the 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 initial losses of SO 2 on ash and ice in the first 7-9 days following the eruption, and have not correctly accounted for OH depletion. The completeness of the chemistry, dynamics, and aerosol microphysics in WACCM uniquely qualify it for studies of stratospheric sulfate aerosol geoengineering.

54 ENVIRONMENTAL SCIENCES↗

Improvement of the prediction of surface ozone concentration over conterminous U.S. by a computationally efficient second-order Rosenbrock solver in CAM4-Chem

The global chemistry-climate model (CAM4-Chem) overestimates the surface ozone concentration over the conterminous U.S. (CONUS). Reasons for this positive bias include emission, meteorology, chemical mechanism, and solver. In this study, we explore the last possibility by examining the sensitivity to the numerical methods for solving the chemistry equations. A second-order Rosenbrock (ROS-2) solver is implemented in CAM4-Chem to examine its influence on the surface ozone concentration and the computational performance of the chemistry program. Results show that under the same time step size (1800 s), statistically significant reduction of positive bias is achieved by the ROS-2 solver. The improvement is as large as 5.2 ppb in Eastern U.S. during summer season. The ROS-2 solver is shown to reduce the positive bias in Europe and Asia as well, indicating the lower surface ozone concentration over the CONUS predicted by the ROS-2 solver is not a trade-off consequence with increasing the ozone concentration at other global regions. In addition, by refining the time step size to 180 s, the first-order implicit solver does not provide statistically significant improvement of surface ozone concentration. It reveals that the better prediction from the ROS-2 solver is not only due to its accuracy but also due to its suitability for stiff chemistry equations. As an added benefit, the computation cost of the ROS-2 solver is almost half of first-order implicit solver. The improved computational efficiency of the ROS-2 solver is due to the reuse of the Jacobian matrix and lower upper (LU) factorization during its multistage calculation.

54 ENVIRONMENTAL SCIENCES↗

A consistent prescription of stratospheric aerosol for both radiation and chemistry in the Community Earth System Model (CESM1)

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. Here, 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.

58 GEOSCIENCES↗

Representation of the Community Earth System Model (CESM1) CAM4-chem within the Chemistry-Climate Model Initiative (CCMI)

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. In conclusion, all experiments still underestimate CO most significantly in Northern Hemisphere spring and show a significant underestimation of hydrocarbons based on surface observations.

54 ENVIRONMENTAL SCIENCES↗

Chemistry in CESM-SE: Evaluation, Performance and Optimization

The purpose of the proposed work focused on development of chemistry representation within the Spectral Element (SE) dynamical core as implemented in the Community Earth System Model (CESM). More specifically, a main focus was on the ability of SE to accurately represent tracer transport. The proposed approach was to incrementally increase the complexity of the problem, starting from specified two-dimensional flow and tracers to simulations using specified dynamics and full chemistry. As demonstrated below, we have successfully studied all aspects of the proposed work, although only part of the work has been published in the refereed literature so far. Furthermore, because the SE dynamical core has been found to have several deficiencies that are still being investigated for solution, not all proposed tasks were finalized. In addition to the tests for SE performance, in an effort to decrease the computational burden of interactive chemistry, especially in the case of a large number of chemical species and chemical reactions, development on a faster chemical solver and implementation on GPUs has been implemented in CESM under the leadership of John Drake (U. Tennessee).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗