Atmospheric chemistry-climate feedbacks

We extend the theory of climate feedbacks to include atmospheric chemistry. A change in temperature caused by a radiative forcing will include, in general, a contribution from the chemical change that is fed back into the climate system; likewise, the change in atmospheric burdens caused by a chemical forcing will include a contribution from the associated climate change that is fed back into the chemical system. The theory includes two feedback gains, G_(che) and G_(cli). G_(che) is defined as the ratio of the change in equilibrium global mean temperature owing to long-lived greenhouse gas radiative forcing, under full climate-chemistry coupling, to that in the absence of coupling. G_(cli) is defined as the ratio of the change in equilibrium mean aerosol or gas-phase burdens owing to chemical forcing under full coupling, to that in the absence of coupling. We employ a climate-atmospheric chemistry model based on the Goddard Institute for Space Studies (GISS) GCM II', including tropospheric gas-phase chemistry, sulfate, nitrate, ammonium, black carbon, and organic carbon. While the model describes many essential couplings between climate and atmospheric chemistry, not all couplings are accounted for, such as indirect aerosol forcing and the role of natural dust and sea salt aerosols. Guided by the feedback theory, we perform perturbation experiments to quantify G_(che) and G_(cli). We find that G_(che) for surface air temperature is essentially equal to 1.00 on a planetary scale. Regionally, G_(che) is estimated to be 0.80–1.30. The gains are small compared to those of the physical feedbacks in the climate system (e.g., water vapor, and cloud feedbacks). These values for G_(che) are robust for the specific model used, but may change when using more comprehensive climate-atmospheric chemistry models. Our perturbation experiments do not allow one to obtain robust values for G_(cli). Globally averaged, the values range from 0.99 to 1.28, depending on the chemical species, while, in areas of high pollution, G_(cli) can be up to 1.15 for ozone, and as large as 1.40 for total aerosol. These preliminary values indicate a significant role of climate feedbacks in the atmospheric chemistry system

Lookup tables to compute high energy cosmic ray induced atmospheric ionization and changes in atmospheric chemistry

A variety of events such as gamma-ray bursts and supernovae may expose the Earth to an increased flux of high-energy cosmic rays, with potentially important effects on the biosphere. Existing atmospheric chemistry software does not have the capability of incorporating the effects of substantial cosmic ray flux above 10 GeV . An atmospheric code, the NASA-Goddard Space Flight Center two-dimensional (latitude, altitude) time-dependent atmospheric model (NGSFC), is used to study atmospheric chemistry changes. Using CORSIKA, we have created tables that can be used to compute high energy cosmic ray (10 GeV - 1 PeV) induced atmospheric ionization and also, with the use of the NGSFC code, can be used to simulate the resulting atmospheric chemistry changes. We discuss the tables, their uses, weaknesses, and strengths.Comment: In press: Journal of Cosmology and Astroparticle Physics. 6 figures, 3 tables, two associated data files. Major revisions, including results of a greatly expanded computation, clarification and updated references. In the future we will expand the table to at least EeV levels

OH and HO2 chemistry in the North Atlantic free troposphere

Interactions between atmospheric hydrogen oxides and aircraft nitrogen oxides determine the impact of aircraft exhaust on atmospheric chemistry. To study these interactions, the Subsonic Assessment: Ozone and Nitrogen Oxide Experiment (SONEX) assembled the most complete measurement complement to date for studying HO(x) (OH and HO2) chemistry in the free troposphere. Observed and modeled HO(x) agree on average to within experimental uncertainties (±40%). However, significant discrepancies occur as a function of NO and at solar zenith angles >70°. Some discrepancies appear to be removed by model adjustments to HO(x)-NO(x) chemistry, particularly by reducing HO2NO2 (PNA) and by including heterogeneous reactions on aerosols and cirrus clouds

Atmospheric Chemistry Modelling of Amine Emissions from Post Combustion CO2 Capture Technology

Emissions from post combustion CO2 capture plants using amine solvents are of concern due to their adverse impacts on the human health and environment. Potent carcinogens such as nitrosamines and nitramines resulting from the degradation of the amine emissions in the atmosphere have not been fully investigated. It is, therefore, imperative to determine the atmospheric fate of these amine emissions, such as their chemical transformation, deposition and transport pathways away from the emitting facility so as to perform essential risk assessments. More importantly, there is a lack of integration of amine atmospheric chemistry with dispersion studies. In this work, the atmospheric chemistry of the reference solvent for CO2 capture, monoethanolamine, and the most common degradation amines, methylamine and dimethylamine, formed as part of the post combustion capture process are considered along with dispersion calculations. Rate constants describing the atmospheric chemistry reactions of the amines of interest are obtained using theoretical quantum chemistry methods and kinetic modeling. The dispersion of these amines in the atmosphere is modeled using an air-dispersion model, ADMS 5. A worst case study on the UK's largest CO2 capture pilot plant, Ferrybridge, is carried out to estimate the maximum tolerable emissions of these amines into the atmosphere so that the calculated concentrations do not exceed guideline values and that the risk is acceptable

Atmospheric Chemistry of Venus-like Exoplanets

We use thermodynamic calculations to model atmospheric chemistry on terrestrial exoplanets that are hot enough for chemical equilibira between the atmosphere and lithosphere, as on Venus. The results of our calculations place constraints on abundances of spectroscopically observable gases, the surface temperature and pressure, and the mineralogy of the surface. These results will be useful in planning future observations of the atmospheres of terrestrial-sized exoplanets by current and proposed space observatories such as the Hubble Space Telescope (HST), Spitzer, James Webb Space Telescope (JWST), Terrestrial Planet Finder, and Darwin.Comment: 35 pages, 4 figures, 3 tables; 1 appendix; submitted to ApJ; version

Martian atmospheric O₃ retrieval development for the NOMAD-UVIS spectrometer

The composition of atmospheric trace gases and aerosols is a highly variable and poorly constrained component of the martian atmosphere, and by affecting martian climate and UV surface dose, represents a key parameter in the assessment of suitability for martian habitability. The ExoMars Trace Gas Orbiter (TGO) carries the Open University (OU) designed Ultraviolet and VIsible Spectrometer (UVIS) instrument as part of the Belgian-led Nadir and Occultation for MArs Discovery (NOMAD) spectrometer suite. NOMAD will begin transmitting science observations of martian surface and atmosphere back-scattered UltraViolet (UV) and visible radiation in Spring 2018, which will be processed to derive spatially and temporally averaged atmospheric trace gas and aerosol concentrations, intended to provide a better understanding of martian atmospheric photo-chemistry and dynamics, and will also improve models of martian atmospheric chemistry, climate and habitability. Work presented here illustrates initial development and testing of the OU’s new retrieval algorithm for determining O3 and aerosol concentrations from the UVIS instrument

Modeling chemistry in and above snow at Summit, Greenland – Part 1: Model description and results

Sun-lit snow is increasingly recognized as a chemical reactor that plays an active role in uptake, transformation, and release of atmospheric trace gases. Snow is known to influence boundary layer air on a local scale, and given the large global surface coverage of snow may also be significant on regional and global scales. We present a new detailed one-dimensional snow chemistry module that has been coupled to the 1-D atmospheric boundary layer model MISTRA. The new 1-D snow module, which is dynamically coupled to the overlaying atmospheric model, includes heat transport in the snowpack, molecular diffusion, and wind pumping of gases in the interstitial air. The model includes gas phase chemical reactions both in the interstitial air and the atmosphere. Heterogeneous and multiphase chemistry on atmospheric aerosol is considered explicitly. The chemical interaction of interstitial air with snow grains is simulated assuming chemistry in a liquid-like layer (LLL) on the grain surface. The coupled model, referred to as MISTRA-SNOW, was used to investigate snow as the source of nitrogen oxides (NOx) and gas phase reactive bromine in the atmospheric boundary layer in the remote snow covered Arctic (over the Greenland ice sheet) as well as to investigate the link between halogen cycling and ozone depletion that has been observed in interstitial air. The model is validated using data taken 10 June–13 June, 2008 as part of the Greenland Summit Halogen-HOx experiment (GSHOX). The model predicts that reactions involving bromide and nitrate impurities in the surface snow can sustain atmospheric NO and BrO mixing ratios measured at Summit, Greenland during this period

Earth Observing System. Volume 1, Part 2: Science and Mission Requirements. Working Group Report Appendix

Areas of global hydrologic cycles, global biogeochemical cycles geophysical processes are addressed including biological oceanography, inland aquatic resources, land biology, tropospheric chemistry, oceanic transport, polar glaciology, sea ice and atmospheric chemistry

Planning, implementation and scientific goals of the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field mission

The Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field mission based at Ellington Field, Texas, during August and September 2013 employed the most comprehensive airborne payload to date to investigate atmospheric composition over North America. The NASA ER-2, DC-8, and SPEC Inc. Learjet flew 57 science flights from the surface to 20 km. The ER-2 employed seven remote sensing instruments as a satellite surrogate and eight in situ instruments. The DC-8 employed 23 in situ and five remote sensing instruments for radiation, chemistry, and microphysics. The Learjet used 11 instruments to explore cloud microphysics. SEAC4RS launched numerous balloons, augmented AErosol RObotic NETwork, and collaborated with many existing ground measurement sites. Flights investigating convection included close coordination of all three aircraft. Coordinated DC-8 and ER-2 flights investigated the optical properties of aerosols, the influence of aerosols on clouds, and the performance of new instruments for satellite measurements of clouds and aerosols. ER-2 sorties sampled stratospheric injections of water vapor and other chemicals by local and distant convection. DC-8 flights studied seasonally evolving chemistry in the Southeastern U.S., atmospheric chemistry with lower emissions of NOx and SO2 than in previous decades, isoprene chemistry under high and low NOx conditions at different locations, organic aerosols, air pollution near Houston and in petroleum fields, smoke from wildfires in western forests and from agricultural fires in the Mississippi Valley, and the ways in which the chemistry in the boundary layer and the upper troposphere were influenced by vertical transport in convective clouds