Indirect long-term global radiative cooling from NOx emissions

Anthropogenic emissions of short‐lived, chemically reactive gases, such as NO x and CO, are known to influence climate by altering the chemistry of the global troposphere and thereby the abundance of the greenhouse gases O3, CH4 and the HFCs. This study uses the characteristics of the natural modes of the tropospheric chemical system to decompose the greenhouse effect of NO x and CO emissions into (i) short‐lived modes involving predominantly tropospheric O3 and (ii) the long‐lived mode involving a global coupled CH4‐CO‐O3 perturbation. Combining these two classes of greenhouse perturbations—large, short‐lived, regional O3 increases and smaller, long‐lived, global decreases in CH4 and O3—we find that most types of anthropogenic NO x emissions lead to a negative radiative forcing and an overall cooling of the earth

Two-Dimensional Intercomparison of Stratospheric Models

A detailed record is provided for the examination of fundamental differences in photochemistry and transport among atmospheric models. The results of 16 different modeling groups are presented for several model experiments

Effects of Chemical Feedbacks on Decadal Methane Emissions Estimates

The coupled chemistry of methane, carbon monoxide (CO), and hydroxyl radical (OH) can modulate methane's 9‐year lifetime. This is often ignored in methane flux inversions, and the impacts of neglecting interactive chemistry have not been quantified. Using a coupled‐chemistry box model, we show that neglecting the effect of methane source perturbation on [OH] can lead to a 25% bias in estimating abrupt changes in methane sources after only 10 years. Further, large CO emissions, such as from biomass burning, can increase methane concentrations by extending the methane lifetime through impacts on [OH]. Finally, we quantify the biases of including (or excluding) coupled chemistry in the context of recent methane and CO trends. Decreasing CO concentrations, beginning in the 2000's, have notable impacts on methane flux inversions. Given these nonnegligible errors, decadal methane emissions inversions should incorporate chemical feedbacks for more robust methane trend analyses and source attributions

Sea Spray Aerosol: Where Marine Biology Meets Atmospheric Chemistry.

Atmospheric aerosols have long been known to alter climate by scattering incoming solar radiation and acting as seeds for cloud formation. These processes have vast implications for controlling the chemistry of our environment and the Earth's climate. Sea spray aerosol (SSA) is emitted over nearly three-quarters of our planet, yet precisely how SSA impacts Earth's radiation budget remains highly uncertain. Over the past several decades, studies have shown that SSA particles are far more complex than just sea salt. Ocean biological and physical processes produce individual SSA particles containing a diverse array of biological species including proteins, enzymes, bacteria, and viruses and a diverse array of organic compounds including fatty acids and sugars. Thus, a new frontier of research is emerging at the nexus of chemistry, biology, and atmospheric science. In this Outlook article, we discuss how current and future aerosol chemistry research demands a tight coupling between experimental (observational and laboratory studies) and computational (simulation-based) methods. This integration of approaches will enable the systematic interrogation of the complexity within individual SSA particles at a level that will enable prediction of the physicochemical properties of real-world SSA, ultimately illuminating the detailed mechanisms of how the constituents within individual SSA impact climate

Importance of composition and hygroscopicity of BC particles to the effect of BC mitigation on cloud properties: Application to California conditions

Black carbon (BC) has many effects on climate including the direct effect on atmospheric absorption, indirect and semi-direct effects on clouds, snow effects, and others. While most of these are positive (warming), the first indirect effect is negative and quantifying its magnitude in addition to other BC feedbacks is important for supporting policies that mitigate BC. We use the detailed aerosol chemistry parcel model of Russell and Seinfeld (1998), observationally constrained by initial measured aerosol concentrations from five California sites, to provide simulated cloud drop number (CDN) concentrations against which two GCM calculations – one run at the global scale and one nested from the global-to-regional scale are compared. The GCM results reflect the combined effects of their emission inventories, advection schemes, and cloud parameterizations. BC-type particles contributed between 16 and 20% of cloud droplets at all sites even in the presence of more hygroscopic particles. While this chemically detailed parcel model result is based on simplified cloud dynamics and does not consider semi-direct or cloud absorption effects, the cloud drop number concentrations are similar to the simulations of both Chen et al. (2010b) and Jacobson (2010) for the average cloud conditions in California. Reducing BC particle concentration by 50% decreased the cloud droplet concentration by between 6% and 9% resulting in the formation of fewer, larger cloud droplets that correspond to a lower cloud albedo. This trend is similar to Chen et al. (2010b) and Jacobson (2010) when BC particles were modeled as hygroscopic. This reduction in CDN in California due to the decrease in activated BC particles supports the concern raised by Chen et al. (2010a) that the cloud albedo effect of BC particles has a cooling effect that partially offsets the direct forcing reduction if other warming effects of BC on clouds are unchanged. These results suggests that for regions like the California sites studied here, where BC mitigation targets fossil fuel sources, a critical aspect of the modeled reduction is the chemical composition and associated hygroscopicity of the BC particles removed as well as their relative contribution to the atmospheric particle concentrations

PREDICTING COMMON CRUPINA HABITAT WITH GEOGRAPHIC AND REMOTE SENSING DATA

Field surveys for common crupina, as part of an eradication program, are time intensive and could be made more efficient if common crupina habitat could be predicted. Slope, aspect, and vegetation data were used as generalized plant community variables to predict common crupina habitat using a transformed logistic regression. Models were constructed using either aspect or slope as an explanatory variable such that one model predicted the overall effect of either slope or aspect and a set of models predicted the effect of slope or aspect at each of three vegetation classes. A second data set was used to validate the prediction equations for slope and aspect. The proposed models fit the data well and validations were successful as indicated by analysis of residual plots. The probability of finding common crupina was highest for southeast to southwest aspects. In addition, common crupina was most likely to occur, overall, at 25 to 30% slope with decreasing probability at gentler and steeper slopes. Slope models fitted at each vegetation class indicated maximums at 25 to 30% slope for forest and mesic grassland areas but the maximum for arid grasslands was 50% slope. A field detection survey of common crupina that was directed according to probability of occurrence differences along aspect and slope gradients could reduce the area surveyed to 34 to 42%, respectively, of the study area (using a probability cutoff of 30% of the model\u27s maximum). Detection surveys directed according to slope models would find 14% more common crupina than aspect models but would survey 8 to 11 % more area. Models that considered vegetation class, when contrasted with models that did not consider vegetation class, did not decrease the total area surveyed while maintaining the same percentage of common crupina found

Chemical transport model ozone simulations for spring 2001 over the western Pacific:comparisons with TRACE-P lidar, ozonesondes, and Total Ozone Mapping Spectrometer columns

Two closely related chemical transport models (CTMs) employing the same high-resolution meteorological data (similar to180 km x similar to180 km x similar to600 m) from the European Centre for Medium-Range Weather Forecasts are used to simulate the ozone total column and tropospheric distribution over the western Pacific region that was explored by the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) measurement campaign in February-April 2001. We make extensive comparisons with ozone measurements from the lidar instrument on the NASA DC-8, with ozonesondes taken during the period around the Pacific Rim, and with TOMS total column ozone. These demonstrate that within the uncertainties of the meteorological data and the constraints of model resolution, the two CTMs (FRSGC/UCI and Oslo CTM2) can simulate the observed tropospheric ozone and do particularly well when realistic stratospheric ozone photochemistry is included. The greatest differences between the models and observations occur in the polluted boundary layer, where problems related to the simplified chemical mechanism and inadequate horizontal resolution are likely to have caused the net overestimation of about 10 ppb mole fraction. In the upper troposphere, the large variability driven by stratospheric intrusions makes agreement very sensitive to the timing of meteorological features

Predicted rocket and shuttle effects on stratospheric ozone

The major chemical effluents of either solid- or liquid-fueled rockets that can potentially perturb stratospheric ozone include chlorine compounds (HCl), nitrogen compounds (NO(x)), and hydrogen compounds (H2 and H2O). Radicals (Cl, ClO, H, OH, HO2, NO, and NO2) formed directly or indirectly from rocket exhaust can cause the catalytic destruction of ozone. Other exhaust compounds that could presumably lead to ozone destruction either by direct reaction with ozone or by providing a surface for heterogeneous processes include the particulates Al2O3, ice, and soot. These topics are discussed in terms of the possible effects of rocket exhausts on stratospheric ozone

Relationships of Biomass-Burning Aerosols to Ice in Orographic Wave Clouds

Ice concentrations in orographic wave clouds at temperatures between −24° and −29°C were shown to be related to aerosol characteristics in nearby clear air during five research flights over the Rocky Mountains. When clouds with influence from colder temperatures were excluded from the dataset, mean ice nuclei and cloud ice number concentrations were very low, on the order of 1–5 L^(−1). In this environment, ice number concentrations were found to be significantly correlated with the number concentration of larger particles, those larger than both 0.1- and 0.5-μm diameter. A variety of complementary techniques was used to measure aerosol size distributions and chemical composition. Strong correlations were also observed between ice concentrations and the number concentrations of soot and biomass-burning aerosols. Ice nuclei concentrations directly measured in biomass-burning plumes were the highest detected during the project. Taken together, this evidence indicates a potential role for biomass-burning aerosols in ice formation, particularly in regions with relatively low concentrations of other ice nucleating aerosols

Studies of aerosol at a coastal site using two aerosol mass spectrometry instruments and identification of biogenic particle types

International audienceDuring August 2004 an Aerosol Time-of-Flight Mass Spectrometer (TSI ATOFMS Model 3800-100) and an Aerodyne Aerosol Mass Spectrometer (AMS) were deployed at Mace Head during the NAMBLEX campaign. Single particle data (size, positive and negative mass spectra) from the ATOFMS were imported into ART 2a, a neural network algorithm, which assigns individual particles to clusters on the basis of their mass spectral similarities. Results are very consistent with previous time consuming manual classifications (Dall'Osto et al., 2004). Three broad classes were found: sea-salt, dust and carbon-containing particles, with a number of sub-classes within each. The Aerodyne (AMS) instrument was also used during NAMBLEX, providing online, real time measurements of the mass of non-refractory components of aerosol particles as function of their size. The ATOFMS detected a type of particle not identified in our earlier analysis, with a strong signal at m/z 24, likely due to magnesium. This type of particle was detected during the same periods as pure unreacted sea salt particles and is thought to be biogenic, originating from the sea surface. AMS data are consistent with this interpretation, showing an additional organic peak in the corresponding size range at times when the Mg-rich particles are detected. The work shows the ATOFMS and AMS to be largely complementary, and to provide a powerful instrumental combination in studies of atmospheric chemistry