Improving our fundamental understanding of the role of aerosol-cloud interactions in the climate system.

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

Hydrocarbon emissions from in-use commercial aircraft during airport operations.

The emissions of selected hydrocarbons from in-use commercial aircraft at a major airport in the United States were characterized using proton-transfer reaction mass spectrometry (PTR-MS) and tunable infrared differential absorption spectroscopy (TILDAS) to probe the composition of diluted exhaust plumes downwind. The emission indices for formaldehyde, acetaldehyde, benzene, and toluene, as well as other hydrocarbon species, were determined through analysis of 45 intercepted plumes identified as being associated with specific aircraft. As would have been predicted for high bypass turbine engines, the hydrocarbon emission index was greater in idle and taxiway acceleration plumes relative to approach and takeoff plumes. The opposite was seen in total NOy emission index, which increased from idle to takeoff. Within the idle plumes sampled in this study, the median emission index for formaldehyde was 1.1 g of HCHO per kg of fuel. For the subset of hydrocarbons measured in this work, the idle emissions levels relative to formaldehyde agree well with those of previous studies. The projected total unburned hydrocarbons (UHC) deduced from the range of in-use idle plumes analyzed in this work is greater than a plausible range of engine types using the defined idle condition (7% of rated engine thrust) in the International Civil Aviation Organization (ICAO) databank reference.

Kinetic studies of the reactions of O2(b 1sigma(g)+) with several atmospheric molecules.

Thermal rate coefficients for the removal (reaction + quenching) of O2(1sigma(g)+) by collision with several atmospheric molecules were determined to be as follows: O3, k3(210-370 K) = (3.63 +/- 0.86) x 10(-11) exp((-115 +/- 66)/T); H2O, k4(250-370 K) = (4.52 +/- 2.14) x 10(-12) exp((89 +/- 210)/T); N2, k5(210-370 K) = (2.03 +/- 0.30) x 10(-15) exp((37 +/- 40)/T); CO2, k6(298 K) = (3.39 +/- 0.36) x 10(-13); CH4, k7(298 K) = (1.08 +/- 0.11) x 10(-13); CO, k8(298 K) = (3.74 +/- 0.87) x 10(-15); all units in cm3 molecule(-1) s(-1). O2(1sigma(g)+) was produced by directly exciting ground-state O2(3sigma(g)-) with a 762 nm pulsed dye laser. The reaction of O2(1sigma(g)+) with O3 was used to produce O(3P), and temporal profiles of O(3P) were measured using VUV atomic resonance fluorescence in the presence of the reactant to determine the rate coefficients for removal of O2(1sigma(g)+). Our results are compared with previous values, where available, and the overall trend in the O2(1sigma(g)+) removal rate coefficients and the atmospheric implications of these rate coefficients are discussed. Additionally, an upper limit for the branching ratio of O2(1sigma(g)+) + CO to give O(3P) + CO2 was determined to be < or = 0.2% and this reaction channel is shown to be of negligible importance in the atmosphere.