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Saharan dust infrared optical depth and altitude retrieved from AIRS: a focus over North Atlantic – comparison to MODIS and CALIPSO

Monthly mean infrared (10 μm) dust layer aerosol optical depth (AOD) and mean altitude are simultaneously retrieved over the tropics (30° S–30° N) from almost seven years of Atmospheric Infrared Sounder (AIRS) observations covering the period January 2003 to September 2009. The method developed relies on the construction of look-up-tables computed for a large selection of atmospheric situations and follows two main steps: first, determination of the observed atmospheric thermodynamic situation and, second, determination of the dust properties. A very good agreement is found between AIRS-retrieved AODs and visible optical depths from the Moderate resolution Imaging Spectroradiometer (MODIS/Aqua) during the main (summer) dust season, in particular for three regions of the tropical North Atlantic and one region of the north-western Indian Ocean. Outside this season, differences are mostly due to the sensitivity of MODIS to aerosol species other than dust and to the more specific sensitivity of AIRS to the dust coarse mode. AIRS-retrieved dust layer mean altitudes are compared to the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP/CALIPSO) aerosol mean layer altitude for the period June 2006 to June 2009. Results for a region of the north tropical Atlantic downwind of the Sahara show a good agreement between the two products (σ≈360 m). Differences observed in the peak-to-trough seasonal amplitude, smaller from AIRS, are principally attributed to the large difference in spatial sampling of the two instruments. They also come from the intrinsic limit in sensitivity of the passive infrared sounders for low altitudes. These results demonstrate the capability of high resolution infrared sounders to measure not only dust aerosol AOD but also the mean dust layer altitude.
Numerical simulations of contrail-to-cirrus transition – Part 2: Impact of initial ice crystal number, radiation, stratification, secondary nucleation and layer depth

Simulations of contrail-to-cirrus transition were performed with an LES model. In Part 1 the impact of relative humidity, temperature and vertical wind shear was explored in a detailed parametric study. Here, we study atmospheric parameters like stratification and depth of the supersaturated layer and processes which may affect the contrail evolution. We consider contrails in various radiation scenarios herein defined by the season, time of day and the presence of lower-level cloudiness which controls the radiance incident on the contrail layer. Under suitable conditions, controlled by the radiation scenario and stratification, radiative heating lifts the contrail-cirrus and prolongs its lifetime. The potential of contrail-driven secondary nucleation is investigated. We consider homogeneous nucleation and heterogeneous nucleation of preactivated soot cores released from sublimated contrail ice crystals. In our model the contrail dynamics triggered by radiative heating does not suffice to force homogeneous freezing of ambient liquid aerosol particles. Furthermore, our model results suggest that heterogeneous nucleation of preactivated soot cores is unimportant. Contrail evolution is not controlled by the depth of the supersaturated layer as long as it exceeds roughly 500 m. Deep fallstreaks however need thicker layers. A variation of the initial ice crystal number is effective during the whole evolution of a contrail. A cut of the soot particle emission by two orders of magnitude can reduce the contrail timescale by one hour and the optical thickness by a factor of 5. Hence future engines with lower soot particle emissions could potentially lead to a reduction of the climate impact of aviation.
Numerical simulations of contrail-to-cirrus transition – Part 1: An extensive parametric study

Simulations of contrail-to-cirrus transition over up to 6 h were performed using a LES-model. The sensitivity of microphysical, optical and geometric contrail properties to relative humidity RHi, temperature T and vertical wind shear s was investigated in an extensive parametric study. The dominant parameter for contrail evolution is relative humidity. Substantial spreading is only visible for RHi≳120%. Vertical wind shear has a smaller effect on optical properties than human observers might expect from the visual impression. Our model shows that after a few hours the water vapour removed by falling ice crystals from the contrail layer can be several times higher than the ice mass that is actually present in the contrail at any instance.
Uncertainties in atmospheric chemistry modelling due to convection parameterisations and subsequent scavenging

Moist convection in global modelling contributes significantly to the transport of energy, momentum, water and trace gases and aerosols within the troposphere. Since convective clouds are on a scale too small to be resolved in a global model their effects have to be parameterised. However, the whole process of moist convection and especially its parameterisations are associated with uncertainties. In contrast to previous studies on the impact of convection on trace gases, which had commonly neglected the convective transport for some or all compounds, we investigate this issue by examining simulations with five different convection schemes. This permits an uncertainty analysis due to the process formulation, without the inconsistencies inherent in entirely neglecting deep convection or convective tracer transport for one or more tracers. Both the simulated mass fluxes and tracer distributions are analysed. Investigating the distributions of compounds with different characteristics, e.g., lifetime, chemical reactivity, solubility and source distributions, some differences can be attributed directly to the transport of these compounds, whereas others are more related to indirect effects, such as the transport of precursors, chemical reactivity in certain regions, and sink processes. The model simulation data are compared with the average regional profiles of several measurement campaigns, and in detail with two campaigns in fall and winter 2005 in Suriname and Australia, respectively. The shorter-lived a compound is, the larger the differences and consequently the uncertainty due to the convection parameterisation are, as long as it is not completely controlled by local production that is independent of convection and its impacts (e.g. water vapour changes). Whereas for long-lived compounds like CO or O3 the mean differences between the simulations are less than 25%), differences for short-lived compounds reach up to ±100% with different convection schemes. A rating of an overall "best" performing scheme is difficult, since the optimal performance depends on the region and compound.
Tropospheric photooxidation of CF3CH2CHO and CF3(CH2)2CHO initiated by Cl atoms and OH radicals

The absolute rate coefficients for the tropospheric reactions of chlorine (Cl) atoms and hydroxyl (OH) radicals with CF3CH2CHO and CF3(CH2)2CHO were measured as a function of temperature (263–371 K) and pressure (50–215 Torr of He) by pulsed UV laser photolysis techniques. Vacuum UV resonance fluorescence was employed to detect and monitor the time evolution of Cl atoms. Laser induced fluorescence was used in this work for the detection of OH radicals as a function of reaction time. No pressure dependence of the bimolecular rate coefficients, kCl and kOH, was found at all temperatures. At room temperature kCl and kOH were (in 10−11 cm3 molecule−1 s−1): kCl(CF3CH2CHO) = (1.55±0.53); kCl(CF3(CH2)2CHO) = (3.39±1.38); kCl(CF3CH2CHO) = (0.259±0.050); kCl(CF3(CH2)2CHO) = (1.28±0.24). A slightly positive temperature dependence of kCl was observed for CF3CH2CHO and CF3(CH2)2CHO, and kOH(CF3CH2CHO). In contrast, kOH(CF3(CH2)2CHO) did not exhibit a temperature dependence over the range investigated. Arrhenius expressions for these reactions were: kCl(CF3CH2CHO) = (4.4±1.0)×10−11 exp{−(316±68)/T} cm3 molecule−1 s−1 kCl(CF3(CH2)2CHO) = (2.9±0.7)×10−10 exp{−(625±80)/T} cm3 molecule−1 s−1 kOH(CF3CH2CHO) = (7.8±2.2)×10−12 exp{−(314±90)/T} cm3 molecule−1 s−1 The atmospheric impact of the homogeneous removal by OH radicals and Cl atoms of these fluorinated aldehydes is discussed in terms of the global atmospheric lifetimes, taking into account different degradation pathways. The calculated lifetimes show that atmospheric oxidation of CF3(CH2)x CHO are globally dominated by OH radicals, however reactions initiated by Cl atoms can act as a source of free radicals at dawn in the troposphere.
The municipal solid waste landfill as a source of ozone-depleting substances in the United States and United Kingdom

This study provides observation-based national estimates of CFC-11, CFC-12, CFC-113, and 1,1,1-trichloroethane emissions for the United States (US) and United Kingdom (UK) from municipal solid waste (MSW) landfills. The scarcity of national estimates has lead to the assumption that a significant fraction of the lingering ozone-depleting substance (ODS) emissions, which have been detected in industrialized countries, could be emitted from landfills. Spatial coverage was achieved through sampling at seven landfills in Massachusetts and through data provided by nine UK landfills. Linear least square regressions of recovered ODS vs. CH4 were used in combination with national estimates of landfill CH4 emissions to estimate 2006 national US and UK ODS landfill emissions. The ODS landfill emission estimates were then compared to recent estimates of total US and UK ODS emissions. US ODS landfill emissions are 0.4%–1% (0.006–0.09 Gg/year) of total US emissions. UK ODS landfill emission estimates are 1% (0.008 Gg/year) and 6% (0.03 Gg/year) of total UK CFC-11 and CFC-12 emissions, respectively. This indicates that landfills are only a minor source of lingering ODS emissions in the US, but may be more significant for CFC-12 emissions in the UK. The implication is that the majority of current ODS emissions in industrialized countries is likely coming from equipment still in use.
Comparison of aromatic hydrocarbon measurements made by PTR-MS, DOAS and GC-FID during the MCMA 2003 Field Experiment

A comparison of aromatic hydrocarbon measurements is reported for the CENICA supersite in the district of Iztapalapa during the Mexico City Metropolitan Area field experiment in April 2003 (MCMA 2003). Data from three different measurement methods were compared: a Proton Transfer Reaction Mass Spectrometer (PTR-MS), long path measurements using a UV Differential Optical Absorption Spectrometer (DOAS), and Gas Chromatography-Flame Ionization analysis (GC-FID) of canister samples. The principle focus was on the comparison between PTR-MS and DOAS data. Lab tests established that the PTR-MS and DOAS calibrations were consistent for a suite of aromatic compounds including benzene, toluene, p-xylene, ethylbenzene, 1,2,4-trimethylbenzene, phenol and styrene. The point sampling measurements by the PTR-MS and GC-FID showed good correlations (r=0.6), and were in reasonable agreement for toluene, C2-alkylbenzenes and C3-alkylbenzenes. The PTR-MS benzene data were consistently high, indicating interference from ethylbenzene fragmentation for the 145 Td drift field intensity used in the experiment. Correlations between the open-path data measured at 16-m height over a 860-m path length (retroreflector in 430 m distance), and the point measurements collected at 37-m sampling height were best for benzene (r=0.61), and reasonably good for toluene, C2-alkylbenzenes, naphthalene, styrene, cresols and phenol (r>0.5). There was good agreement between DOAS and PTR-MS measurements of benzene after correction for the PTR-MS ethylbenzene interference. Mixing ratios measured by DOAS were on average a factor of 1.7 times greater than the PTR-MS data for toluene, C2-alkylbenzenes, naphthalene and styrene. The level of agreement for the toluene data displayed a modest dependence on wind direction, establishing that spatial gradients – horizontal, vertical, or both – in toluene mixing ratios were significant, and up to a factor of 2 despite the fact that all measurements were conducted above roof level. Our analysis highlights a potential problem in defining a VOC sampling strategy that is meaningful for the comparison with photochemical transport models: meaningful measurements require a spatial fetch that is comparable to the grid cell size of models, which is typically a few 10 km2. Long-path DOAS measurements inherently average over a larger spatial scale than point measurements. The spatial representativeness can be further increased if observations are conducted outside the surface roughness sublayer, which might require measurements at altitudes as high as 10 s of metres above roof level.
A numerical evaluation of global oceanic emissions of α-pinene and isoprene

A numerical evaluation of global oceanic emissions of α-pinene and isoprene based on both "bottom-up" and "top-down" methods is presented. We infer that the global "bottom-up" oceanic emissions of α-pinene and isoprene are 0.013 TgC yr−1 and 0.32 TgC yr−1, respectively. By constraining global chemistry model simulations with the shipborne measurement of Organics over the Ocean Modifying Particles in both Hemispheres summer cruise, we derived the global "top-down" oceanic α-pinene source of 29.5 TgC yr−1 and isoprene source of 11.6 TgC yr−1. Both the "bottom-up" and "top-down" values are subject to large uncertainties. The incomplete understanding of the in-situ phytoplankton communities and their range of emission potentials significantly impact the estimated global "bottom-up" oceanic emissions, while the estimated total amounts of the global "top-down" oceanic sources can be influenced by emission parameterizations, model and input data spatial resolutions, boundary layer mixing processes, and the treatments of chemical reactions. The global oceanic α-pinene source and its impact on organic aerosol formation is significant based on "top-down" method, but is negligible based on "bottom-up" approach. Our research highlights the importance of carrying out further research (especially measurements) to resolve the large offset in the derived oceanic organic emission based on two different approaches.
Simultaneous factor analysis of organic particle and gas mass spectra: AMS and PTR-MS measurements at an urban site

During the winter component of the SPORT (Seasonal Particle Observations in the Region of Toronto) field campaign, particulate non-refractory chemical composition and concentration of selected volatile organic compounds (VOCs) were measured by an Aerodyne time-of-flight aerosol mass spectrometer (AMS) and a proton transfer reaction-mass spectrometer (PTR-MS), respectively. Sampling was performed in downtown Toronto ~15 m from a major road. The mass spectra from the AMS and PTR-MS were combined into a unified dataset, which was analysed using positive matrix factorization (PMF). The two instruments were given balanced weight in the PMF analysis by the application of a scaling factor to the uncertainties of each instrument. A residual based metric, Δesc, was used to evaluate the instrument relative weight within each solution. The PMF analysis yielded a 6-factor solution that included factors characteristic of regional transport, local traffic emissions, charbroiling and oxidative processing. The unified dataset provides information on emission sources (particle and VOC) and atmospheric processing that cannot be obtained from the datasets of the individual instruments: (1) apportionment of oxygenated VOCs to either direct emission sources or secondary reaction products; (2) improved correlation of oxygenated aerosol factors with photochemical age; and (3) increased detail regarding the composition of oxygenated organic aerosol factors. This analysis represents the first application of PMF to a unified AMS/PTR-MS dataset.
Potential climatic impacts and reliability of very large-scale wind farms

Meeting future world energy needs while addressing climate change requires large-scale deployment of low or zero greenhouse gas (GHG) emission technologies such as wind energy. The widespread availability of wind power has fueled substantial interest in this renewable energy source as one of the needed technologies. For very large-scale utilization of this resource, there are however potential environmental impacts, and also problems arising from its inherent intermittency, in addition to the present need to lower unit costs. To explore some of these issues, we use a three-dimensional climate model to simulate the potential climate effects associated with installation of wind-powered generators over vast areas of land or coastal ocean. Using wind turbines to meet 10% or more of global energy demand in 2100, could cause surface warming exceeding 1 °C over land installations. In contrast, surface cooling exceeding 1 °C is computed over ocean installations, but the validity of simulating the impacts of wind turbines by simply increasing the ocean surface drag needs further study. Significant warming or cooling remote from both the land and ocean installations, and alterations of the global distributions of rainfall and clouds also occur. These results are influenced by the competing effects of increases in roughness and decreases in wind speed on near-surface turbulent heat fluxes, the differing nature of land and ocean surface friction, and the dimensions of the installations parallel and perpendicular to the prevailing winds. These results are also dependent on the accuracy of the model used, and the realism of the methods applied to simulate wind turbines. Additional theory and new field observations will be required for their ultimate validation. Intermittency of wind power on daily, monthly and longer time scales as computed in these simulations and inferred from meteorological observations, poses a demand for one or more options to ensure reliability, including backup generation capacity, very long distance power transmission lines, and onsite energy storage, each with specific economic and/or technological challenges.