Tanja J. Schuck

Imposing strong constraints on tropical terrestrial CO2 fluxes using passenger aircraft based measurements

[1] Because very few measurements of atmospheric carbon dioxide (CO2) are available in the tropics, estimates of surface CO2 fluxes in tropical regions are beset with considerable uncertainties. To improve estimates of tropical terrestrial fluxes, atmospheric CO2 inversion was performed using passenger aircraft based measurements of the Comprehensive Observation Network for Trace gases by Airliner (CONTRAIL) project in addition to the surface measurement data set of GLOBALVIEW–CO2. Regional monthly fluxes at the earth’s surface were estimated using the Bayesian synthesis approach focusing on the period 2006–2008 using the Nonhydrostatic Icosahedral Atmospheric Model-based Transport Model (NICAM-TM). By adding the aircraft to the surface data, the posterior flux errors were greatly reduced; specifically, error reductions of up to 64% were found for tropical Asia regions. This strong impact is closely related to efficient vertical transport in the tropics. The optimized surface fluxes using the CONTRAIL data were evaluated by comparing the simulated atmospheric CO2 distributions with independent aircraft measurements of the Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC) project. The inversion with the CONTRAIL data yields the global carbon sequestration rates of 2.22 � 0.28 Pg C yr � 1 for the terrestrial biosphere and 2.24 � 0.27 Pg C yr � 1 for the oceans (the both are adjusted by riverine input of CO2). For the first time the CONTRAIL CO2 measurements were used in an inversion system to identify the areas of greatest impact in terms of reducing flux uncertainties.

Distribution of methane in the tropical upper troposphere measured by CARIBIC and CONTRAIL aircraft

Received 29 May 2012; revised 8 August 2012; accepted 16 August 2012; published 4 October 2012. [1] We investigate the upper tropospheric distribution of methane (CH4) at low latitudes based on the analysis of air samples collected from aboard passenger aircraft. The distribution of CH4 exhibits spatial and seasonal differences, such as the pronounced seasonal cycles over tropical Asia and elevated mixing ratios over central Africa. Over Africa, the correlations of methane, ethane, and acetylene with carbon monoxide indicate that these high mixing ratios originate from biomass burning as well as from biogenic sources. Upper tropospheric mixing ratios of CH4were modeled using a chemistry transport model. The simulation captures the large-scale features of the distributions along different flight routes, but discrepancies occur in some regions. Over Africa, where emissions are not well constrained, the model predicts a too steep interhemispheric gradient. During summer, efficient convective vertical transport and enhanced emissions give rise to a large-scale CH4 maximum in the upper troposphere over subtropical Asia. This seasonal (monsoonal) cycle is analyzed with a tagged tracer simulation. The model confirms that in this region convection links upper tropospheric mixing ratios to regional sources on the Indian subcontinent, subtropical East Asia, and Southeast Asia. This type of aircraft data can therefore provide information about surface fluxes.

Chemical composition and morphology of individual aerosol particles from a CARIBIC flight at 10 km altitude between 50°N and 30°S

Analysis of individual particles by analytical electron microscopy as well as quantitative analysis using particle-induced X-ray emission (PIXE) and particle elastic scattering analysis (PESA) were carried out on samples collected from a flight at 10 km altitude between 50 degrees N and 30 degrees S as part of the Civil Aircraft for Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC) project (http://www.caribic-atmospheric.com). Particle morphology showed large variability with sampling latitude. Complicated branched structures dominated the large particles of the extratropical northern and southern hemisphere and the northern tropics. Particles in the tropics of the southern hemisphere were small in size and large in number concentration, whereas particles in or close to the intertropical convergence zone were few and small in size. Particles in the lowermost stratosphere were found to have similar structures but more branched than the ones found in the upper troposphere of the extratropics. Quantitative analysis revealed that the sulfur concentration varied by a factor of 50 in the nine samples analyzed in this study. The carbon-to-sulfur mass concentration ratio was lowest in the lowermost stratosphere (0.5) and highest in the tropics of the southern hemisphere (3.5). The elemental distribution of carbon and sulfur in individual particles was mapped by energy-filtered transmission electron microscopy (EFTEM). Almost all particles analyzed contained a mixture of carbonaceous and sulfurous matter. Particles with satellites were found by EFTEM to contain both carbon and sulfur in the central particle, whereas in the satellite particles only carbonaceous material was detected. (Less)

Investigation of chlorine radical chemistry in the Eyjafjallajökull volcanic plume using observed depletions in non‐methane hydrocarbons

As part of the effort to understand volcanic plume composition and chemistry during the eruption of the Icelandic volcano Eyjafjallajkull, the CARIBIC atmospheric observatory was deployed for three special science flights aboard a Lufthansa passenger aircraft. Measurements made during these flights included the collection of whole air samples, which were analyzed for non-methane hydrocarbons (NMHCs). Hydrocarbon concentrations in plume samples were found to be reduced to levels below background, with relative depletions characteristic of reaction with chlorine radicals (Cl). Recent observations of halogen oxides in volcanic plumes provide evidence for halogen radical chemistry, but quantitative data for free halogen radical concentrations in volcanic plumes were absent. Here we present the first observation-based calculations of Cl radical concentrations in volcanic plumes, estimated from observed NMHC depletions. Inferred Cl concentrations were between 1.3 × 10 and 6.6 × 10 Cl cm. The relationship between NMHC variability and local lifetimes was used to investigate the ratio between OH and Cl within the plume, with [OH]/[Cl] estimated to be ∼37. Copyright 2011 by the American Geophysical Union.