Constraints on oceanic methane emissions west of Svalbard from atmospheric in situ measurements and Lagrangian transport modeling.

Methane stored in seabed reservoirs such as methane hydrates can reach the atmosphere in the form of bubbles or dissolved in water. Hydrates could destabilize with rising temperature further increasing greenhouse gas emissions in a warming climate. To assess the impact of oceanic emissions from the area west of Svalbard, where methane hydrates are abundant, we used measurements collected with a research aircraft (Facility for Airborne Atmospheric Measurements) and a ship (Helmer Hansen) during the Summer 2014 and for Zeppelin Observatory for the full year. We present a model-supported analysis of the atmospheric CH4 mixing ratios measured by the different platforms. To address uncertainty about where CH4 emissions actually occur, we explored three scenarios: areas with known seeps, a hydrate stability model, and an ocean depth criterion. We then used a budget analysis and a Lagrangian particle dispersion model to compare measurements taken upwind and downwind of the potential CH4 emission areas. We found small differences between the CH4 mixing ratios measured upwind and downwind of the potential emission areas during the campaign. By taking into account measurement and sampling uncertainties and by determining the sensitivity of the measured mixing ratios to potential oceanic emissions, we provide upper limits for the CH4 fluxes. The CH4 flux during the campaign was small, with an upper limit of 2.5 nmol m-2 s-1 in the stability model scenario. The Zeppelin Observatory data for 2014 suggest CH4 fluxes from the Svalbard continental platform below 0.2 Tg yr-1. All estimates are in the lower range of values previously reported.

Street canyon aerosol pollutant transport measurements.

Current understanding of dispersion in street canyons is largely derived from relatively simple dispersion models. Such models are increasingly used in planning and regulation capacities but are based upon a limited understanding of the transport of substances within a real canyon. In recent years, some efforts have been made to numerically model localised flow in idealised canyons (e.g., J. Appl. Meteorol. 38 (1999) 1576-89) and stepped canyons (Assimakopoulos V. Numerical modelling of dispersion of atmospheric pollution in and above urban canopies. PhD thesis, Imperial College, London, 2001) but field studies in real canyons are rare. To further such an understanding, a measurement campaign has been conducted in an asymmetric street canyon with busy one-way traffic in central Manchester in northern England. The eddy correlation method was used to determine fluxes of size-segregated accumulation mode aerosol. Measurements of aerosol at a static location were made concurrently with measurements on a platform lift giving vertical profiles. Size-segregated measurements of ultrafine and coarse particle concentrations were also made simultaneously at various heights. In addition, a small mobile system was used to make measurements of turbulence at various pavement locations within the canyon. From this data, various features of turbulent transport and dispersion in the canyon will be presented. The concentration and the ventilation fluxes of vehicle-related aerosol pollutants from the canyon will be related to controlling factors. The results will also be compared with citywide ventilation data from a separate measurement campaign conducted above the urban canopy.

The influence of small aerosol particles on the properties of water and ice clouds.

In this paper, results are presented of the influence of small organic- and soot-containing particles on the formation of water and ice clouds. There is strong evidence that these particles have grown from nano particle seeds produced by the combustion of oil products. Two series of field experiments are selected to represent the observations made. The first is the CLoud-Aerosol Characterisation Experiment (CLACE) series of experiments performed at a high Alpine site (Jungfraujoch), where cloud was in contact with the ground and the measuring station. Both water and ice clouds were examined at different times of the year. The second series of experiments is the CLOud Processing of regional Air Pollution advecting over land and sea (CLOPAP) series, where ageing pollution aerosol from UK cities was observed, from an airborne platform, to interact with warm stratocumulus cloud in a cloud-capped atmospheric boundary layer. Combining the results it is shown that aged pollution aerosol consists of an internal mixture of organics, sulfate, nitrate and ammonium, the organic component is dominated by highly oxidized secondary material. The relative contributions and absolute loadings of the components vary with location and season. However, these aerosols act as Cloud Condensation Nuclei (CCN) and much of the organic material, along with the other species, is incorporated into cloud droplets. In ice and mixed phase cloud, it is observed that very sharp transitions (extending over just a few metres) are present between highly glaciated regions and regions consisting of supercooled water. This is a unique finding; however, aircraft observations in cumulus suggest that this kind of structure may be found in these cloud types too. It is suggested that this sharp transition is caused by ice nucleation initiated by oxidised organic aerosol coated with sulfate in more polluted regions of cloud, sometimes enhanced by secondary ice particle production in these regions.