Long-range Transport Pathways Research Articles

The LAGRANTO Lagrangian analysis tool – version 2.0

Abstract. Lagrangian trajectories are widely used in the atmospheric sciences, for instance to identify flow structures in extratropical cyclones (e.g., warm conveyor belts) and long-range transport pathways of moisture and trace substances. Here a new version of the Lagrangian analysis tool LAGRANTO (Wernli and Davies, 1997) is introduced, which offers considerably enhanced functionalities. Trajectory starting positions can be defined easily and flexibly based on different geometrical and/or meteorological conditions, e.g., equidistantly spaced within a prescribed region and on a stack of pressure (or isentropic) levels. After the computation of the trajectories, a versatile selection of trajectories is offered based on single or combined criteria. These criteria are passed to LAGRANTO with a simple command language (e.g., "GT:PV:2" readily translates into a selection of all trajectories with potential vorticity, PV, greater than 2 PVU; 1 PVU = 10−6 K m2 kg−1 s−1). Full versions of this new version of LAGRANTO are available for global ECMWF and regional COSMO data, and core functionality is provided for the regional WRF and MetUM models and the global 20th Century Reanalysis data set. The paper first presents the intuitive application of LAGRANTO for the identification of a warm conveyor belt in the North Atlantic. A further case study then shows how LAGRANTO can be used to quasi-operationally diagnose stratosphere–troposphere exchange events. Whereas these examples rely on the ECMWF version, the COSMO version and input fields with 7 km horizontal resolution serve to resolve the rather complex flow structure associated with orographic blocking due to the Alps, as shown in a third example. A final example illustrates the tool's application in source–receptor analysis studies. The new distribution of LAGRANTO is publicly available and includes auxiliary tools, e.g., to visualize trajectories. A detailed user guide describes all LAGRANTO capabilities.

The effect of long-range air mass transport pathways on PM10 and NO2 concentrations at urban and rural background sites in Ireland: Quantification using clustering techniques

The specific aims of this paper are to: (i) quantify the effects of various long range transport pathways nitrogen dioxide (NO2) and particulate matter with diameter less than 10μm (PM10) concentrations in Ireland and identify air mass movement corridors which may lead to incidences poor air quality for application in forecasting; (ii) compare the effects of such pathways at various sites; (iii) assess pathways associated with a period of decreased air quality in Ireland. The origin of and the regions traversed by an air mass 96h prior to reaching a receptor is modelled and k-means clustering is applied to create air-mass groups. Significant differences in air pollution levels were found between air mass cluster types at urban and rural sites. It was found that easterly or recirculated air masses lead to higher NO2 and PM10 levels with average NO2 levels varying between 124% and 239% of the seasonal mean and average PM10 levels varying between 103% and 199% of the seasonal mean at urban and rural sites. Easterly air masses are more frequent during winter months leading to higher overall concentrations. The span in relative concentrations between air mass clusters is highest at the rural site indicating that regional factors are controlling concentration levels. The methods used in this paper could be applied to assist in modelling and forecasting air quality based on long range transport pathways and forecast meteorology without the requirement for detailed emissions data over a large regional domain or the use of computationally demanding modelling techniques.

Perfluoroalkyl Acids in the Atlantic and Canadian Arctic Oceans

We report here on the spatial distribution of C(4), C(6), and C(8) perfluoroalkyl sulfonates, C(6)-C(14) perfluoroalkyl carboxylates, and perfluorooctanesulfonamide in the Atlantic and Arctic Oceans, including previously unstudied coastal waters of North and South America, and the Canadian Arctic Archipelago. Perfluorooctanoate (PFOA) and perfluorooctanesulfonate (PFOS) were typically the dominant perfluoroalkyl acids (PFAAs) in Atlantic water. In the midnorthwest Atlantic/Gulf Stream, sum PFAA concentrations (∑PFAAs) were low (77-190 pg/L) but increased rapidly upon crossing into U.S. coastal water (up to 5800 pg/L near Rhode Island). ∑PFAAs in the northeast Atlantic were highest north of the Canary Islands (280-980 pg/L) and decreased with latitude. In the South Atlantic, concentrations increased near Rio de la Plata (Argentina/Uruguay; 350-540 pg/L ∑PFAAs), possibly attributable to insecticides containing N-ethyl perfluorooctanesulfonamide, or proximity to Montevideo and Buenos Aires. In all other southern hemisphere locations, ∑PFAAs were <210 pg/L. PFOA/PFOS ratios were typically ≥1 in the northern hemisphere, ∼1 near the equator, and ≤1 in the southern hemisphere. In the Canadian Arctic, ∑PFAAs ranged from 40 to 250 pg/L, with perfluoroheptanoate, PFOA, and PFOS among the PFAAs detected at the highest concentrations. PFOA/PFOS ratios (typically ≫1) decreased from Baffin Bay to the Amundsen Gulf, possibly attributable to increased atmospheric inputs. These data help validate global emissions models and contribute to understanding of long-range transport pathways and sources of PFAAs to remote regions.

Manufacturing Origin of Perfluorooctanoate (PFOA) in Atlantic and Canadian Arctic Seawater

The extent to which different manufacturing sources and long-range transport pathways contribute to perfluorooctanoate (PFOA) in the world's oceans, particularly in remote locations, is widely debated. Here, the relative contribution of historic (i.e., electrochemically fluorinated) and contemporary (i.e., telomer) manufacturing sources was assessed for PFOA in various seawater samples by an established isomer profiling technique. The ratios of individual branched PFOA isomers were indistinguishable from those in authentic historic standards in 93% of the samples examined, indicating that marine processes had little influence on isomer profiles, and that isomer profiling is a valid source apportionment tool for seawater. Eastern Atlantic PFOA was largely (83-98%) of historic origin, but this decreased to only 33% close to the Eastern U.S. seaboard. Similarly, PFOA in the Norwegian Sea was near exclusively historic, but the relative contribution decreased to ∼50% near the Baltic Sea. Such observations of contemporary PFOA in coastal source regions coincided with elevated concentrations, suggesting that the continued production and use of PFOA is currently adding to the marine burden of this contaminant. In the Arctic, a spatial trend was observed whereby PFOA in seawater originating from the Atlantic was predominantly historic (up to 99%), whereas water in the Archipelago (i.e., from the Pacific) was predominantly of contemporary origin (as little as 17% historic). These data help to explain reported temporal and spatial trends from Arctic wildlife biomonitoring, and suggest that the dominant PFOA source(s) to the Pacific and Canadian Arctic Archipelago are either (a) from direct emissions of contemporary PFOA via manufacturing or use in Asia, or (b) from atmospheric transport and oxidation of contemporary PFOA-precursors.

Interfacial Engineering of Organic Nanofibril Heterojunctions into Highly Photoconductive Materials

Photoconductive organic materials have gained increasing interest in various optoelectronics, such as sensors, photodetectors, and photovoltaics. However, the availability of such materials is very limited due to their intrinsic low charge carrier density and mobility. Here, we present a simple approach based on nanofibril heterojunction to achieve high photoconductivity with fast photoresponse, that is, interfacial engineering of electron donor (D) coating onto acceptor (A) nanofibers via optimization of hydrophobic interaction between long alkyl side-chains. Such nanofibril heterojunctions possess two prominent features that are critical for efficient photocurrent generation: the nanofibers both create a large D/A interface for increased charge separation and act as long-range transport pathways for photogenerated charge carriers toward the electrodes, and the alkyl groups employed not only enable effective surface adsorption of D molecules on the nanofibers for effective electron-transfer communication, but also spatially separate the photogenerated charge carriers to prevent their recombination. The reported approach represents a simple, adaptable method that allows for the development and optimization of photoconductive organic materials.