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In situ and denuder-based measurements of elemental and reactive gaseous mercury with analysis by laser-induced fluorescence – results from the Reno Atmospheric Mercury Intercomparison Experiment

The University of Miami (UM) deployed a sequential two-photon laser-induced fluorescence (2P-LIF) instrument for the in situ measurement of gaseous elemental mercury, Hg(0), during the Reno Atmospheric Mercury Intercomparison Experiment (RAMIX) campaign. A number of extended sampling experiments, typically lasting 6–8 h but on one occasion extending to ∼ 24 h, were conducted, allowing the 2P-LIF measurements of Hg(0) concentrations to be compared with two independently operated instruments using gold amalgamation sampling coupled with cold vapor atomic fluorescence spectroscopic (CVAFS) analysis. At the highest temporal resolution, ∼ 5 min samples, the three instruments measured concentrations that agreed to within 10–25 %. Measurements of total mercury (TM) were made by using pyrolysis to convert total oxidized mercury (TOM) to Hg(0). TOM was then obtained by difference. Variability in the ambient Hg(0) concentration limited our sensitivity for measurement of ambient TOM using this approach. In addition, manually sampled KCl-coated annular denuders were deployed and analyzed using thermal dissociation coupled with single-photon LIF detection of Hg(0). The TOM measurements obtained were normally consistent with KCl denuder measurements obtained with two Tekran speciation systems and with the manual KCl denuder measurements but with very large uncertainty. They were typically lower than measurements reported by the University of Washington (UW) Detector for Oxidized Hg Species (DOHGS) system. The ability of the 2P-LIF pyrolysis system to measure TM was demonstrated during one of the manifold HgBr2 spikes but the results did not agree well with those reported by the DOHGS system. The limitations of the RAMIX experiment and potential improvements that should be implemented in any future mercury instrument intercomparison are discussed. We suggest that instrumental artifacts make a substantial contribution to the discrepancies in the reported measurements over the course of the RAMIX campaign. This suggests that caution should be used in drawing significant implications for the atmospheric cycling of mercury from the RAMIX results.
Impacts of air pollution and climate on materials in Athens, Greece

For more than 10 years now the National and Kapodistrian University of Athens, Greece, has contributed to the UNECE (United Nations Economic Commission for Europe) ICP Materials (International Co-operative Programme on Effects on Materials including Historic and Cultural Monuments) programme for monitoring the corrosion/soiling levels of different kinds of materials due to environmental air-quality parameters. In this paper we present the results obtained from the analysis of observational data that were collected in Athens during the period 2003–2012. According to these results, the corrosion/soiling of the particular exposed materials tends to decrease over the years, except for the case of copper. Based on this long experimental database that is applicable to the multi-pollutant situation in the Athens basin, we present dose–response functions (DRFs) considering that <q>dose</q> stands for the air pollutant concentration, <q>response</q> for the material mass loss (normally per annum) and <q>function</q>, the relationship derived by the best statistical fit to the data.
A statistical approach for estimating representative emission rates of biogenic volatile organic compounds and their determination for 192 plant species/genera in China

To obtain more and accurate biogenic volatile organic compound (BVOC) emission rates for more plant species in China and further improve the accuracy of emission rates used in BVOC emission inventories, we conducted field measurements and developed a statistical approach for estimating representative emission rates. We performed field measurements of BVOC emissions from 50 plant species at nine locations in China using our established semi-static enclosure system. The emissions of 102 VOCs, including isoprene, α-pinene, β-pinene, and other VOC species, were analyzed with a custom-built online gas chromatography-mass spectrometry/flame ionization detector system. From the results, broadleaf trees were the greatest potential emitters of isoprene, while needle-leaf trees emitted more pinene. Shrubs had lower isoprene and pinene emission potentials, but higher emission potentials for other VOCs. Methyl methacrylate, isopropylbenzene, isopentane, acetone, ethane, propane, toluene, and xylene were the dominant species among other VOCs, probably with high emission intensities. Therefore, their emissions should be considered in future global and regional BVOC estimation studies. Next, we summarized our field measurements along with reported emission rates from China and abroad. The emission intensity categories were produced based on statistics, with more detailed categories, accurate emission rate intervals and representative rates compared to previous studies. The results showed that the BVOC emission intensities of plants displayed different categories, such as lowest, lower, low, moderate, high, higher, and highest. The isoprene emission rate intervals and representative rates were: lowest, 0.08–0.11 and 0.1 μg C gdw−1 h−1; lower, 0.9–1.3 and 1.0 μg C gdw−1 h−1; low, 5.2–6.5 and 5.8 μg C gdw−1 h−1; moderate, 13.1–15.3 and 14.4 μg C gdw−1 h−1; high, 31.1–37.0 and 33.6 μg C gdw−1 h−1; higher, 67.2–75.1 and 70.1 μg C gdw−1 h−1; and highest, 135.1–157.6 and 142.5 μg C gdw−1 h−1. The monoterpene emission rate intervals and representative rates were: lowest, 0.08–0.11 and 0.1 μg C gdw−1 h−1; lower, 0.17–0.22 and 0.2 μg C gdw−1 h−1; low, 0.5–0.7 and 0.6 μg C gdw−1 h−1; moderate, 1.2–1.5 and 1.4 μg C gdw−1 h−1; high, 2.8–3.3 and 3.0 μg C gdw−1 h−1; and higher, 11.1–14.9 and 12.6 μg C gdw−1 h−1. Using these established emission intervals, we determined the isoprene and monoterpene emission rates for 192 plant species/genera in China, including 30 dominant tree species, 149 shrub and grass genera, and 13 crop species. These estimations would be further improved by integrating larger quantities of rigorous field measurements from China in the future.
Characterisation of Central-African aerosol and trace-gas emissions based on MAX-DOAS measurements and model simulations over Bujumbura, Burundi

We present MAX-DOAS measurements of NO2, HCHO, and aerosols performed in Central Africa, in the city of Bujumbura, Burundi (3.38° S, 29.3° E). A MAX-DOAS instrument has been operated at this location by BIRA-IASB since late 2013. Aerosol-extinction and trace-gas vertical profiles are retrieved by applying the optimal-estimation-based profiling tool bePRO to the measured O4, NO2 and HCHO slant-column densities. The MAX-DOAS vertical columns and profiles are used for investigating the diurnal and seasonal cycles of NO2, HCHO, and aerosols. Regarding the aerosols, the retrieved AODs are compared to co-located AERONET sun-photometer measurements for verification purposes, while in the case of NO2 and HCHO, the MAX-DOAS vertical columns and profiles are compared to GOME-2 and OMI satellite observations. To characterise the biomass-burning and biogenic emissions in the Bujumbura region, the trace gases and aerosol MAX-DOAS retrievals are used in combination with MODIS fire radiative-power values and the tropospheric 3D chemical transport model IMAGES, as well as simulations from the NOAA backward-trajectory model HYSPLIT. The first results show that the aerosol and HCHO seasonal variation is driven by the alternation of rain and dry periods, the latter being associated with intense biomass-burning agricultural activities and forest fires in the south/south-east and transport from this region to Bujumbura. In contrast, NO2 is seen to depend mainly on local emissions close to the city, due to the short lifetime of this species (typically 1–2 hours).
Revisiting the observed surface climate response to large volcanic eruptions

In light of the range in presently available observational, reanalysis and model data, we revisit the surface climate response to large tropical volcanic eruptions from the end of the 19th century until present. We focus on the dynamically driven response of the North Atlantic Oscillation (NAO) and the radiative-driven tropical temperature response. Using 10 different reanalysis products and the Hadley Centre Sea Level Pressure observational dataset (HadSLP2) we confirm a positive tendency in the phase of the NAO during boreal winters following large volcanic eruptions, although we conclude that it is not as clear cut as the current literature suggests. While different reanalyses agree well on the sign of the surface volcanic NAO response for individual volcanoes, the spread in the response is often large (∼ 1/2 standard deviation). This inter-reanalysis spread is actually larger for the more recent volcanic eruptions, and in one case does not encompass observations (El Chichón). These are all in the satellite era and therefore assimilate more atmospheric data that may lead to a more complex interaction for the surface response. The phase of the NAO leads to a dynamically driven warm anomaly over northern Europe in winter, which is present in all datasets considered. The general cooling of the surface temperature due to reduced incoming shortwave radiation is therefore disturbed by dynamical impacts. In the tropics, where less dynamically driven influences are present, we confirm a predominant cooling after most but not all eruptions. All datasets agree well on the strength of the tropical response, with the observed and reanalysis response being statistically significant but the modelled response not being significant due to the high variability across models.
Diurnal variability of the atmospheric boundary layer height over a tropical station in the Indian monsoon region

The diurnal variation of atmospheric boundary layer (ABL) height is studied using high-resolution radiosonde observations available at 3 h intervals for 3 days continuously from 34 intensive campaigns conducted during the period December 2010–March 2014 over a tropical station Gadanki (13.5° N, 79.2° E; 375 m), in the Indian monsoon region. The heights of the ABL during the different stages of its diurnal evolution, namely, the convective boundary layer (CBL), the stable boundary layer (SBL), and the residual layer (RL) are obtained to study the diurnal variabilities. A clear diurnal variation is observed in 9 campaigns out of the 34 campaigns. In 7 campaigns the SBL did not form in the entire day and in the remaining 18 campaigns the SBL formed intermittently. The SBL forms for 33–55 % of the time during nighttime and 9 and 25 % during the evening and morning hours, respectively. The mean SBL height is within 0.3 km above the surface which increases slightly just after midnight (02:00 IST) and remains almost constant until the morning. The mean CBL height is within 3.0 km above the surface, which generally increases from morning to evening. The mean RL height is within 2 km above the surface which generally decreases slowly as the night progresses. The diurnal variation of the ABL height over the Indian region is stronger during the pre-monsoon and weaker during winter season. The CBL is higher during the summer monsoon and lower during the winter season while the RL is higher during the winter season and lower during the summer season. During all the seasons, the ABL height peaks during the afternoon (∼ 14:00 IST) and remains elevated until evening (∼ 17:00 IST). The ABL suddenly collapses at 20:00 IST and increases slightly in the night. Interestingly, it is found that the low level clouds have an effect on the ABL height variability, but the deep convective clouds do not. The lifting condensation level (LCL) is generally found to occur below the ABL for the majority of the database and they are randomly related.
Substorm onset identification using neural networks and Pi2 pulsations

The pattern recognition capabilities of artificial neural networks (ANNs) have for the first time been used to identify Pi2 pulsations in magnetometer data, which in turn serve as indicators of substorm onsets and intensifications. The pulsation spectrum was used as input to the ANN and the network was trained to give an output of +1 for Pi2 signatures and -1 for non-Pi2 signatures. In order to evaluate the degree of success of the neural-network procedure for identifying Pi2 pulsations, the ANN was used to scan a number of data sets and the results compared with visual identification of Pi2 signatures. The ANN performed extremely well with a success rate of approximately 90% for Pi2 identification and a timing accuracy generally within 1 min compared to visual identification. A number of potential applications of the neural-network Pi2 scanning procedure are discussed.
Spatial structure of the plasma sheet boundary layer at distances greater than 180 RE as derived from energetic particle measurements on GEOTAIL

We have analyzed the onsets of energetic particle bursts detected by the ICS and STICS sensors of the EPIC instrument on board the GEOTAIL spacecraft in the deep magnetotail (i.e., at distances greater than 180 RE). Such bursts are commonly observed at the plasma-sheet boundary layer (PSBL) and are highly collimated along the magnetic field. The bursts display a normal velocity dispersion (i.e., the higher-speed particles are seen first, while the progressively lower speed particles are seen later) when observed upon entry of the spacecraft from the magnetotail lobes into the plasma sheet. Upon exit from the plasma sheet a reverse velocity dispersion is observed (i.e., lower-speed particles disappear first and higher-speed particles disappear last). Three major findings are as follows. First, the tailward-jetting energetic particle populations of the distant-tail plasma sheet display an energy layering: the energetic electrons stream along open PSBL field lines with peak fluxes at the lobes. Energetic protons occupy the next layer, and as the spacecraft moves towards the neutral sheet progressively decreasing energies are encountered systematically. These plasma-sheet layers display spatial symmetry, with the plane of symmetry the neutral sheet. Second, if we consider the same energy level of energetic particles, then the H+ layer is confined within that of the energetic electron, the He++ layer is confined within that of the proton, and the oxygen layer is confined within the alpha particle layer. Third, whenever the energetic electrons show higher fluxes inside the plasma sheet as compared to those at the boundary layer, their angular distribution is isotropic irrespective of the Earthward or tailward character of fluxes, suggesting a closed field line topology.
Optimisation of a parallel ocean general circulation model

This paper presents the development of a general-purpose parallel ocean circulation model, for use on a wide range of computer platforms, from traditional scalar machines to workstation clusters and massively parallel processors. Parallelism is provided, as a modular option, via high-level message-passing routines, thus hiding the technical intricacies from the user. An initial implementation highlights that the parallel efficiency of the model is adversely affected by a number of factors, for which optimisations are discussed and implemented. The resulting ocean code is portable and, in particular, allows science to be achieved on local workstations that could otherwise only be undertaken on state-of-the-art supercomputers.
Assessment of the ocean circulation in the Azores region as predicted by a numerical model assimilating altimeter data from Topex/Poseidon and ERS-1 satellites

Two years of altimetric data from Topex/Poseidon (October 1992–September 1994) and ERS-1 (October 1992–December 1993) were assimilated into a numerical model of the North Atlantic. The results of these simulations are analysed in the Azores region to assess the performance of our model in this particular region. Maps of instantaneous dynamic topography and transports show that the model performs well in reproducing the velocities and transports of the Azores Front. Drifter data from the Semaphore experiment are also used to study the correlation between the drifter velocities and the corresponding model velocities. Some interesting oceanographic results are also obtained by examining the seasonal and interannual variability of the circulation and the influence of bathymetry on the variability of the Azores Front. Thus, on the basis of our two year experiment, it is possible to confirm the circulation patterns proposed by previous studies regarding the seasonal variations in the origin of the Azores Current. Moreover, it is shown that the Azores Current is quite narrow in the first year of assimilation (1992–1993), but becomes much wider in the second year (1993–1994). The role of the bathymetry appears important in this area since the mesoscale activity is shown to be strongly related to the presence of topographic slopes. Finally, spectral analyses of sea-level changes over time and space are used to identify two types of wave already noticed in other studies: a wave with (300 km)–1 wave number and (120 days)–1 frequency, which is characteristic of mesoscale undulation, and a wave with (600 km)–1 wave number and (250 days)–1 frequency which probably corresponds to a Rossby wave generated in the east of the basin.