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  • 1
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 10, No. 1 ( 2017-01-02), p. 1-14
    Abstract: Abstract. Remote sensing of the gaseous composition of non-eruptive, passively degassing volcanic plumes can be a tool to gain insight into volcano interior processes. Here, we report on a field study in September 2015 that demonstrates the feasibility of remotely measuring the volcanic enhancements of carbon dioxide (CO2), hydrogen fluoride (HF), hydrogen chloride (HCl), sulfur dioxide (SO2), and bromine monoxide (BrO) in the downwind plume of Mt. Etna using portable and rugged spectroscopic instrumentation. To this end, we operated the Fourier transform spectrometer EM27/SUN for the shortwave-infrared (SWIR) spectral range together with a co-mounted UV spectrometer on a mobile platform in direct-sun view at 5 to 10 km distance from the summit craters. The 3 days reported here cover several plume traverses and a sunrise measurement. For all days, intra-plume HF, HCl, SO2, and BrO vertical column densities (VCDs) were reliably measured exceeding 5  × 1016, 2  × 1017, 5  × 1017, and 1  × 1014 molec cm−2, with an estimated precision of 2.2  × 1015, 1.3  × 1016, 3.6  × 1016, and 1.3  × 1013 molec cm−2, respectively. Given that CO2, unlike the other measured gases, has a large and well-mixed atmospheric background, derivation of volcanic CO2 VCD enhancements (ΔCO2) required compensating for changes in altitude of the observing platform and for background concentration variability. The first challenge was met by simultaneously measuring the overhead oxygen (O2) columns and assuming covariation of O2 and CO2 with altitude. The atmospheric CO2 background was found by identifying background soundings via the co-emitted volcanic gases. The inferred ΔCO2 occasionally exceeded 2  ×  1019 molec cm−2 with an estimated precision of 3.7  ×  1018 molec cm−2 given typical atmospheric background VCDs of 7 to 8  ×  1021 molec cm−2. While the correlations of ΔCO2 with the other measured volcanic gases confirm the detection of volcanic CO2 enhancements, correlations were found of variable significance (R2 ranging between 0.88 and 0.00). The intra-plume VCD ratios ΔCO2 ∕ SO2, SO2 ∕ HF, SO2 ∕ HCl, and SO2 ∕ BrO were in the range 7.1 to 35.4, 5.02 to 21.2, 1.54 to 3.43, and 2.9  ×  103 to 12.5  ×  103, respectively, showing pronounced day-to-day and intra-day variability.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2505596-3
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  • 2
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 10, No. 1 ( 2017-01-02), p. 1-18
    Abstract: Abstract. It is a widely established fact that standard semi-Lagrangian advection schemes are highly efficient numerical techniques for simulating the transport of atmospheric tracers. However, as they are not formally mass conserving, it is essential to use some method for restoring mass conservation in long time range forecasts. A common approach is to use global mass fixers. This is the case of the semi-Lagrangian advection scheme in the Integrated Forecasting System (IFS) model used by the Copernicus Atmosphere Monitoring Service (CAMS) at the European Centre for Medium-Range Weather Forecasts (ECMWF).Mass fixers are algorithms with substantial differences in complexity and sophistication but in general of low computational cost. This paper shows the positive impact mass fixers have on the inter-hemispheric gradient of total atmospheric column-averaged CO2 and CH4, a crucial feature of their spatial distribution. Two algorithms are compared: the simple "proportional" and the more complex Bermejo–Conde schemes. The former is widely used by several Earth system climate models as well the CAMS global forecasts and analysis of atmospheric composition, while the latter has been recently implemented in IFS. Comparisons against total column observations demonstrate that the proportional mass fixer is shown to be suitable for the low-resolution simulations, but for the high-resolution simulations the Bermejo–Conde scheme clearly gives better results. These results have potential repercussions for climate Earth system models using proportional mass fixers as their resolution increases. It also emphasises the importance of benchmarking the tracer mass fixers with the inter-hemispheric gradient of long-lived greenhouse gases using observations.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2456725-5
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 12 ( 2023-06-22), p. 6897-6922
    Abstract: Abstract. Methane (CH4) is a potent greenhouse gas, and anthropogenic CH4 emissions contribute significantly to global warming. In this study, the CH4 emissions of the second most populated city in Germany, Hamburg, were quantified with measurements from four solar-viewing Fourier transform infrared (FTIR) spectrometers, mobile in situ measurements, and an inversion framework. For source type attribution, an isotope ratio mass spectrometer was deployed in the city. The urban district hosts an extensive industrial and port area in the south as well as a large conglomerate of residential areas north of the Elbe River. For emission modeling, the TNO GHGco (Netherlands Organisation for Applied Scientific Research greenhouse gas and co-emitted species emission database) inventory was used as a prior for the inversion. In order to improve the inventory, two approaches were followed: (1) the addition of a large natural CH4 source, the Elbe River, which was previously not included in the inventory, and (2) mobile measurements were carried out to update the spatial distribution of emissions in the TNO GHGco gridded inventory and derive two updated versions of the inventory. The addition of the river emissions improved model performance, whereas the correction of the spatial distribution with mobile measurements did not have a significant effect on the total emission estimates for the campaign period. A comparison of the updated inventories with emission estimates from a Gaussian plume model (GPM) showed that the updated versions of the inventory match the GPM emissions estimates well in several cases, revealing the potential of mobile measurements to update the spatial distribution of emission inventories. The mobile measurement survey also revealed a large and, at the time of the study, unknown point source of thermogenic origin with a magnitude of 7.9 ± 5.3 kg h−1 located in a refinery. The isotopic measurements show strong indications that there is a large biogenic CH4 source in Hamburg that produced repeated enhancements of over 1 ppm which correlated with the rising tide of the river estuary. The CH4 emissions (anthropogenic and natural) of the city of Hamburg were quantified as 1600 ± 920 kg h−1, 900 ± 510 kg h−1 of which is of anthropogenic origin. This study reveals that mobile street-level measurements may miss the majority of total methane emissions, potentially due to sources located within buildings, including stoves and boilers operating on natural gas. Similarly, the CH4 enhancements recorded during the mobile survey from large-area sources, such as the Alster lakes, were too small to generate GPM emission estimates with confidence, but they could nevertheless influence the emission estimates based on total column measurements.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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