Abstract. Excessive numerical diffusion is one of the major limitations in the representation of long-range transport by chemistry transport models. In the present study, we focus on excessive diffusion in the vertical direction, which has been shown to be a major issue, and we explore three possible ways of addressing this problem: increasing the vertical resolution, using an advection scheme with anti-diffusive properties and more accurately representing the vertical wind. This study was carried out using the CHIMERE chemistry transport model for the 18 March 2012 eruption of Mount Etna, which released about 3 kt of sulfur dioxide into the atmosphere in a plume that was observed by satellite instruments (the Infrared Atmospheric Sounding Interferometer instrument, IASI, and the Ozone Monitoring Instrument, OMI) for several days. The change from the classical Van Leer (1977) scheme to the Després and Lagoutière (1999) anti-diffusive scheme in the vertical direction was shown to provide the largest improvement to model outputs in terms of preserving the thin plume emitted by the volcano. To a lesser extent, the improved representation of the vertical wind field was also shown to reduce plume dispersion. Both of these changes helped to reduce vertical diffusion in the model as much as a brute-force approach (increasing vertical resolution).
Abstract:Monitoring gaseous and particulate volcanic emissions with remote observations is of particular importance for climate studies, air quality and natural risk assessment. The concurrent impact of the simultaneous presence of sulphur dioxide (SO 2 ) emissions and the subsequently formed secondary sulphate aerosols (SSA) on the thermal infraRed (TIR) satellite observations is not yet well quantified. In this paper, we present the first assessment of the combined sensitivity of pseudo-observations from three TIR satellite instruments (the Infrared Atmospheric Sounding Interferometer (IASI), the MODerate resolution Imaging Spectro radiometer (MODIS) and the Spinning Enhanced Visible and InfraRed Imager (SEVIRI)) to these two volcanic effluents, following an idealized moderate stratospheric eruption. Direct radiative transfer calculations have been performed using the 4A (Automatized Atmospheric Absorption Atlas) radiative transfer model during short-term atmospheric sulphur cycle evolution. The results show that the mutual effect of the volcanic SO 2 and SSA on the TIR outgoing radiation is obvious after three to five days from the eruption. Therefore, retrieval efforts of SO 2 concentration should consider the progressively formed SSA and vice-versa. This result is also confirmed by estimating the information content of the TIR pseudo-observations to the bi-dimensional retrieved vector formed by the total masses of sulphur dioxide and sulphate aerosols. We find that it is important to be careful when attempting to quantify SO 2 burdens in aged volcanic plumes using broad-band instruments like SEVIRI and MODIS as these retrievals present high uncertainties. For IASI, the total errors are smaller and the two parameters can be retrieved as independent quantities.
We developed a new retrieval algorithm based on the Infrared Atmospheric Sounding Interferometer (IASI) observations, called AEROIASI-H2SO4, to measure the extinction and mass concentration of sulphate aerosols (binary solution droplets of sulphuric acid and water), with moderate random uncertainties (typically ∼35% total uncertainty for column mass concentration estimations). The algorithm is based on a self-adapting Tikhonov–Phillips regularization method. It is here tested over a moderate-intensity eruption of Mount Etna volcano (18 March 2012), Italy, and is used to characterise this event in terms of the spatial distribution of the retrieved plume. Comparisons with simultaneous and independent aerosol optical depth observations from MODIS (Moderate Resolution Imaging Spectroradiometer), SO2 plume observations from IASI and simulations with the CHIMERE chemistry/transport model show that AEROIASI-H2SO4 correctly identifies the volcanic plume horizontal morphology, thus providing crucial new information towards the study of volcanic emissions, volcanic sulphur cycle in the atmosphere, plume evolution processes, and their impacts. Insights are given on the possible spectroscopic evidence of the presence in the plume of larger-sized particles than previously reported for secondary sulphate aerosols from volcanic eruptions.
Abstract. We developed an optimal-estimation algorithm to simultaneously retrieve, for the first time, co-emitted volcanic gaseous SO2 and sulphate aerosols (SA) from groundbased FTIR observations. These effluents, both linked to magmatic/degassing and subsequent atmospheric evolution processes, have overlapping spectral signatures leading to mutual potential interferences when retrieving one species without considering the other.We show that significant overestimations may be introduced in SO2 retrievals if the radiative impact of co-existent SA is not accounted for, which may have impacted existing SO2 long-term series, e.g. from satellite platform. The method was applied to proximal observations at Masaya volcano, where SO2 and SA concentrations, and SA acidity were retrieved. A gas-to-particle sulphur partitioning of 400 and a strong SA acidity (sulphuric acid concentration: 65 %) where found, consistently with past in-situ observations at this volcano. This method is easily exportable to other volcanoes, to monitor magma extraction processes and the atmospheric sulphur cycle.
Abstract. We developed an optimal-estimation algorithm to simultaneously retrieve, for the first time, coexisting volcanic gaseous SO2 and sulfate aerosols (SA) from ground-based Fourier transform infrared (FTIR) observations. These effluents, both linked to magmatic degassing process and subsequent atmospheric evolution processes, have overlapping spectral signatures leading to mutual potential interferences when retrieving one species without considering the other. We show that significant overestimations may be introduced in SO2 retrievals if the radiative impact of coexistent SA is not accounted for, which may have impacted existing SO2 long-term series, e.g. from satellite platforms. The method was applied to proximal observations at Masaya volcano, where SO2 and SA concentrations, and SA acidity, were retrieved. A gas-to-particle sulfur partitioning of 400 and a strong SA acidity (sulfuric acid concentration: 65 %) were found, consistent with past in situ observations at this volcano. This method is easily exportable to other volcanoes to monitor magma extraction processes and the atmospheric sulfur cycle in the case of ash-free plumes.
Abstract. We developed a new retrieval algorithm based on the Infrared Atmospheric Sounding Interferometer (IASI) observations, called AEROIASI-Sulphates, to measure vertically-resolved sulphate aerosols (SA) extinction and mass concentration profiles, with limited theoretical uncertainties (typically ~25 % total uncertainty for SA mass column estimations). The algorithm, based on a self-adapting Tikhonov-Phillips regularization method, is applied to a medium-sized-intensity eruption of Mount Etna volcano (18 March 2012). Comparisons with simultaneous and independent SO2 plume observations and simulations show that AEROIASI-Sulphates correctly identifies the volcanic plume morphology both horizontally and vertically. This method provided, for the first time, crucial information pieces to describe the gaseous-to-particulate volcanic sulphur mass balance (60 % of the injected sulphur mass is converted to particulate matter, after ~24 hours) and to estimate the regional shortwave direct radiative forcing (a regional forcing of −0.8 W/m2 is exerted in the eastern Mediterranean) for moderate volcanic eruptions.
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