Sub-grid scale representation of halogen chemistry in volcanic plumes based on 1D MOCAGE model simulations

2021 ◽  
Author(s):  
Virginie Marécal ◽  
Ronan Voisin-Pessis ◽  
Tjarda Roberts ◽  
Paul Hamer ◽  
Alessandro Aiuppa ◽  
...  
Keyword(s):  
Transport Model ◽  
Scale Effects ◽  
Regional Scale ◽  
Global Scale ◽  
Horizontal Resolution ◽  
Mt Etna ◽  
Modelling Studies ◽  
1D Model ◽  
High Concentrations ◽  
The Impact

<p>Halogen halides emitted by volcanoes are known to rapidly convert within plumes into BrO while depleting ozone, as clearly shown by observations and models over the past 2 decades (e.g. review by Gutmann et al., 2018). So far, most of the modelling studies have focused on the plume processes occurring in the first few hours after the emission. The only study at the regional scale is that of Jourdain et al. (2016). They assessed the impact of volcanic halogens for a period of strong degassing of the Ambrym volcano, showing in particular its effect on the atmospheric oxidizing capacity and methane lifetime.</p><p>A step further would be to quantify the impact of volcanic halogens at the global scale using global chemistry models. This type of model uses a horizontal resolution (greater than 50 km) that is much coarser than the plume size. This raises the issue of, whether at this resolution, it is possible to represent the chemistry occurring under high concentrations within the plume. To assess this, a sub-grid scale parameterization is proposed. It has been tested in the 1D version of MOCAGE global and regional chemistry transport model for a short eruption of Mt Etna on the 10<sup>th</sup> of May 2008. The results show that while using the subgrid-scale plume parameterization or not does change the timing of when the maximum BrO occurs but does not affect the predicted maximum concentration. The same finding is made when using a range of different settings in the parameterization regarding dilution of the plume with its environment. The 1D model results show a sensitivity of BrO formation to parameters other than the sub-grid scale effects: composition of the plume at the vent, injection height of the emissions, and time of the day when the eruption takes place.</p>

scholarly journals Using the 3D MOCAGE CTM to simulate the chemistry of halogens in the volcanic plume of Etna's eruption in December 2018 at the regional scale

2021 ◽  
Author(s):  
Herizo Narivelo ◽  
Virginie Marécal ◽  
Paul David Hamer ◽  
Luke Surl ◽  
Tjarda Roberts ◽  
...  
Keyword(s):  
Remote Sensing ◽  
Transport Model ◽  
Regional Scale ◽  
Mount Etna ◽  
Volcanic Plume ◽  
Gaseous Species ◽  
Modelling Studies ◽  
Order Of Magnitude ◽  
The Impact ◽  
Halogen Species

<p><span>Volcanoes emit different gaseous species, SO₂ and in particular halogen species especially bromine and chlorine compounds. In general, halogens play an important role in the atmosphere by contributing to ozone depletion in the stratosphere (WMO Ozone assessment, 2018) and by modifying air composition and oxidizing capacity in the troposphere (Von Glasow et al. 2004). The halogen species emitted by volcanoes are halides. The chemical processing occurring within the plume leads to the formation of BrO from HBr following the ‘bromine explosion’ mechanism as evidenced from both observations and modelling (e.g., Bobrowski et al. Nature, 2003; Roberts et al., Chem. Geol. 2009). Oxidized forms of chlorine and bromine are modelled to be formed within the plume due to the heterogenous reaction of HOBr with HCl and HBr, forming BrCl and Br₂ that photolyses and produces Br and Cl radicals. So far, modelling studies were mainly focused on the very local scale and processes occurring within a few hours after eruption.</span></p><p><span>In this study, the objective is to go a step further by analyzing the impact at the regional scale over the Mediterranean basin of a Mt Etna eruption event. For this, we use the MOCAGE model (Guth et al., GMD, 2016), a chemistry transport model run with a resolution of 0.2°x 0.2°, to quantify the impacts of the halogens species emitted by the volcano on the tropospheric composition. We have selected here the case of the eruption of Mount Etna around Christmas 2018 characterised by large amounts of emissions over several days (Calvari et al., remote sensing 2020; Corrdadini et al., remote sensing 2020). The results show that MOCAGE represents rather well the chemistry of the halogens in the volcanic plume because it established theory of plume chemistry. The bromine explosion process takes place on the first day of the eruption and even more strongly the day after, with a rapid increase of the in-plume BrO concentrations and a corresponding strong reduction of ozone and NO2 concentrations.</span></p><p><span>We also compared MOCAGE results with the WRF-CHEM model simulations for the same case study. We note that the tropospheric column of BrO and SO₂ in the two models have the same order of magnitude with more rapid bromine explosion occurring in WRF-CHEM simulations. Finally, we compared the MOCAGE results to tropospheric columns of BrO and SO</span><sub><span>2</span></sub><span> retrieved from TROPOMI spaceborne instrument.</span></p>

scholarly journals Multi-species inversion of CH<sub>4</sub>, CO and H<sub>2</sub> emissions from surface measurements

2009 ◽  
Vol 9 (14) ◽  
pp. 5281-5297 ◽  
Author(s):  
I. Pison ◽  
P. Bousquet ◽  
F. Chevallier ◽  
S. Szopa ◽  
D. Hauglustaine
Keyword(s):  
Transport Model ◽  
Regional Scale ◽  
Surface Concentration ◽  
Temporal Variations ◽  
Global Scale ◽  
Chemical Transport Model ◽  
Methyl Chloroform ◽  
Emission Fluxes ◽  
Surface Measurements ◽  
One Year

Abstract. In order to study the spatial and temporal variations of the emissions of greenhouse gases and of their precursors, we developed a data assimilation system and applied it to infer emissions of CH4, CO and H2 for one year. It is based on an atmospheric chemical transport model and on a simplified scheme for the oxidation chain of hydrocarbons, including methane, formaldehyde, carbon monoxide and molecular hydrogen together with methyl chloroform. The methodology is exposed and a first attempt at evaluating the inverted fluxes is made. Inversions of the emission fluxes of CO, CH4 and H2 and concentrations of HCHO and OH were performed for the year 2004, using surface concentration measurements of CO, CH4, H2 and CH3CCl3 as constraints. Independent data from ship and aircraft measurements and satellite retrievals are used to evaluate the results. The total emitted mass of CO is 30% higher after the inversion, due to increased fluxes by up to 35% in the Northern Hemisphere. The spatial distribution of emissions of CH4 is modified by a decrease of fluxes in boreal areas up to 60%. The comparison between mono- and multi-species inversions shows that the results are close at a global scale but may significantly differ at a regional scale because of the interactions between the various tracers during the inversion.

scholarly journals Influence of aquifer and streambed heterogeneity on the distribution of groundwater discharge

2009 ◽  
Vol 13 (1) ◽  
pp. 69-77 ◽  
Author(s):  
E. Kalbus ◽  
C. Schmidt ◽  
J. W. Molson ◽  
F. Reinstorf ◽  
M. Schirmer
Keyword(s):  
Groundwater Flow ◽  
Transport Model ◽  
Regional Scale ◽  
Base Case ◽  
Case Scenario ◽  
Base Case Scenario ◽  
Heterogeneous Distribution ◽  
Heterogeneous Aquifer ◽  
The Impact ◽  
Low K

Abstract. The spatial distribution of groundwater fluxes through a streambed can be highly variable, most often resulting from a heterogeneous distribution of aquifer and streambed permeabilities along the flow pathways. Using a groundwater flow and heat transport model, we defined four scenarios of aquifer and streambed permeability distributions to simulate and assess the impact of subsurface heterogeneity on the distribution of groundwater fluxes through the streambed: (a) a homogeneous low-K streambed within a heterogeneous aquifer; (b) a heterogeneous streambed within a homogeneous aquifer; (c) a well connected heterogeneous low-K streambed within a heterogeneous aquifer; and (d) a poorly connected heterogeneous low-K streambed within a heterogeneous aquifer. The simulation results were compared with a base case scenario, in which the streambed had the same properties as the aquifer, and with observed data. The results indicated that the aquifer has a stronger influence on the distribution of groundwater fluxes through the streambed than the streambed itself. However, a homogeneous low-K streambed, a case often implemented in regional-scale groundwater flow models, resulted in a strong homogenization of fluxes, which may have important implications for the estimation of peak mass flows. The flux distributions simulated with heterogeneous low-K streambeds were similar to the flux distributions of the base case scenario, despite the lower permeability. The representation of heterogeneous distributions of aquifer and streambed properties in the model has been proven to be beneficial for the accuracy of flow simulations.

scholarly journals Impact of transport model errors on the global and regional methane emissions estimated by inverse modelling

2013 ◽  
Vol 13 (19) ◽  
pp. 9917-9937 ◽  
Author(s):  
R. Locatelli ◽  
P. Bousquet ◽  
F. Chevallier ◽  
A. Fortems-Cheney ◽  
S. Szopa ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Initial Conditions ◽  
Spatial Scales ◽  
Global Scale ◽  
Methane Emissions ◽  
Inverse Modelling ◽  
Model Errors ◽  
Inverse Systems ◽  
The Impact

Abstract. A modelling experiment has been conceived to assess the impact of transport model errors on methane emissions estimated in an atmospheric inversion system. Synthetic methane observations, obtained from 10 different model outputs from the international TransCom-CH4 model inter-comparison exercise, are combined with a prior scenario of methane emissions and sinks, and integrated into the three-component PYVAR-LMDZ-SACS (PYthon VARiational-Laboratoire de Météorologie Dynamique model with Zooming capability-Simplified Atmospheric Chemistry System) inversion system to produce 10 different methane emission estimates at the global scale for the year 2005. The same methane sinks, emissions and initial conditions have been applied to produce the 10 synthetic observation datasets. The same inversion set-up (statistical errors, prior emissions, inverse procedure) is then applied to derive flux estimates by inverse modelling. Consequently, only differences in the modelling of atmospheric transport may cause differences in the estimated fluxes. In our framework, we show that transport model errors lead to a discrepancy of 27 Tg yr−1 at the global scale, representing 5% of total methane emissions. At continental and annual scales, transport model errors are proportionally larger than at the global scale, with errors ranging from 36 Tg yr−1 in North America to 7 Tg yr−1 in Boreal Eurasia (from 23 to 48%, respectively). At the model grid-scale, the spread of inverse estimates can reach 150% of the prior flux. Therefore, transport model errors contribute significantly to overall uncertainties in emission estimates by inverse modelling, especially when small spatial scales are examined. Sensitivity tests have been carried out to estimate the impact of the measurement network and the advantage of higher horizontal resolution in transport models. The large differences found between methane flux estimates inferred in these different configurations highly question the consistency of transport model errors in current inverse systems. Future inversions should include more accurately prescribed observation covariances matrices in order to limit the impact of transport model errors on estimated methane fluxes.

scholarly journals The dispersion characteristics of air pollution from the world's megacities

2013 ◽  
Vol 13 (19) ◽  
pp. 9975-9996 ◽  
Author(s):  
M. Cassiani ◽  
A. Stohl ◽  
S. Eckhardt
Keyword(s):  
Human Population ◽  
Scale Effects ◽  
Lower Troposphere ◽  
Global Scale ◽  
The Arctic ◽  
Particle Model ◽  
Modeling Framework ◽  
Local Conditions ◽  
The Impact ◽  
The City

Abstract. Megacities are extreme examples of the continuously growing urbanization of the human population that pose (new) challenges to the environment and human health at a local scale. However, because of their size megacities also have larger-scale effects, and more research is needed to quantify their regional- and global-scale impacts. We performed a study of the characteristics of pollution plumes dispersing from a group of 36 of the world's megacities using the Lagrangian particle model FLEXPART and focusing on black carbon (BC) emissions during the years 2003–2005. BC was selected since it is representative of combustion-related emissions and has a significant role as a short-lived climate forcer. Based on the BC emissions two artificial tracers were modeled: a purely passive tracer and one subject to wet and dry deposition more closely resembling the behavior of a true aerosol. These tracers allowed us to investigate the role of deposition processes in determining the impact of megacities' pollutant plumes. The particles composing the plumes have been sampled in space and time. The time sampling allowed us to investigate the evolution of the plume from its release up to 48 days after emission and to generalize our results for any substance decaying with a timescale sufficiently shorter than the time window of 48 days. The physical characteristics of the time-averaged plume have been investigated, and this showed that, although local conditions are important, overall a city's latitude is the main factor influencing both the local and the regional-to-global dispersion of its pollution. We also repeated the calculations of some of the regional-pollution-potential metrics previously proposed by Lawrence et al. (2007), thus extending their results to a depositing scalar and retaining the evolution in time for all the plumes. Our results agreed well with their previous results despite being obtained using a totally different modeling framework. For the environmental impact on a global scale we focused on the export of mass from the megacities to the sensitive polar regions. We found that the sole city of Saint Petersburg contributes more to the lower-troposphere pollution and deposition in the Arctic than the whole ensemble of Asian megacities. In general this study showed that the pollution of urban origin in the lower troposphere of the Arctic is mainly generated by northern European sources. We also found that the deposition of the modeled artificial BC aerosol in the Antarctic due to megacities is comparable to the emissions of BC generated by local shipping activities. Finally multiplying population and ground level concentration maps, we found that the exposure of human population to megacity pollution occurs mainly inside the city boundaries, and this is especially true if deposition is accounted for. However, some exceptions exist (Beijing, Tianjin, Karachi) where the impact on population outside the city boundary is larger than that inside the city boundary.

scholarly journals Clouds, photolysis and regional tropospheric ozone budgets

2009 ◽  
Vol 9 (3) ◽  
pp. 13889-13916 ◽  
Author(s):  
A. Voulgarakis ◽  
O. Wild ◽  
N. H. Savage ◽  
G. D. Carver ◽  
J. A. Pyle
Keyword(s):  
Tropospheric Ozone ◽  
Large Scale ◽  
Transport Model ◽  
Regional Scale ◽  
Three Dimensional ◽  
Global Scale ◽  
Chemical Production ◽  
Chemical Transport Model ◽  
Photolysis Rates ◽  
Boundary Layer Ozone

Abstract. We use a three-dimensional chemical transport model to examine the shortwave radiative effects of clouds on the tropospheric ozone budget. In addition to looking at changes in global concentrations as previous studies have done, we examine changes in ozone chemical production and loss caused by clouds and how these vary in different parts of the troposphere. On a global scale, we find that clouds have a modest effect on ozone chemistry, but on a regional scale their role is much more significant, with the size of the response dependent on the region. The largest averaged changes in chemical budgets (±10–14%) are found in the marine troposphere, where cloud optical depths are high. We demonstrate that cloud effects are small on average in the middle troposphere because this is a transition region between reduction and enhancement in photolysis rates. We show that increases in boundary layer ozone due to clouds are driven by large-scale changes in downward ozone transport from higher in the troposphere rather than by decreases in in-situ ozone chemical loss rates. Increases in upper tropospheric ozone are caused by higher production rates due to backscattering of radiation and consequent increases in photolysis rates, mainly J(NO2). The global radiative effect of clouds on isoprene is stronger than on ozone. Tropospheric isoprene lifetime increases by 7% when taking clouds into account. We compare the importance of clouds in contributing to uncertainties in the global ozone budget with the role of other radiatively-important factors. The budget is most sensitive to the overhead ozone column, while surface albedo and clouds have smaller effects. However, uncertainty in representing the spatial distribution of clouds may lead to a large sensitivity on regional scales.

scholarly journals Geo-Climatic Changes and Apomixis as Major Drivers of Diversification in the Mediterranean Sea Lavenders (Limonium Mill.)

2021 ◽  
Vol 11 ◽  
Author(s):  
Konstantina Koutroumpa ◽  
Ben H. Warren ◽  
Spyros Theodoridis ◽  
Mario Coiro ◽  
Maria M. Romeiras ◽  
...  
Keyword(s):  
Species Diversity ◽  
Regional Scale ◽  
Mediterranean Area ◽  
Global Scale ◽  
Significant Shift ◽  
Extrinsic Factors ◽  
Diversification Rates ◽  
The Mediterranean ◽  
The Impact

The Mediterranean realm, comprising the Mediterranean and Macaronesian regions, has long been recognized as one of the world’s biodiversity hotspots, owing to its remarkable species richness and endemism. Several hypotheses on biotic and abiotic drivers of species diversification in the region have been often proposed but rarely tested in an explicit phylogenetic framework. Here, we investigate the impact of both species-intrinsic and -extrinsic factors on diversification in the species-rich, cosmopolitan Limonium, an angiosperm genus with center of diversity in the Mediterranean. First, we infer and time-calibrate the largest Limonium phylogeny to date. We then estimate ancestral ranges and diversification dynamics at both global and regional scales. At the global scale, we test whether the identified shifts in diversification rates are linked to specific geological and/or climatic events in the Mediterranean area and/or asexual reproduction (apomixis). Our results support a late Paleogene origin in the proto-Mediterranean area for Limonium, followed by extensive in situ diversification in the Mediterranean region during the late Miocene, Pliocene, and Pleistocene. We found significant increases of diversification rates in the “Mediterranean lineage” associated with the Messinian Salinity Crisis, onset of Mediterranean climate, Plio-Pleistocene sea-level fluctuations, and apomixis. Additionally, the Euro-Mediterranean area acted as the major source of species dispersals to the surrounding areas. At the regional scale, we infer the biogeographic origins of insular endemics in the oceanic archipelagos of Macaronesia, and test whether woodiness in the Canarian Nobiles clade is a derived trait linked to insular life and a biotic driver of diversification. We find that Limonium species diversity on the Canary Islands and Cape Verde archipelagos is the product of multiple colonization events followed by in situ diversification, and that woodiness of the Canarian endemics is indeed a derived trait but is not associated with a significant shift to higher diversification rates. Our study expands knowledge on how the interaction between abiotic and biotic drivers shape the uneven distribution of species diversity across taxonomic and geographical scales.

scholarly journals Impact of transport model errors on the global and regional methane emissions estimated by inverse modelling

2013 ◽  
Vol 13 (4) ◽  
pp. 10961-11021
Author(s):  
R. Locatelli ◽  
P. Bousquet ◽  
F. Chevallier ◽  
A. Fortems-Cheney ◽  
S. Szopa ◽  
...  
Keyword(s):  
Transport Model ◽  
Atmospheric Transport ◽  
Spatial Scales ◽  
Global Scale ◽  
Methane Emissions ◽  
Inverse Modelling ◽  
Model Errors ◽  
Inverse Systems ◽  
Set Up ◽  
The Impact

Abstract. A modelling experiment has been conceived to assess the impact of transport model errors on the methane emissions estimated by an atmospheric inversion system. Synthetic methane observations, given by 10 different model outputs from the international TransCom-CH4 model exercise, are combined with a prior scenario of methane emissions and sinks, and integrated into the PYVAR-LMDZ-SACS inverse system to produce 10 different methane emission estimates at the global scale for the year 2005. The same set-up has been used to produce the synthetic observations and to compute flux estimates by inverse modelling, which means that only differences in the modelling of atmospheric transport may cause differences in the estimated fluxes. In our framework, we show that transport model errors lead to a discrepancy of 27 Tg CH4 per year at the global scale, representing 5% of the total methane emissions. At continental and yearly scales, transport model errors have bigger impacts depending on the region, ranging from 36 Tg CH4 in north America to 7 Tg CH4 in Boreal Eurasian (from 23% to 48%). At the model gridbox scale, the spread of inverse estimates can even reach 150% of the prior flux. Thus, transport model errors contribute to significant uncertainties on the methane estimates by inverse modelling, especially when small spatial scales are invoked. Sensitivity tests have been carried out to estimate the impact of the measurement network and the advantage of higher resolution models. The analysis of methane estimated fluxes in these different configurations questions the consistency of transport model errors in current inverse systems. For future methane inversions, an improvement in the modelling of the atmospheric transport would make the estimations more accurate. Likewise, errors of the observation covariance matrix should be more consistently prescribed in future inversions in order to limit the impact of transport model errors on estimated methane fluxes.

scholarly journals Assimilation of IASI satellite CO fields into a global chemistry transport model for validation against aircraft measurements

2012 ◽  
Vol 12 (10) ◽  
pp. 4493-4512 ◽  
Author(s):  
A. Klonecki ◽  
M. Pommier ◽  
C. Clerbaux ◽  
G. Ancellet ◽  
J.-P. Cammas ◽  
...  
Keyword(s):  
Transport Model ◽  
Source Region ◽  
Specific Treatment ◽  
Arctic Region ◽  
The Arctic ◽  
Chemistry Transport Model ◽  
Mixing Ratios ◽  
High Concentrations ◽  
The Impact

Abstract. This work evaluates the IASI CO product against independent in-situ aircraft data from the MOZAIC program and the POLARCAT aircraft campaign. The validation is carried out by analysing the impact of assimilation of eight months of IASI CO columns retrieved for the period of May to December 2008 into the global chemistry transport model LMDz-INCA. A modelling system based on a sub-optimal Kalman filter was developed and a specific treatment that takes into account the representativeness of observations at the scale of the model grid is applied to the IASI CO columns and associated errors before their assimilation in the model. Comparisons of the assimilated CO profiles with in situ CO measurements indicate that the assimilation leads to a considerable improvement of the model simulations in the middle troposphere as compared with a control run with no assimilation. Model biases in the simulation of background values are reduced and improvement in the simulation of very high concentrations is observed. The improvement is due to the transport by the model of the information present in the IASI CO retrievals. Our analysis also shows the impact of assimilation of CO on the representation of transport into the Arctic region during the POLARCAT summer campaign. A considerable increase in CO mixing ratios over the Asian source region was observed when assimilation was used leading to much higher values of CO during the cross-pole transport episode. These higher values are in good agreement with data from the POLARCAT flights that sampled this plume.

scholarly journals Modelling of nitrate and ammonium-containing aerosols in presence of sea salt

2006 ◽  
Vol 6 (12) ◽  
pp. 4809-4821 ◽  
Author(s):  
G. Myhre ◽  
A. Grini ◽  
S. Metzger
Keyword(s):  
Aerosol Optical Depth ◽  
Optical Depth ◽  
Radiative Forcing ◽  
Transport Model ◽  
Meteorological Condition ◽  
Global Scale ◽  
Sea Salt ◽  
Aerosol Composition ◽  
Fine Mode ◽  
High Concentrations

Abstract. A thermodynamical model for treatment of gas/aerosol partitioning of semi volatile inorganic aerosols has been implemented in a global chemistry and aerosol transport model (Oslo CTM2). The sulphur cycle and sea salt particles have been implemented earlier in the Oslo CTM2 and the focus of this study is on nitrate partitioning to the aerosol phase and if particulate nitrate is expected to form in fine or coarse mode aerosols. Modelling of the formation of fine mode nitrate particles is complicated since it depends on other aerosol components and aerosol precursors as well as meteorological condition. The surface concentrations from the model are compared to observed surface concentrations at around 20 sites around Europe for nitrate and ammonium. The agreement for nitrate is good but the modelled values are somewhat underestimated compared to observations at high concentrations, whereas for ammonium the agreement is very good. However, we underscore that such a comparison is not of large importance for the aerosol optical depth of particulate nitrate since the vertical profile of aerosol components and their precursors are so important. Fine mode nitrate formation depends on vertical profiles of both ammonia/ammonium and sulphate. The model results show that fine mode particulate nitrate play a non-negligible role in the total aerosol composition in certain industrialized regions and therefore have a significant local radiative forcing. On a global scale the aerosol optical depth of fine mode nitrate is relatively small due to limited availability of ammonia and loss to larger sea salt particles. Inclusion of sea salt in the calculations reduces the aerosol optical depth and burden of fine mode nitrate by 25% on a global scale but with large regional variations.

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