scholarly journals Modeling study of the impact of SO<sub>2</sub> volcanic passive emissions on the tropospheric sulfur budget

2021 ◽  
Vol 21 (14) ◽  
pp. 11379-11404
Author(s):  
Claire Lamotte ◽  
Jonathan Guth ◽  
Virginie Marécal ◽  
Martin Cussac ◽  
Paul David Hamer ◽  
...  
Keyword(s):  
Transport Model ◽  
Sensitivity Study ◽  
Accurate Information ◽  
Volcanic Emissions ◽  
Ozone Monitoring Instrument ◽  
So2 Emissions ◽  
Transport Models ◽  
Sulfur Species ◽  
The Impact ◽  
Sulfur Emissions

Abstract. Well constrained volcanic emissions inventories in chemistry transport models are necessary to study the impacts induced by these sources on the tropospheric sulfur composition and on sulfur species concentrations and depositions at the surface. In this paper, the changes induced by the update of the volcanic sulfur emissions inventory are studied using the global chemistry transport model MOCAGE (MOdèle de Chimie Atmosphérique à Grande Échelle). Unlike the previous inventory (Andres and Kasgnoc, 1998), the updated one (Carn et al., 2016, 2017) uses more accurate information and includes contributions from both passive degassing and eruptive emissions. Eruptions are provided as daily total amounts of sulfur dioxide (SO2) emitted by volcanoes in the Carn et al. (2016, 2017) inventories, and degassing emissions are provided as annual averages with the related mean annual uncertainties of those emissions by volcano. Information on plume altitudes is also available and has been used in the model. We chose to analyze the year 2013, for which only a negligible amount of eruptive volcanic SO2 emissions is reported, allowing us to focus the study on the impact of passive degassing emissions on the tropospheric sulfur budget. An evaluation against the Ozone Monitoring Instrument (OMI) SO2 total column and MODIS (Moderate-Resolution Imaging Spectroradiometer) aerosol optical depth (AOD) observations shows the improvements of the model results with the updated inventory. Because the global volcanic SO2 flux changes from 13 Tg yr−1 in Andres and Kasgnoc (1998) to 23.6 Tg yr−1 in Carn et al. (2016, 2017), significant differences appear in the global sulfur budget, mainly in the free troposphere and in the tropics. Even though volcanic SO2 emissions represent 15 % of the total annual sulfur emissions, the volcanic contribution to the tropospheric sulfate aerosol burden is 25 %, which is due to the higher altitude of emissions from volcanoes. Moreover, a sensitivity study on passive degassing emissions, using the annual uncertainties of emissions per volcano, also confirmed the nonlinear link between tropospheric sulfur species content with respect to volcanic SO2 emissions. This study highlights the need for accurate estimates of volcanic sources in chemistry transport models in order to properly simulate tropospheric sulfur species.

scholarly journals Modeling study of the impact of SO<sub>2</sub> volcanic passive emissions on the tropospheric sulfur budget

2020 ◽  
Author(s):  
Claire Lamotte ◽  
Jonathan Guth ◽  
Virginie Marécal ◽  
Martin Cussac
Keyword(s):  
Transport Model ◽  
Sensitivity Study ◽  
Volcanic Emissions ◽  
So2 Emissions ◽  
Sulfur Species ◽  
Emissions Inventory ◽  
Modis Aod ◽  
Non Linear ◽  
The Impact ◽  
Sulfur Emissions

Abstract. The contribution of volcanic emissions is argued as non-linear on the sulfur species burden. Thus, well constraining volcanic emissions inventories is necessary to better study the impacts induced by these pollution sources on the troposheric sulfur composition, as well as on sulfur species concentrations and depositions at the global surface. In this paper, the changes induced by the update of the volcanic sulfur emissions inventory on the global chemistry-transport model MOCAGE (MOdèle de Chimie Atmosphérique à Grande Échelle) are studied. Unlike the current inventory [Andres and Kasgnoc (1998)], the new inventory [Carn et al. (2016, 2017)] includes contributions from both passive degassing and eruptive emissions with more accu- rate information. Eruptions are provided as daily total amounts of sulfur dioxide (SO2) emitted by volcanoes, while degassing are provided as annual averages with annual uncertainties by volcanoes. Information on plumes altitudes is also available and has been used in the model. The choice is made to look at the year 2013, when a neglieable amount of eruptive volcanic SO2 emissions is referenced, allowing us to focus the study on the impact of passive degassing emissions on the tropospheric sulfur budget. A validation against GOME-2 SO2 total column and MODIS AOD observations shows the improvements of the model results with the new inventory. Because the global volcanic SO2 flux changes from 13 Tg.yr−1 in the current inventory to 23.6 Tg.yr−1 in the new inventory, the updated inventory shows significant differences in the global sulfur budget, mainly in the free troposphere and in the tropics. Even though volcanic SO2 emissions represent 15 % of the total annual sulfur emissions, the volcanic contribution to the tropospheric sulfate aerosol burden is 27 %. Moreover, a sensitivity study on passive degassing emissions, using the annual uncertainties of emissions per volcanoes, also confirmed the non-linear link between tropospheric sulfur species and volcanic emissions. This study highlights the necessity of using accurate estimates of volcanic sources in chemistry-transport models in order to properly simulate tropospheric sulfur species.

scholarly journals Model – TCCON comparisons of column-averaged methane with a focus on the stratosphere

2016 ◽  
Author(s):  
Andreas Ostler ◽  
Ralf Sussmann ◽  
Prabir K. Patra ◽  
Sander Houweling ◽  
Marko De Bruine ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Meteorological Data ◽  
Michelson Interferometer ◽  
Total Carbon ◽  
Data Sets ◽  
Transport Models ◽  
Improved Model ◽  
The Impact ◽  
Chemistry Experiment

Abstract. The distribution of methane (CH4) in the stratosphere can be a major driver of spatial variability in the dry-air column-averaged CH4 mixing ratio (XCH4), which is being measured increasingly for the assessment of CH4 surface emissions. Chemistry-transport models (CTMs) therefore need to simulate the tropospheric and stratospheric fractional columns of XCH4 accurately for estimating surface emissions from XCH4. Simulations from three CTMs are tested against XCH4 observations from the Total Carbon Column Network (TCCON). We analyze how the model-TCCON agreement in XCH4 depends on the model representation of stratospheric CH4 distributions. Model equivalents of TCCON XCH4 are computed with stratospheric CH4 fields from both the model simulations and from satellite-based CH4 distributions from MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) and MIPAS CH4 fields adjusted to ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations. In comparison to simulated model fields we find an improved model-TCCON XCH4 agreement for all models with MIPAS-based stratospheric CH4 fields. For the Atmospheric Chemistry Transport Model (ACTM) the average XCH4 bias is significantly reduced from 38.1 ppb to 13.7 ppb, whereas small improvements are found for the models TM5 (Transport Model, version 5; from 8.7 ppb to 4.3 ppb), and LMDz (Laboratoire de Météorologie Dynamique model with Zooming capability; from 6.8 ppb to 4.3 ppb), respectively. MIPAS stratospheric CH4 fields adjusted to ACE-FTS reduce the average XCH4 bias for ACTM (3.3 ppb), but increase the average XCH4 bias for TM5 (10.8 ppb) and LMDz (20.0 ppb). These findings imply that the range of satellite-based stratospheric CH4 is insufficient to resolve a possible stratospheric contribution to differences in total column CH4 between TCCON and TM5 or LMDz. Applying transport diagnostics to the models indicates that model-to-model differences in the simulation of stratospheric transport, notably the age of stratospheric air, can largely explain the inter-model spread in stratospheric CH4 and, hence, its contribution to XCH4. This implies that there is a need to better understand the impact of individual model transport components (e.g., physical parameterization, meteorological data sets, model horizontal/vertical resolution) on modeled stratospheric CH4.

scholarly journals The importance of transport model uncertainties for the estimation of CO<sub>2</sub> sources and sinks using satellite measurements

2010 ◽  
Vol 10 (20) ◽  
pp. 9981-9992 ◽  
Author(s):  
S. Houweling ◽  
I. Aben ◽  
F.-M. Breon ◽  
F. Chevallier ◽  
N. Deutscher ◽  
...  
Keyword(s):  
Transport Model ◽  
Atmospheric Transport ◽  
A Priori ◽  
Model Errors ◽  
Tracer Transport ◽  
Satellite Measurements ◽  
Transport Models ◽  
Sources And Sinks ◽  
The Impact ◽  
Ppm Level

Abstract. This study presents a synthetic model intercomparison to investigate the importance of transport model errors for estimating the sources and sinks of CO2 using satellite measurements. The experiments were designed for testing the potential performance of the proposed CO2 lidar A-SCOPE, but also apply to other space borne missions that monitor total column CO2. The participating transport models IFS, LMDZ, TM3, and TM5 were run in forward and inverse mode using common a priori CO2 fluxes and initial concentrations. Forward simulations of column averaged CO2 (xCO2) mixing ratios vary between the models by σ=0.5 ppm over the continents and σ=0.27 ppm over the oceans. Despite the fact that the models agree on average on the sub-ppm level, these modest differences nevertheless lead to significant discrepancies in the inverted fluxes of 0.1 PgC/yr per 106 km2 over land and 0.03 PgC/yr per 106 km2 over the ocean. These transport model induced flux uncertainties exceed the target requirement that was formulated for the A-SCOPE mission of 0.02 PgC/yr per 106 km2, and could also limit the overall performance of other CO2 missions such as GOSAT. A variable, but overall encouraging agreement is found in comparison with FTS measurements at Park Falls, Darwin, Spitsbergen, and Bremen, although systematic differences are found exceeding the 0.5 ppm level. Because of this, our estimate of the impact of transport model uncerainty is likely to be conservative. It is concluded that to make use of the remote sensing technique for quantifying the sources and sinks of CO2 not only requires highly accurate satellite instruments, but also puts stringent requirements on the performance of atmospheric transport models. Improving the accuracy of these models should receive high priority, which calls for a closer collaboration between experts in atmospheric dynamics and tracer transport.

scholarly journals The constraint of CO<sub>2</sub> measurements made onboard passenger aircraft on surface-atmosphere fluxes: the impact of transport model errors in vertical mixing

2016 ◽  
Author(s):  
Shreeya Verma ◽  
Julia Marshall ◽  
Christoph Gerbig ◽  
Christian Roedenbeck ◽  
Kai Uwe Totsche
Keyword(s):  
Transport Model ◽  
Atmospheric Transport ◽  
Vertical Mixing ◽  
Synthetic Data ◽  
Vertical Profiles ◽  
Model Errors ◽  
Transport Models ◽  
Boundary Layer Height ◽  
Temporal Sampling ◽  
The Impact

Abstract. Inaccurate representation of atmospheric processes by transport models is a dominant source of uncertainty in inverse analyses and can lead to large discrepancies in the retrieved flux estimates. We investigate the impact of uncertainties in vertical transport as simulated by atmospheric transport models on fluxes retrieved using vertical profiles from aircraft as an observational constraint. Our numerical experiments are based on synthetic data with realistic spatial and temporal sampling of aircraft measurements. The impact of such uncertainties on the flux retrieved using the ground-based network with those retrieved using the aircraft profiles are compared. We find that the posterior flux retrieved using aircraft profiles is less susceptible to errors in boundary layer height as compared to the ground- based network. This highlights the benefit of utilizing atmospheric observations made onboard aircraft over surface measurements for flux estimation using inverse methods. We further use synthetic vertical profiles of CO2 in an inversion to estimate the potential of these measurements, which will be made available through the IAGOS (In-Service Aircraft for a Global Observing System) project in future, in constraining the regional carbon budget. Our results show that the regions tropical Africa and temperate Eurasia, that are under constrained by the existing surface based network, will benefit the most from these measurements, the reduction of posterior flux uncertainty being about 7 to 10 %.

scholarly journals The impact of shipping emissions on air pollution in the greater North Sea region – Part 2: Scenarios for 2030

2016 ◽  
Vol 16 (2) ◽  
pp. 759-776 ◽  
Author(s):  
V. Matthias ◽  
A. Aulinger ◽  
A. Backes ◽  
J. Bieser ◽  
B. Geyer ◽  
...  
Keyword(s):  
North Sea ◽  
Transport Model ◽  
So2 Emissions ◽  
Chemistry Transport Model ◽  
The North ◽  
International Regulations ◽  
The North Sea ◽  
Sea Area ◽  
The Impact ◽  
Ship Fuels

Abstract. Scenarios for future shipping emissions in the North Sea have been developed in the framework of the Clean North Sea Shipping project. The effects of changing NOx and SO2 emissions were investigated with the CMAQ chemistry transport model for the year 2030 in the North Sea area. It has been found that, compared to today, the contribution of shipping to the NO2 and O3 concentrations will increase due to the expected enhanced traffic by more than 20 and 5 %, respectively, by 2030 if no regulation for further emission reductions is implemented in the North Sea area. PM2.5 will decrease slightly because the sulfur contents in ship fuels will be reduced as international regulations foresee. The effects differ largely between regions, seasons and date of the implementation of stricter regulations for NOx emissions from newly built ships.

scholarly journals On the ability of chemical transport models to simulate the vertical structure of the N<sub>2</sub>O, NO<sub>2</sub> and HNO<sub>3</sub> species in the mid-latitude stratosphere

2005 ◽  
Vol 5 (6) ◽  
pp. 12373-12401
Author(s):  
G. Berthet ◽  
N. Huret ◽  
F. Lefèvre ◽  
G. Moreau ◽  
C. Robert ◽  
...  
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Transport Models ◽  
One Dimensional ◽  
Chemical Transport Models ◽  
Dimensional Version ◽  
The Impact

Abstract. In this paper we study the impact of the modelling of N2O on the simulation of NO2 and HNO3 by comparing in situ vertical profiles measured at mid-latitudes with the results of the Reprobus 3-D CTM (Three-dimensional Chemical Transport Model) computed with the kinetic parameters from the JPL recommendation in 2002. The analysis of the measured in situ profile of N2O shows particular features indicating different air mass origins. The measured N2O, NO2 and HNO3 profiles are not satisfyingly reproduced by the CTM when computed using the current 6-hourly ECMWF operational analysis. Improving the simulation of N2O transport allows us to calculate quantities of NO2 and HNO3 in reasonable agreement with observations. This is achieved using 3-hourly winds obtained from ECMWF forecasts. The best agreement is obtained by constraining a one-dimensional version of the model with the observed N2O. This study shows that modelling the NOy partitioning with better accuracy relies at least on a correct simulation of N2O and thus of total NOy.

scholarly journals New strategies for vertical transport in chemistry transport models: application to the case of the Mount Etna eruption on 18 March 2012 with CHIMERE v2017r4

2020 ◽  
Vol 13 (11) ◽  
pp. 5707-5723
Author(s):  
Mathieu Lachatre ◽  
Sylvain Mailler ◽  
Laurent Menut ◽  
Solène Turquety ◽  
Pasquale Sellitto ◽  
...  
Keyword(s):  
Transport Model ◽  
Vertical Direction ◽  
Vertical Wind ◽  
Mount Etna ◽  
Plume Dispersion ◽  
Vertical Resolution ◽  
Ozone Monitoring Instrument ◽  
Vertical Diffusion ◽  
Transport Models ◽  
Brute Force Approach

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).

scholarly journals Combined assimilation of IASI and MLS observations to constrain tropospheric and stratospheric ozone in a global chemical transport model

2013 ◽  
Vol 13 (8) ◽  
pp. 21455-21505
Author(s):  
E. Emili ◽  
B. Barret ◽  
S. Massart ◽  
E. Le Flochmoen ◽  
A. Piacentini ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Chemical Transport ◽  
Free Troposphere ◽  
Chemical Transport Model ◽  
Ozone Monitoring Instrument ◽  
Global Chemical Transport Model ◽  
The Impact

Abstract. Accurate and temporally resolved fields of free-troposphere ozone are of major importance to quantify the intercontinental transport of pollution and the ozone radiative forcing. In this study we examine the impact of assimilating ozone observations from the Microwave Limb Sounder (MLS) and the Infrared Atmospheric Sounding Interferometer (IASI) in a global chemical transport model (MOdèle de Chimie Atmosphérique à Grande Échelle, MOCAGE). The assimilation of the two instruments is performed by means of a variational algorithm (4-D-VAR) and allows to constrain stratospheric and tropospheric ozone simultaneously. The analysis is first computed for the months of August and November 2008 and validated against ozone-sondes measurements to verify the presence of observations and model biases. It is found that the IASI Tropospheric Ozone Column (TOC, 1000–225 hPa) should be bias-corrected prior to assimilation and MLS lowermost level (215 hPa) excluded from the analysis. Furthermore, a longer analysis of 6 months (July–August 2008) showed that the combined assimilation of MLS and IASI is able to globally reduce the uncertainty (Root Mean Square Error, RMSE) of the modeled ozone columns from 30% to 15% in the Upper-Troposphere/Lower-Stratosphere (UTLS, 70–225 hPa) and from 25% to 20% in the free troposphere. The positive effect of assimilating IASI tropospheric observations is very significant at low latitudes (30° S–30° N), whereas it is not demonstrated at higher latitudes. Results are confirmed by a comparison with additional ozone datasets like the Measurements of OZone and wAter vapour by aIrbus in-service airCraft (MOZAIC) data, the Ozone Monitoring Instrument (OMI) total ozone columns and several high-altitude surface measurements. Finally, the analysis is found to be little sensitive to the assimilation parameters and the model chemical scheme, due to the high frequency of satellite observations compared to the average life-time of free-troposphere/low-stratosphere ozone.

scholarly journals OMI NO<sub>2</sub> column densities over North American urban cities: the effect of satellite footprint resolution

2016 ◽  
Vol 9 (3) ◽  
pp. 1111-1123 ◽  
Author(s):  
Hyun Cheol Kim ◽  
Pius Lee ◽  
Laura Judd ◽  
Li Pan ◽  
Barry Lefer
Keyword(s):  
Spatial Information ◽  
Transport Model ◽  
Model Simulation ◽  
Nox Emission ◽  
Scale Model ◽  
Fine Scale ◽  
Ozone Monitoring Instrument ◽  
Vertical Column ◽  
The Impact ◽  
Emission Policy

Abstract. Nitrogen dioxide vertical column density (NO2 VCD) measurements via satellite are compared with a fine-scale regional chemistry transport model, using a new approach that considers varying satellite footprint sizes. Space-borne NO2 VCD measurement has been used as a proxy for surface nitrogen oxide (NOx) emission, especially for anthropogenic urban emission, so accurate comparison of satellite and modeled NO2 VCD is important in determining the future direction of NOx emission policy. The NASA Ozone Monitoring Instrument (OMI) NO2 VCD measurements, retrieved by the Royal Netherlands Meteorological Institute (KNMI), are compared with a 12 km Community Multi-scale Air Quality (CMAQ) simulation from the National Oceanic and Atmospheric Administration. We found that the OMI footprint-pixel sizes are too coarse to resolve urban NO2 plumes, resulting in a possible underestimation in the urban core and overestimation outside. In order to quantify this effect of resolution geometry, we have made two estimates. First, we constructed pseudo-OMI data using fine-scale outputs of the model simulation. Assuming the fine-scale model output is a true measurement, we then collected real OMI footprint coverages and performed conservative spatial regridding to generate a set of fake OMI pixels out of fine-scale model outputs. When compared to the original data, the pseudo-OMI data clearly showed smoothed signals over urban locations, resulting in roughly 20–30 % underestimation over major cities. Second, we further conducted conservative downscaling of OMI NO2 VCDs using spatial information from the fine-scale model to adjust the spatial distribution, and also applied averaging kernel (AK) information to adjust the vertical structure. Four-way comparisons were conducted between OMI with and without downscaling and CMAQ with and without AK information. Results show that OMI and CMAQ NO2 VCDs show the best agreement when both downscaling and AK methods are applied, with the correlation coefficient R = 0.89. This study suggests that satellite footprint sizes might have a considerable effect on the measurement of fine-scale urban NO2 plumes. The impact of satellite footprint resolution should be considered when using satellite observations in emission policy making, and the new downscaling approach can provide a reference uncertainty for the use of satellite NO2 measurements over most cities.

scholarly journals A model study of the pollution effects of the first 3 months of the Holuhraun volcanic fissure: comparison with observations and air pollution effects

2016 ◽  
Vol 16 (15) ◽  
pp. 9745-9760 ◽  
Author(s):  
Birthe Marie Steensen ◽  
Michael Schulz ◽  
Nicolas Theys ◽  
Hilde Fagerli
Keyword(s):  
European Union ◽  
Extreme Values ◽  
Model Simulation ◽  
Volcanic Emissions ◽  
Ozone Monitoring Instrument ◽  
So2 Emissions ◽  
Pollution Effects ◽  
The North ◽  
Model Study ◽  
European Union Countries

Abstract. The volcanic fissure at Holuhraun, Iceland started at the end of August 2014 and continued for 6 months to the end of February 2015, with an extensive lava flow onto the Holuhraun plain. This event was associated with large SO2 emissions, amounting up to approximately 4.5 times the daily anthropogenic SO2 emitted from the 28 European Union countries, Norway, Switzerland and Iceland. In this paper we present results from EMEP/MSC-W model simulations to which we added 750 kg s−1 SO2 emissions at the Holuhraun plain from September to November (SON), testing three different emission heights. The three simulated SO2 concentrations, weighted with the OMI (Ozone Monitoring Instrument) satellite averaging kernel, are found to be within 30 % of the satellite-observed SO2 column burden. Constraining the SO2 column burden with the satellite data while using the kernel along with the three simulated height distributions of SO2, we estimate that the median of the daily burdens may have been between 13 and 40 kt in the North Atlantic area under investigation. We suggest this to be the uncertainty in the satellite-derived burdens of SO2, mainly due to the unknown vertical distribution of SO2. Surface observations in Europe outside Iceland showed concentration increases up to > 500 µg m−3 SO2 from volcanic plumes passing. Three well identified episodes, where the plume crossed several countries, are compared in detail to surface measurements. For all events, the general timing of the observed concentration peaks compared quite well to the model results. The overall changes to the European SO2 budget due to the volcanic fissure are estimated. Three-monthly wet deposition (SON) of SOx in the 28 European Union countries, Norway and Switzerland is found to be more than 30 % higher in the model simulation with Holuhraun emissions compared to a model simulation with no Holuhraun emissions. The largest increases, apart from extreme values on Iceland, are found on the coast of northern Norway, a region with frequent precipitation during westerly winds. Over a 3-month average (during SON 2014) over Europe, SO2 and PM2.5 surface concentrations, due to the volcanic emissions, increased by only ten and 6 % respectively. Although the percent increase of PM2.5 concentration is highest over Scandinavia and Scotland, an increase in PM exceedance days is found over Ireland and the already polluted Benelux region (up to 3 additional days), where any small increase in particulate matter concentration leads to an increase in exceedance days.

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