scholarly journals MIPAS observations of volcanic sulfate aerosol and sulfur dioxide in the stratosphere

2018 ◽  
Vol 18 (2) ◽  
pp. 1217-1239 ◽  
Author(s):  
Annika Günther ◽  
Michael Höpfner ◽  
Björn-Martin Sinnhuber ◽  
Sabine Griessbach ◽  
Terry Deshler ◽  
...  
Keyword(s):  
Transport Model ◽  
Michelson Interferometer ◽  
Background Level ◽  
Volcanic Eruptions ◽  
Sulfate Aerosol ◽  
Boreal Summer ◽  
Chemical Transport Model ◽  
In Situ Data

Abstract. Volcanic eruptions can increase the stratospheric sulfur loading by orders of magnitude above the background level and are the most important source of variability in stratospheric sulfur. We present a set of vertical profiles of sulfate aerosol volume densities and derived liquid-phase H2SO4 (sulfuric acid) mole fractions for 2005–2012, retrieved from infrared limb emission measurements performed with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board of the Environmental Satellite (Envisat). Relative to balloon-borne in situ measurements of aerosol at Laramie, Wyoming, the MIPAS aerosol data have a positive bias that has been corrected, based on the observed differences to the in situ data. We investigate the production of stratospheric sulfate aerosol from volcanically emitted SO2 for two case studies: the eruptions of Kasatochi in 2008 and Sarychev in 2009, which both occurred in the Northern Hemisphere midlatitudes during boreal summer. With the help of chemical transport model (CTM) simulations for the two volcanic eruptions we show that the MIPAS sulfate aerosol and SO2 data are qualitatively and quantitatively consistent with each other. Further, we demonstrate that the lifetime of SO2 is explained well by its oxidation by hydroxyl radicals (OH). While the sedimentation of sulfate aerosol plays a role, we find that the long-term decay of stratospheric sulfur after these volcanic eruptions in midlatitudes is mainly controlled by transport via the Brewer–Dobson circulation. Sulfur emitted by the two midlatitude volcanoes resides mostly north of 30∘ N at altitudes of ∼ 10–16 km, while at higher altitudes (∼ 18–22 km) part of the volcanic sulfur is transported towards the Equator where it is lifted into the stratospheric “overworld” and can further be transported into both hemispheres.

scholarly journals MIPAS observations of volcanic sulphate aerosol and sulphur dioxide in the stratosphere

2017 ◽  
Author(s):  
Annika Günther ◽  
Michael Höpfner ◽  
Björn-Martin Sinnhuber ◽  
Sabine Griessbach ◽  
Terry Deshler ◽  
...  
Keyword(s):  
Sulphur Dioxide ◽  
Transport Model ◽  
Michelson Interferometer ◽  
Background Level ◽  
Volcanic Eruptions ◽  
Boreal Summer ◽  
Chemical Transport Model ◽  
Sulphate Aerosol ◽  
Aerosol Volume

Abstract. Volcanic eruptions can increase the stratospheric sulphur content by orders of magnitude above the background level and are the most important source of variability of stratospheric sulphur loading. We present a set of vertical profiles of sulphate aerosol volume densities and derived liquid-phase H2SO4 mole-fractions for 2005–2012, retrieved from infrared limb emission measurements by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board of the Environmental Satellite. The MIPAS aerosol dataset has been corrected for a possible altitude-dependent bias by comparison with balloon-borne in situ aerosol measurements at Laramie, Wyoming. The MIPAS data of stratospheric sulphate aerosol is linked to MIPAS observations of sulphur dioxide (SO2) with the help of Chemical Transport Model simulations. We investigate the production of sulphate aerosol and its fate from volcanically emitted SO2 for two volcanic case studies: the eruptions of Kasatochi in 2008 and Sarychev in 2009, which both occurred in the Northern Hemisphere mid-latitudes during boreal summer. We show that the MIPAS sulphate aerosol and SO2 data are qualitatively and quantitatively consistent to each other. Further, we demonstrate that the lifetime of SO2 is well described by its oxidation by hydroxyl radicals. While sedimentation of the sulphate aerosol plays a role, we find that the dominant mechanism controlling the stratospheric lifetime of sulphur after these volcanic eruptions at mid-latitudes is transport in the Brewer-Dobson circulation. Sulphur emitted by the two mid-latitude volcanoes resides mostly north of 30° N at altitudes of ~ 10–16 km, while at higher altitudes (~ 18–22 km) part of the volcanic sulphur is transported towards the equator where it is lifted into the stratospheric overworld and can further be transported into both hemispheres.

Global Methane Emissions Through an Isotopic Lens

2020 ◽  
Author(s):  
Alice Drinkwater ◽  
Tim Arnold ◽  
Paul Palmer
Keyword(s):  
Transport Model ◽  
Global Climate ◽  
Agricultural Practices ◽  
Isotope Ratios ◽  
Atmospheric Methane ◽  
Source Attribution ◽  
Chemical Transport Model ◽  
Magnitude Distribution ◽  
In Situ Data

<p>Changes in atmospheric methane (CH<sub>4</sub>) are mainly driven by natural, anthropogenic and pyrogenic emissions and oxidation by OH.</p><p>There is no consensus about the underlying explanations about hemispheric-scale changes in atmospheric methane (CH<sub>4</sub>). This is partly due to sparse data that do not exclusively identify individual changes in surface emissions and surface and atmospheric losses of CH<sub>4</sub>. This challenge represents a major scientific weakness in our understanding of this potent greenhouse gas, with implications for meeting global climate policy obligations.  A confounding challenge is that the regional importance of individual emission sources change with time due to, for example, innovations in agricultural practices, climate-sensitive wetlands, and political decisions associated with climate friendlier transitional fuels.  </p><p><br>Here we use bulk isotope ratios δ<sup>13</sup>C and δD of CH<sub>4</sub> that have been previously shown to provide effective constraints on source apportionment: different CH<sub>4</sub> sources have characteristic isotope ratios. One of the key challenges associated with using these data is that region-specific isotope ratios change with time due to varying source prevalance, in addition to source signatures having inherent uncertainties. We use the GEOS-Chem global 3-D chemical transport model to describe the spatial and temporal isotopic behaviour of atmospheric CH<sub>4</sub>. We develop a Maximum A-Posteriori inverse method to simultaneously infer time dependent CH<sub>4</sub> emissions and isotope ratios from in situ data. </p><p>We will report the magnitude, distribution and source attribution of CH<sub>4</sub> emissions from 2004 to 2017, inferred from in situ measurements of total atmospheric CH<sub>4</sub> mole fraction and the corresponding measurements of δ<sup>13</sup>C and δD. We will compare our results with previous studies.</p>

scholarly journals Intercomparison methods for satellite measurements of atmospheric composition: application to tropospheric ozone from TES and OMI

2010 ◽  
Vol 10 (1) ◽  
pp. 1417-1456 ◽  
Author(s):  
L. Zhang ◽  
D. J. Jacob ◽  
X. Liu ◽  
J. A. Logan ◽  
K. Chance ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Kernel Smoothing ◽  
Transport Model ◽  
Atmospheric Composition ◽  
Chemical Transport Model ◽  
Ozone Monitoring Instrument ◽  
Satellite Measurements ◽  
In Situ Data ◽  
In Situ Method

Abstract. We analyze three different methods to validate and intercompare satellite measurements of atmospheric composition, and apply them to tropospheric ozone retrievals from the Tropospheric Emission Spectrometer (TES) and the Ozone Monitoring Instrument (OMI). The first method (in situ method) uses in situ vertical profiles for absolute instrument validation; it is limited by the sparseness of in situ data. The second method (CTM method) uses a chemical transport model (CTM) as an intercomparison platform; it provides a globally complete intercomparison with relatively small noise added by model error. The third method (averaging kernel smoothing method) involves smoothing the retrieved profile from one instrument with the averaging kernel matrix of the other; it also provides a global intercomparison but dampens the actual difference between instruments and adds noise from the a priori. Application to a full year (2006) of TES and OMI data shows mean positive biases of 5.3 parts per billion volume (ppbv) (10%) for TES and 2.8 ppbv (5%) for OMI at 500 hPa relative to in situ data from ozonesondes. We show that the CTM method (using the GEOS-Chem CTM) closely approximates results from the in situ method while providing global coverage. It reveals that differences between TES and OMI are generally less than 10 ppbv (18%), except at northern mid-latitudes in summer and over tropical continents. The CTM method allows for well-constrained CTM evaluation in places where the satellite observations are consistent. We thus find that GEOS-Chem underestimates tropospheric ozone in the tropics, reflecting a combination of possible factors, and overestimates ozone in the northern subtropics and southern mid-latitudes, likely because of excessive stratospheric influx.

scholarly journals Intercomparison methods for satellite measurements of atmospheric composition: application to tropospheric ozone from TES and OMI

2010 ◽  
Vol 10 (10) ◽  
pp. 4725-4739 ◽  
Author(s):  
L. Zhang ◽  
D. J. Jacob ◽  
X. Liu ◽  
J. A. Logan ◽  
K. Chance ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Kernel Smoothing ◽  
Transport Model ◽  
Atmospheric Composition ◽  
Chemical Transport Model ◽  
Ozone Monitoring Instrument ◽  
Satellite Measurements ◽  
In Situ Data ◽  
In Situ Method

Abstract. We analyze the theoretical basis of three different methods to validate and intercompare satellite measurements of atmospheric composition, and apply them to tropospheric ozone retrievals from the Tropospheric Emission Spectrometer (TES) and the Ozone Monitoring Instrument (OMI). The first method (in situ method) uses in situ vertical profiles for absolute instrument validation; it is limited by the sparseness of in situ data. The second method (CTM method) uses a chemical transport model (CTM) as an intercomparison platform; it provides a globally complete intercomparison with relatively small noise from model error. The third method (averaging kernel smoothing method) involves smoothing the retrieved profile from one instrument with the averaging kernel matrix of the other; it also provides a global intercomparison but dampens the actual difference between instruments and adds noise from the a priori. We apply the three methods to a full year (2006) of TES and OMI data. Comparison with in situ data from ozonesondes shows mean positive biases of 5.3 parts per billion volume (ppbv) (10%) for TES and 2.8 ppbv (5%) for OMI at 500 hPa. We show that the CTM method (using the GEOS-Chem CTM) closely approximates results from the in situ method while providing global coverage. It reveals that differences between TES and OMI are generally less than 10 ppbv (18%), except at northern mid-latitudes in summer and over tropical continents. The CTM method further allows for CTM evaluation using both satellite observations. We thus find that GEOS-Chem underestimates tropospheric ozone in the tropics due to possible underestimates of biomass burning, soil, and lightning emissions. It overestimates ozone in the northern subtropics and southern mid-latitudes, likely because of excessive stratospheric influx of ozone.

scholarly journals Global estimates of CO sources with high resolution by adjoint inversion of multiple satellite datasets (MOPITT, AIRS, SCIAMACHY, TES)

2009 ◽  
Vol 9 (5) ◽  
pp. 19967-20018 ◽  
Author(s):  
M. Kopacz ◽  
D. J. Jacob ◽  
J. A. Fisher ◽  
J. A. Logan ◽  
L. Zhang ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Transport Model ◽  
Large Fraction ◽  
A Priori ◽  
A Posteriori ◽  
Chemical Transport Model ◽  
In Situ Data ◽  
Global Emission ◽  
Cold Starts

Abstract. We combine CO column measurements from the MOPITT, AIRS, SCIAMACHY, and TES satellite instruments in a full-year (May 2004–April 2005) global inversion of CO sources at 4°×5° spatial resolution and monthly temporal resolution. The inversion uses the GEOS-Chem chemical transport model (CTM) and its adjoint applied to MOPITT, AIRS, and SCIAMACHY. Observations from TES, surface sites (NOAA/GMD), and aircraft (MOZAIC) are used for evaluation of the a posteriori solution. Global intercomparison of the different satellite datasets using GEOS-Chem as a common intercomparison platform shows consistency between the satellite datasets and with the in situ data. The majority of the differences between the datasets can be explained by different averaging kernels and a priori information. The global CO emission from combustion as constrained in the inversion is 1350 Tg a−1, with an additional 217 Tg a−1 from oxidation of co-emitted VOCs. This is much higher than current bottom-up emission inventories. Consistent with both the satellite and in situ data, a large fraction of the correction results from a seasonal underestimate of CO sources at northern mid-latitudes and suggests a larger-than-expected CO source from vehicle cold starts and residential heating. A posteriori emissions also indicate a general underestimation of biomass burning relative to the GFED2 inventory. However, the tropical biomass burning constraints are not consistent across the different datasets. Although the datasets reveal regional inconsistencies over tropical biomass burning regions, we find the global emission estimates to be a balance of information from all three instruments.

scholarly journals Regional and intercontinental pollution signatures on modeled and measured PAN at northern mid-latitude mountain sites

2018 ◽  
Author(s):  
Arlene M. Fiore ◽  
Emily V. Fischer ◽  
Shubha Pandey Deolal ◽  
Oliver Wild ◽  
Dan Jaffe ◽  
...  
Keyword(s):  
Transport Model ◽  
Ozone Production ◽  
Anthropogenic Emissions ◽  
Chemical Transport Model ◽  
Reservoir Species ◽  
Remote Troposphere ◽  
Global Chemical Transport Model ◽  
Peroxy Acetyl Nitrate ◽  
Source Receptor Relationships

Abstract. Peroxy acetyl nitrate (PAN) is the most important reservoir species for nitrogen oxides (NOx) in the remote troposphere. Upon decomposition in remote regions, PAN promotes efficient ozone production. We evaluate monthly mean PAN abundances from global chemical transport model simulations (HTAP1) for 2001 with measurements from five northern mid-latitude mountain sites (four European and one North American). The multi-model mean generally captures the observed monthly mean PAN but individual models simulate a factor of ~ 4–8 range in monthly abundances. We quantify PAN source-receptor relationships at the measurement sites with sensitivity simulations that decrease regional anthropogenic emissions of PAN (and ozone) precursors by 20 % from North America (NA), Europe (EU), and East Asia (EA). The HTAP1 models attribute more of the observed PAN at Jungfraujoch (Switzerland) to emissions in NA and EA, and less to EU, than a prior trajectory-based estimate. The trajectory-based and modeling approaches agree that EU emissions play a role in the observed springtime PAN maximum at Jungfraujoch. The signal from anthropogenic emissions on PAN is strongest at Jungfraujoch and Mount Bachelor (Oregon, U.S.A.) during April. In this month, PAN source-receptor relationships correlate both with model differences in regional anthropogenic volatile organic compound (AVOC) emissions and with ozone source-receptor relationships. PAN observations at mountaintop sites can thus provide key information for evaluating models, including links between PAN and ozone production and source-receptor relationships. Establishing routine, long-term, mountaintop measurements is essential given the large observed interannual variability in PAN.

scholarly journals Evaluation of water vapour assimilation in the tropical upper troposphere and lower stratosphere by a chemical transport model

2016 ◽  
Vol 9 (9) ◽  
pp. 4355-4373 ◽  
Author(s):  
Swagata Payra ◽  
Philippe Ricaud ◽  
Rachid Abida ◽  
Laaziz El Amraoui ◽  
Jean-Luc Attié ◽  
...  
Keyword(s):  
Water Vapour ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Michelson Interferometer ◽  
Model Space ◽  
Global Scale ◽  
Chemical Transport Model ◽  
Data Set ◽  
Upper Troposphere ◽  
Sensitivity Studies

Abstract. The present analysis deals with one of the most debated aspects of the studies on the upper troposphere/lower stratosphere (UTLS), namely the budget of water vapour (H2O) at the tropical tropopause. Within the French project “Multiscale water budget in the upper troposphere and lower stratosphere in the TROpics” (TRO-pico), a global-scale analysis has been set up based on space-borne observations, models and assimilation techniques. The MOCAGE-VALENTINA assimilation tool has been used to assimilate the Aura Microwave Limb Sounder (MLS) version 3.3 H2O measurements within the 316–5 hPa range from August 2011 to March 2013 with an assimilation window of 1 h. Diagnostics based on observations minus analysis and forecast are developed to assess the quality of the assimilated H2O fields. Comparison with an independent source of H2O measurements in the UTLS based on the space-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) observations and with meteorological ARPEGE analyses is also shown. Sensitivity studies of the analysed fields have been performed by (1) considering periods when no MLS measurements are available and (2) using H2O data from another MLS version (4.2). The studies have been performed within three different spaces in time and space coincidences with MLS (hereafter referred to as MLS space) and MIPAS (MIPAS space) observations and with the model (model space) outputs and at three different levels: 121 hPa (upper troposphere), 100 hPa (tropopause) and 68 hPa (lower stratosphere) in January and February 2012. In the MLS space, the analyses behave consistently with the MLS observations from the upper troposphere to the lower stratosphere. In the model space, the analyses are wetter than the reference atmosphere as represented by ARPEGE and MLS in the upper troposphere (121 hPa) and around the tropopause (100 hPa), but are consistent with MLS and MIPAS in the lower stratosphere (68 hPa). In the MIPAS space, the sensitivity and the vertical resolution of the MIPAS data set at 121 and 100 hPa prevent assessment of the behaviour of the analyses at 121 and 100 hPa, particularly over intense convective areas as the South American, the African and the Maritime continents but, in the lower stratosphere (68 hPa), the analyses are very consistent with MIPAS. Sensitivity studies show the improvement on the H2O analyses in the tropical UTLS when assimilating space-borne measurements of better quality, particularly over the convective areas.

scholarly journals Rainfall Estimates on a Gridded Network (REGEN) – a global land-based gridded dataset of daily precipitation from 1950 to 2016

2020 ◽  
Vol 24 (2) ◽  
pp. 919-943 ◽  
Author(s):  
Steefan Contractor ◽  
Markus G. Donat ◽  
Lisa V. Alexander ◽  
Markus Ziese ◽  
Anja Meyer-Christoffer ◽  
...  
Keyword(s):  
Daily Precipitation ◽  
In Situ Data ◽  
Global Precipitation Climatology Centre ◽  
Historical Climatology ◽  
Global Land ◽  
Global Historical Climatology Network ◽  
Global Precipitation ◽  
Rainfall Estimates

Abstract. We present a new global land-based daily precipitation dataset from 1950 using an interpolated network of in situ data called Rainfall Estimates on a Gridded Network – REGEN. We merged multiple archives of in situ data including two of the largest archives, the Global Historical Climatology Network – Daily (GHCN-Daily) hosted by National Centres of Environmental Information (NCEI), USA, and one hosted by the Global Precipitation Climatology Centre (GPCC) operated by Deutscher Wetterdienst (DWD). This resulted in an unprecedented station density compared to existing datasets. The station time series were quality-controlled using strict criteria and flagged values were removed. Remaining values were interpolated to create area-average estimates of daily precipitation for global land areas on a 1∘ × 1∘ latitude–longitude resolution. Besides the daily precipitation amounts, fields of standard deviation, kriging error and number of stations are also provided. We also provide a quality mask based on these uncertainty measures. For those interested in a dataset with lower station network variability we also provide a related dataset based on a network of long-term stations which interpolates stations with a record length of at least 40 years. The REGEN datasets are expected to contribute to the advancement of hydrological science and practice by facilitating studies aiming to understand changes and variability in several aspects of daily precipitation distributions, extremes and measures of hydrological intensity. Here we document the development of the dataset and guidelines for best practices for users with regards to the two datasets.

scholarly journals The Canadian atmospheric transport model for simulating greenhouse gas evolution on regional scales: GEM-MACH-GHG v.137-reg

2019 ◽  
Author(s):  
Jinwoong Kim ◽  
Saroja Polavarapu ◽  
Douglas Chan ◽  
Michael Neish
Keyword(s):  
Greenhouse Gas ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Forecast Error ◽  
Regional Scale ◽  
The United States ◽  
Regional Model ◽  
Boreal Summer ◽  
Chemical Transport Model ◽  
Atmospheric Transport Model

Abstract. In this study, we present the development of a regional atmospheric transport model for greenhouse gas (GHG) simulation based on an operational weather forecast model and a chemical transport model at Environment and Climate Change Canada (ECCC), with the goal of improving our understanding of the high spatio-temporal resolution interaction between the atmosphere and surface GHG fluxes over Canada and the United States. The regional model uses 10 km × 10 km horizontal grid spacing and 80 vertical levels spanning the ground to 0.1 hPa. The lateral boundary conditions of meteorology and tracers are provided by the global transport model used for GHG simulation at ECCC. The performance of the regional model and added benefit of the regional model over our lower resolution global models is investigated in terms of modelled CO2 concentration and meteorological forecast quality for multiple seasons in 2015. We find that our regional model has the capability to simulate high spatial (horizontal and vertical) and temporal scales of atmospheric CO2 concentrations, based on comparisons to surface and aircraft observations. In addition, reduced bias and standard deviation of forecast error in boreal summer are obtained by the regional model. Better representation of model topography in the regional model reduces transport and representation errors significantly compared to the global model, especially in regions of complex topography, as revealed by the more precise and detailed structure of the CO2 diurnal cycle produced at observation sites and in model space. The new regional model will form the basis of a flux inversion system that estimates regional scale fluxes of GHGs over Canada.

scholarly journals Retrieval of total column and surface NO<sub>2</sub> from Pandora zenith-sky measurements

2019 ◽  
Author(s):  
Xiaoyi Zhao ◽  
Debora Griffin ◽  
Vitali Fioletov ◽  
Chris McLinden ◽  
Jonathan Davies ◽  
...  
Keyword(s):  
Transport Model ◽  
Surface Concentration ◽  
In Situ Measurements ◽  
Radiative Transfer Model ◽  
Retrieval Algorithm ◽  
Transfer Model ◽  
Chemical Transport Model ◽  
High Quality ◽  
Vertical Column

Abstract. Pandora spectrometers can retrieve nitrogen dioxide (NO2) vertical column densities (VCDs) via two viewing geometries: direct-sun and zenith-sky. The direct-sun NO2 VCD measurements have high quality (0.1 DU accuracy in clear-sky conditions) and do not rely on any radiative transfer model to calculate air mass factors (AMFs); however, they are not available when the sun is obscured by clouds. To perform NO2 measurements in cloudy conditions, a simple but robust NO2 retrieval algorithm is developed for Pandora zenith-sky measurements. This algorithm derives empirical zenith-sky NO2 AMFs from coincident high-quality direct-sun NO2 observations. Moreover, the retrieved Pandora zenith-sky NO2 VCD data are converted to surface NO2 concentrations with a scaling algorithm that uses chemical-transport-model predictions and satellite measurements as inputs. NO2 VCDs and surface concentrations are retrieved from Pandora zenith-sky measurements made in Toronto, Canada, from 2015 to 2017. The retrieved Pandora zenith-sky NO2 data (VCD and surface concentration) show good agreement with both satellite and in situ measurements. The diurnal and seasonal variations of derived Pandora zenith-sky surface NO2 data also agree well with in situ measurements (diurnal difference within ±2 ppbv). Overall, this work shows that the new Pandora zenith-sky NO2 products have the potential to be used in various applications such as future satellite validation in moderate cloudy scenes and air quality monitoring.

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