scholarly journals Validation of TES methane with HIPPO aircraft observations: implications for inverse modeling of methane sources

2011 ◽  
Vol 11 (10) ◽  
pp. 27887-27911
Author(s):  
K. J. Wecht ◽  
D. J. Jacob ◽  
S. C. Wofsy ◽  
E. A. Kort ◽  
J. R. Worden ◽  
...  
Keyword(s):  
Simulation Experiment ◽  
Transport Model ◽  
Observation System ◽  
Chemical Transport Model ◽  
Surface Type ◽  
Upper Troposphere ◽  
The Pacific ◽  
Standard Product ◽  
Aircraft Observations ◽  
Better Than

Abstract. We validate satellite methane observations from the Tropospheric Emission Spectrometer (TES) with 151 aircraft vertical profiles over the Pacific from the HIAPER Pole-to-Pole Observation (HIPPO) program. We find that a collocation window of ±750 km and ±24 h does not introduce significant error in comparing TES and aircraft profiles. We validate both the TES standard product (V004) and an experimental product with two pieces of information in the vertical (V005). We determine a V004 mean bias of 65.7 ppb with residual standard deviation of 44.2 ppb. For V005 we determine mean biases (residual standard deviations) in the lower and upper troposphere of 18.2 (31.1) and 49.4 (33.2) ppb, respectively. TES errors show no significant dependence on latitude or surface type. Even when V005 cannot retrieve two pieces of information it still performs better than V004. An observation system simulation experiment (OSSE) with the GEOS-Chem chemical transport model (CTM) and its adjoint shows that TES V004 has only limited value for constraining methane sources. Our successful validation of V005 encourages its production as a standard retrieval to replace V004.

scholarly journals Validation of TES methane with HIPPO aircraft observations: implications for inverse modeling of methane sources

2012 ◽  
Vol 12 (4) ◽  
pp. 1823-1832 ◽  
Author(s):  
K. J. Wecht ◽  
D. J. Jacob ◽  
S. C. Wofsy ◽  
E. A. Kort ◽  
J. R. Worden ◽  
...  
Keyword(s):  
Transport Model ◽  
Lower Troposphere ◽  
Observation System ◽  
Chemical Transport Model ◽  
Instrument Error ◽  
The Pacific ◽  
Standard Product ◽  
Aircraft Observations ◽  
Low Latitudes ◽  
Better Than

Abstract. We validate satellite methane observations from the Tropospheric Emission Spectrometer (TES) with 151 aircraft vertical profiles over the Pacific from the HIAPER Pole-to-Pole Observation (HIPPO) program. We find that a collocation window of ±750 km and ±24 h does not introduce significant error in comparing TES and aircraft profiles. We validate both the TES standard product (V004) and an experimental product with two pieces of information in the vertical (V005). We determine a V004 mean bias of 65.8 ppb and random instrument error of 43.3 ppb. For V005 we determine a mean bias of 42.3 ppb and random instrument error of 26.5 ppb in the upper troposphere, and mean biases (random instrument errors) in the lower troposphere of 28.8 (28.7) and 16.9 (28.9) ppb at high and low latitudes respectively. Even when V005 cannot retrieve two pieces of information it still performs better than V004. An observation system simulation experiment (OSSE) with the GEOS-Chem chemical transport model (CTM) and its adjoint shows that TES V004 has only limited value for constraining methane sources. Our successful validation of V005 encourages its production as a standard retrieval to replace V004.

scholarly journals CO source contribution analysis for California during ARCTAS-CARB

2011 ◽  
Vol 11 (2) ◽  
pp. 3627-3661 ◽  
Author(s):  
G. G. Pfister ◽  
J. Avise ◽  
C. Wiedinmyer ◽  
D. P. Edwards ◽  
L. K. Emmons ◽  
...  
Keyword(s):  
Transport Model ◽  
Anthropogenic Sources ◽  
Relative Importance ◽  
Free Troposphere ◽  
Chemical Transport Model ◽  
Time Period ◽  
The Pacific ◽  
Aircraft Observations ◽  
Satellite Retrievals ◽  
Local Emissions

Abstract. Air pollution is of concern in many parts of California and is impacted by both local emissions and also by pollution inflow from the Pacific. In this study, we use the regional chemical transport model WRF-Chem V3.2 to examine the CO budget over California. We include model CO tracers for different emission sources in the model, which allow estimating the relative importance of local sources versus pollution inflow on the distribution of CO at the surface and in the free troposphere. The focus of our study is on the 15 June–15 July 2008 time period, which coincides with the aircraft deployment of the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission over California. Model simulations are evaluated using these aircraft observations as well as satellite retrievals and surface observations of CO. Evaluation results show that the model overall predicts the observed CO fields well, but points towards an underestimate of CO from the fires in Northern California, which had a strong influence during the study period, and towards a slight overestimate of CO from pollution inflow and local anthropogenic sources. The analysis of the CO budget over California reveals that inflow of CO explains on average 53 ± 21% of surface CO during the study period, compared to 22 ± 18% for local anthropogenic sources and 18 ± 22% for fires. In the free troposphere, the average CO contributions are estimated as 78 ± 16% for CO inflow, 6 ± 4% for CO from local anthropogenic sources and 11 ± 13% for CO from fires.

First estimate of NO2 in the upper troposphere from TROPOMI

2020 ◽  
Author(s):  
Eloise Marais ◽  
Joanna Joiner ◽  
Sungyeon Choi
Keyword(s):  
Transport Model ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Ozone Monitoring Instrument ◽  
Commercial Aircraft ◽  
Upper Troposphere ◽  
Aircraft Observations ◽  
Research Aircraft ◽  
Ozone Monitoring ◽  
Sky Conditions

<p>Nitrogen oxides (NO<sub> x</sub> = NO + NO<sub>2</sub>) in the upper troposphere (~10-12 km) are effective at producing ozone in the upper troposphere where ozone is a potent greenhouse gas. Observations of NO<sub>x</sub> in the upper troposphere are limited in time to a few intensive research aircraft campaigns and in space to commercial aircraft campaigns. There are satellite-derived observations of NO<sub>2</sub> in the upper troposphere from the Ozone Monitoring Instrument (OMI), but these are at very coarse resolutions (seasonal, > 2,000 km). The high-resolution Sentinel-5P/TROPOMI instrument offers higher spatial resolution and better cloud-resolving capability than OMI. Here we use synthetic columns of NO<sub>2</sub> from the GEOS-Chem chemical transport model to assess feasibility of deriving NO<sub>2</sub> in the upper troposphere using partial columns of NO<sub>2</sub> above cloudy scenes (the so-called cloud-slicing technique). The model is also used to quantify errors induced by uncertainties in cloud-top height and to determine whether NO<sub>2</sub> over cloudy scenes is representative of all-sky conditions (the "truth"). We find that the cloud-slicing approach is spatially consistent (R =0.5) with the "truth", but with a small (10 pptv) bias in background NO<sub>2</sub>. Cloud-slicing is then applied to TROPOMI total columns of NO<sub>2</sub> to derive near-global observations of NO<sub>2</sub> in the upper troposphere and assessed against the existing OMI products and aircraft observations from NASA DC8 aircraft campaigns.</p>

scholarly journals Observing atmospheric formaldehyde (HCHO) from space: validation and intercomparison of six retrievals from four satellites (OMI, GOME2A, GOME2B, OMPS) with SEAC<sup>4</sup>RS aircraft observations over the Southeast US

2016 ◽  
Author(s):  
Lei Zhu ◽  
Daniel J. Jacob ◽  
Patrick S. Kim ◽  
Jenny A. Fisher ◽  
Karen Yu ◽  
...  
Keyword(s):  
Transport Model ◽  
Research Groups ◽  
Chemical Transport Model ◽  
Shape Factors ◽  
Aircraft Observations ◽  
Volatile Organic ◽  
Satellite Retrievals ◽  
Mass Factor ◽  
The Mean ◽  
Southeast Us

Abstract. Formaldehyde (HCHO) column data from satellites are widely used as a proxy for emissions of volatile organic compounds (VOCs), but validation of the data has been extremely limited. Here we use highly accurate HCHO aircraft observations from the NASA SEAC4RS campaign over the Southeast US in August–September 2013 to validate and intercompare six operational and research retrievals of HCHO columns from four different satellite instruments (OMI, GOME2A, GOME2B and OMPS) and three different research groups. The GEOS-Chem chemical transport model provides a common intercomparison platform. We find that all retrievals capture the HCHO maximum over Arkansas and Louisiana, reflecting high emissions of biogenic isoprene, and are consistent in their spatial variability over the Southeast US (r = 0.4–0.8 on a 0.5° × 0.5° grid) as well as their day-to-day variability (r = 0.5–0.8). However, all satellite retrievals are biased low in the mean by 20–51 %, which would lead to corresponding bias in estimates of isoprene emissions from the satellite data. The smallest bias is for OMI-BIRA, which has the highest corrected slant columns and the lowest scattering weights in its air mass factor (AMF) calculation. Correcting the assumed HCHO vertical profiles (shape factors) used in the AMF calculation would further reduce the bias in the OMI-BIRA data. We conclude that current satellite HCHO data provide a reliable proxy for isoprene emission variability but with a low mean bias due both to the corrected slant columns and the scattering weights used in the retrievals.

scholarly journals Modeling the transport of very short-lived substances into the tropical upper troposphere and lower stratosphere

2009 ◽  
Vol 9 (5) ◽  
pp. 18511-18543 ◽  
Author(s):  
J. Aschmann ◽  
B. M. Sinnhuber ◽  
E. L. Atlas ◽  
S. M. Schauffler
Keyword(s):  
Large Scale ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport Model ◽  
Heating Rates ◽  
Model Calculations ◽  
Upper Troposphere ◽  
Mass Fluxes ◽  
Tropical Upper Troposphere

Abstract. The transport of very short-lived substances into the tropical upper troposphere and lower stratosphere is investigated by a three-dimensional chemical transport model using archived convective updraft mass fluxes (or detrainment rates) from the European Centre for Medium-Range Weather Forecast's ERA-Interim reanalysis. Large-scale vertical velocities are calculated from diabatic heating rates. With this approach we explicitly model the large scale subsidence in the tropical troposphere with convection taking place in fast and isolated updraft events. The model calculations agree generally well with observations of bromoform and methyl iodide from aircraft campaigns and with ozone and water vapor from sonde and satellite observations. Using a simplified treatment of dehydration and bromine product gas washout we give a range of 1.6 to 3 ppt for the contribution of bromoform to stratospheric bromine, assuming a uniform source in the boundary layer of 1 ppt. We show that the most effective region for VSLS transport into the stratosphere is the West Pacific, accounting for about 55% of the bromine from bromoform transported into the stratosphere under the supposition of a uniformly distributed source.

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.

A recent slowdown in the decline of CFC-11 concentrations in the upper troposphere

2020 ◽  
Author(s):  
Patrick Sheese ◽  
Kaley Walker ◽  
Chris Boone ◽  
Laura Saunders ◽  
Sandip Dhomse ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Recent Change ◽  
Fourier Transform Spectrometer ◽  
Chemical Transport Model ◽  
Surface Level ◽  
Upper Troposphere ◽  
The Past ◽  
Ozone Depleting Substances ◽  
Chemistry Experiment

&lt;p&gt;Since 2004, the Atmospheric Chemistry Experiment &amp;#8211; Fourier Transform Spectrometer (ACE-FTS) instrument has been measuring concentrations of chlorofluorocarbons (CFCs) in the stratosphere and upper troposphere and is currently the only satellite instrument that measures vertically resolved profiles of CFC&amp;#8209;11. Since CFCs are major ozone depleting substances, monitoring their atmospheric abundances is critical for understanding ozone layer recovery. Recent studies based solely on surface-level measurements have shown strong evidence for new CFC&amp;#8209;11 production, leading to an increase in CFC&amp;#8209;11 emissions over the past decade. In this study, the TOMCAT/SLIMCAT 3-D chemical transport model is used in order to bridge the altitude/geolocation gap between ACE-FTS measurements in the UTLS and surface level measurements. Trends in two different time periods over the ACE-FTS mission, 2004-2012 and 2013-2018, are examined to determine if the recent change in surface level CFC-11 trends is influencing UTLS concentrations. The ACE-FTS measurements show that, below ~10 km, the rate of decrease of global CFC-11 concentrations was slower during 2013-2018 (-1.2 pptv/year) than during 2004-2012 (&amp;#8209;2.0 pptv/year). Similar trends are observed in the model data for the same spatial/temporal regions.&lt;/p&gt;

scholarly journals Using beryllium-7 to assess cross-tropopause transport in global models

2016 ◽  
Vol 16 (7) ◽  
pp. 4641-4659 ◽  
Author(s):  
Hongyu Liu ◽  
David B. Considine ◽  
Larry W. Horowitz ◽  
James H. Crawford ◽  
Jose M. Rodriguez ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Transport Model ◽  
Meteorological Data ◽  
Data Sets ◽  
High Latitudes ◽  
Chemical Transport Model ◽  
Modeling Framework ◽  
Global Models ◽  
Deposition Fluxes ◽  
Upper Troposphere

Abstract. We use the Global Modeling Initiative (GMI) modeling framework to assess the utility of cosmogenic beryllium-7 (7Be), a natural aerosol tracer, for evaluating cross-tropopause transport in global models. The GMI chemical transport model (CTM) was used to simulate atmospheric 7Be distributions using four different meteorological data sets (GEOS1-STRAT DAS, GISS II′ GCM, fvGCM, and GEOS4-DAS), featuring significantly different stratosphere–troposphere exchange (STE) characteristics. The simulations were compared with the upper troposphere and/or lower stratosphere (UT/LS) 7Be climatology constructed from  ∼  25 years of aircraft and balloon data, as well as climatological records of surface concentrations and deposition fluxes. Comparison of the fraction of surface air of stratospheric origin estimated from the 7Be simulations with observationally derived estimates indicates excessive cross-tropopause transport at mid-latitudes in simulations using GEOS1-STRAT and at high latitudes using GISS II′ meteorological data. These simulations also overestimate 7Be deposition fluxes at mid-latitudes (GEOS1-STRAT) and at high latitudes (GISS II′), respectively. We show that excessive cross-tropopause transport of 7Be corresponds to overestimated stratospheric contribution to tropospheric ozone. Our perspectives on STE in these meteorological fields based on 7Be simulations are consistent with previous modeling studies of tropospheric ozone using the same meteorological fields. We conclude that the observational constraints for 7Be and observed 7Be total deposition fluxes can be used routinely as a first-order assessment of cross-tropopause transport in global models.

scholarly journals Global tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants

2021 ◽  
Author(s):  
Xuan Wang ◽  
Daniel J. Jacob ◽  
William Downs ◽  
Shuting Zhai ◽  
Lei Zhu ◽  
...  
Keyword(s):  
Marine Boundary Layer ◽  
Transport Model ◽  
Ph Dependence ◽  
Primary Source ◽  
Mixing Ratio ◽  
Chemical Transport Model ◽  
Oxidation Of Methane ◽  
Aircraft Observations ◽  
Chlorine Radicals ◽  
Global Mean

Abstract. We present an updated mechanism for tropospheric halogen (Cl + Br + I) chemistry in the GEOS-Chem global atmospheric chemical transport model and apply it to investigate halogen radical cycling and implications for tropospheric oxidants. Improved representation of HOBr heterogeneous chemistry and its pH dependence in our simulation leads to less effective recycling and mobilization of bromine radicals, and enables the model to include mechanistic sea salt aerosol debromination without generating excessive BrO. The resulting global mean tropospheric BrO mixing ratio is 0.19 ppt, lower than previous versions of GEOS-Chem. Model BrO shows variable consistency and biases in comparison to surface and aircraft observations in marine air, which are often near or below the detection limit. The model underestimates the daytime measurements of Cl2 and BrCl from the ATom aircraft campaign over the Pacific and Atlantic, which if correct would imply a very large missing primary source of chlorine radicals. Model IO is highest in the marine boundary layer and uniform in the free troposphere, with a global mean tropospheric mixing ratio of 0.08 ppt, and shows consistency with surface and aircraft observations. The modeled global mean tropospheric concentration of Cl atoms is 630 cm−3, contributing 0.8 % of the global oxidation of methane, 14 % of ethane, 8 % of propane, and 7 % of higher alkanes. Halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %. Most of the ozone decrease is driven by iodine-catalyzed loss. The resulting GEOS-Chem ozone simulation is unbiased in the Southern Hemisphere but too low in the Northern Hemisphere.

scholarly journals The MOPITT Version 6 product: algorithm enhancements and validation

2014 ◽  
Vol 7 (11) ◽  
pp. 3623-3632 ◽  
Author(s):  
M. N. Deeter ◽  
S. Martínez-Alonso ◽  
D. P. Edwards ◽  
L. K. Emmons ◽  
J. C. Gille ◽  
...  
Keyword(s):  
Transport Model ◽  
A Priori ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Upper Troposphere ◽  
Community Atmosphere Model ◽  
Model Community ◽  
Modern Era ◽  
Retrieval Bias ◽  
Co Concentrations

Abstract. The Measurements of Pollution in the Troposphere (MOPITT) Version 6 (V6) product for carbon monoxide (CO) incorporates several enhancements which will benefit many users of MOPITT data. V6 algorithm improvements are described in detail, and V6 validation results are presented. First, a geolocation bias related to the orientation of the MOPITT instrument relative to the TERRA platform was characterized and eliminated. Second, the variable a priori for CO concentrations for V6 is based on simulations performed with the chemical transport model Community Atmosphere Model with Chemistry (CAM-chem) for the years 2000–2009 instead of the model-derived climatology for 1997–2004 used for V5. Third, meteorological fields required for V6 retrieval processing are extracted from the MERRA (Modern-Era Retrospective Analysis For Research And Applications) reanalysis. Finally, a significant latitude-dependent retrieval bias in the upper troposphere in Version 5 products has been substantially reduced.

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