scholarly journals New approach to evaluate satellite-derived XCO<sub>2</sub> over oceans by integrating ship and aircraft observations

2021 ◽  
Vol 21 (10) ◽  
pp. 8255-8271
Author(s):  
Astrid Müller ◽  
Hiroshi Tanimoto ◽  
Takafumi Sugita ◽  
Toshinobu Machida ◽  
Shin-ichiro Nakaoka ◽  
...  
Keyword(s):  
Carbon Cycle ◽  
Atmospheric Chemistry ◽  
Transport Model ◽  
Satellite Observations ◽  
Reference Dataset ◽  
Commercial Aircraft ◽  
Model Calculations ◽  
New Approach ◽  
Mixing Ratios ◽  
Spatially Resolved

Abstract. Satellite observations provide spatially resolved global estimates of column-averaged mixing ratios of CO2 (XCO2) over the Earth's surface. The accuracy of these datasets can be validated against reliable standards in some areas, but other areas remain inaccessible. To date, limited reference data over oceans hinder successful uncertainty quantification or bias correction efforts and preclude reliable conclusions about changes in the carbon cycle in some regions. Here, we propose a new approach to analyze and evaluate seasonal, interannual, and latitudinal variations of XCO2 over oceans by integrating cargo-ship (Ship Of Opportunity – SOOP) and commercial aircraft (Comprehensive Observation Network for Trace gases by Airliner – CONTRAIL) observations with the aid of state-of-the art atmospheric chemistry-transport model calculations. The consistency of the “observation-based column-averaged CO2” dataset (obs. XCO2) with satellite estimates was analyzed over the western Pacific between 2014 and 2017, and its utility as a reference dataset evaluated. Our results demonstrate that the new dataset accurately captures seasonal and interannual variations of CO2. Retrievals of XCO2 over the ocean from GOSAT (Greenhouse Gases Observing Satellite: National Institute for Environmental Studies – NIES v02.75; Atmospheric CO2 Observation from Space – ACOS v7.3) and OCO-2 (Orbiting Carbon Observatory, v9r) observations show a negative bias of about 1 part per million (ppm) in northern midlatitudes, which was attributed to measurement uncertainties of the satellite observations. The NIES retrieval had higher consistency with obs. XCO2 at midlatitudes as compared to the other retrievals. At low latitudes, it shows many fewer valid data and high scatter, such that ACOS and OCO-2 appear to provide a better representation of the carbon cycle. At different times, the seasonal cycles of all three retrievals show positive phase shifts of 1 month relative to the observation-based data. The study indicates that even if the retrievals complement each other, remaining uncertainties limit the accurate interpretation of spatiotemporal changes in CO2 fluxes. A continuous long-term XCO2 dataset with wide latitudinal coverage based on the new approach has great potential as a robust reference dataset for XCO2 and can help to better understand changes in the carbon cycle in response to climate change using satellite observations.

scholarly journals New approach to evaluate satellite derived XCO<sub>2</sub> over oceans by integrating ship and aircraft observations

2020 ◽  
Author(s):  
Astrid Müller ◽  
Hiroshi Tanimoto ◽  
Takafumi Sugita ◽  
Toshinobu Machida ◽  
Shin-ichiro Nakaoka ◽  
...  
Keyword(s):  
Carbon Cycle ◽  
Atmospheric Chemistry ◽  
Transport Model ◽  
Satellite Observations ◽  
Reference Dataset ◽  
Model Calculations ◽  
New Approach ◽  
Mixing Ratios ◽  
In Situ Data

Abstract. Satellite observations provide spatially-resolved global estimates of column-averaged mixing ratios of CO2 (XCO2) over the Earth's surface. The accuracy of these datasets can be validated against reliable standards in some areas, but other areas remain inaccessible. To date, limited reference data over oceans hinders successful uncertainty quantification or bias correction efforts, and precludes reliable conclusions about changes in the carbon cycle in some regions. Here, we propose a new approach to analyze and evaluate seasonal, interannual and latitudinal variations of XCO2 over oceans by integrating cargo-ship (SOOP, Ship Of Opportunity) and commercial aircraft (CONTRAIL, Comprehensive Observation Network for Trace gases by Airliner) observations with the aid of state-of-the art atmospheric chemistry-transport model calculations. The consistency of the in situ based column-averaged CO2 dataset (in situ XCO2) with satellite estimates was analyzed over the Western Pacific between 2014 and 2017, and its utility as reference dataset evaluated. Our results demonstrate that the new dataset accurately captures seasonal and interannual variations of CO2. Retrievals of XCO2 over the ocean from GOSAT (Greenhouse gases observing satellite: NIES v02.75, National Institute for Environmental Studies; ACOS v7.3, Atmospheric CO2 Observation from Space) and OCO-2 (Orbiting Carbon Observatory, v9r) observations show a negative bias of about 1 parts per million (ppm) in northern midlatitudes, which was attributed to measurement uncertainties of the satellite observations. The NIES retrieval had higher consistency with in situ XCO2 at midlatitudes as compared to the other retrievals. At low latitudes, it shows many fewer valid data and high scatter, such that ACOS and OCO-2 appear to provide a better representation of the carbon cycle. At different times, the seasonal cycles of all three retrievals show positive phase shifts of one month relative to the in situ data. The study indicates that even if the retrievals complement each other, remaining uncertainties limit the accurate interpretation of spatiotemporal changes in CO2 fluxes. A continuous long-term XCO2 dataset with wide latitudinal coverage based on the new approach has a great potential as a robust reference dataset for XCO2 and can help to better understand changes in the carbon cycle in response to climate change using satellite observations.

scholarly journals Diurnal variation of stratospheric and lower mesospheric HOCl, ClO and HO<sub>2</sub> at the equator: comparison of 1-D model calculations with measurements by satellite instruments

2013 ◽  
Vol 13 (15) ◽  
pp. 7587-7606 ◽  
Author(s):  
M. Khosravi ◽  
P. Baron ◽  
J. Urban ◽  
L. Froidevaux ◽  
A. I. Jonsson ◽  
...  
Keyword(s):  
Diurnal Variation ◽  
Atmospheric Chemistry ◽  
Michelson Interferometer ◽  
Space Station ◽  
Satellite Observations ◽  
Local Times ◽  
Night Time ◽  
Model Calculations ◽  
Mixing Ratios ◽  
Variable Species

Abstract. The diurnal variation of HOCl and the related species ClO, HO2 and HCl measured by satellites has been compared with the results of a one-dimensional photochemical model. The study compares the data from various limb-viewing instruments with model simulations from the middle stratosphere to the lower mesosphere. Data from three sub-millimetre instruments and two infrared spectrometers are used, namely from the Sub-Millimetre Radiometer (SMR) on board Odin, the Microwave Limb Sounder (MLS) on board Aura, the Superconducting Submillimeter-wave Limb-Emission Sounder (SMILES) on the International Space Station, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board ENVISAT, and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on board SCISAT. Inter-comparison of the measurements from instruments on sun-synchronous satellites (SMR, MLS, MIPAS) and measurements from solar occultation instruments (ACE-FTS) is challenging since the measurements correspond to different solar zenith angles (or local times). However, using a model which covers all solar zenith angles and data from the SMILES instrument which measured at all local times over a period of several months provides the possibility to verify the model and to indirectly compare the diurnally variable species. The satellite data were averaged for latitudes of 20° S to 20° N for the SMILES observation period from November 2009 to April 2010 and were compared at three altitudes: 35, 45 and 55 km. Besides presenting the SMILES data, the study also shows a first comparison of the latest MLS data (version 3.3) of HOCl, ClO, and HO2 with other satellite observations, as well as a first evaluation of HO2 observations made by Odin/SMR. The MISU-1D model has been carefully initialised and run for conditions and locations of the observations. The diurnal cycle features for the species investigated here are generally well reproduced by the model. The satellite observations and the model agree well in terms of absolute mixing ratios. The differences between the day and night values of the model are in good agreement with the observations although the amplitude of the HO2 diurnal variation is 10–20% lower in the model than in the observations. In particular, the data offered the opportunity to study the reaction ClO+HO2 → HOCl+O2 in the lower mesosphere at 55 km. At this altitude the HOCl night-time variation depends only on this reaction. The result of this analysis points towards a value of the rate constant within the range of the JPL 2006 recommendation and the upper uncertainty limit of the JPL 2011 recommendation at 55 km.

scholarly journals Diurnal variation of stratospheric HOCl, ClO and HO<sub>2</sub> at the equator: comparison of 1-D model calculations with measurements of satellite instruments

2012 ◽  
Vol 12 (8) ◽  
pp. 21065-21104 ◽  
Author(s):  
M. Khosravi ◽  
P. Baron ◽  
J. Urban ◽  
L. Froidevaux ◽  
A. I. Jonsson ◽  
...  
Keyword(s):  
Diurnal Variation ◽  
Atmospheric Chemistry ◽  
Michelson Interferometer ◽  
Space Station ◽  
Satellite Observations ◽  
Local Times ◽  
Model Calculations ◽  
Reaction Rate Constants ◽  
Mixing Ratios ◽  
Variable Species

Abstract. The diurnal variation of HOCl and the related species ClO, HO2 and HCl measured by satellites has been compared with the results of a one-dimensional photochemical model. The study compares the data from various limb-viewing instruments with model simulations from the middle stratosphere to the lower mesosphere. Data from three sub-millimeter instruments and two infrared spectrometers are used, namely from the Sub-Millimeter Radiometer (SMR) on board Odin, the Microwave Limb Sounder (MLS) on board Aura, the Superconducting Submillimeter-wave Limb-Emission Sounder (SMILES) on the International Space Station, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board ENVISAT, and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on board SCISAT. Inter-comparison of the measurements from instruments on sun-synchronous satellites (SMR, MLS, MIPAS) and measurements from solar occultation instruments (ACE-FTS) is challenging since the measurements correspond to different solar zenith angles (or local times). However, using a model which covers all solar zenith angles and the new SMILES instrument which measures at all local times over a period of several months provides the possibility to indirectly compare the diurnally variable species. The satellite data were averaged for latitudes of 20° S to 20° N for the SMILES observation period from November 2009 to April 2010 and were compared at three altitudes: 35, 45 and 55 km. This study presents the first evaluation of HO2 Odin/SMR data and also the first comparison of the new SMILES data and the latest version of MLS (version 3.3) with other satellite observations. The MISU-1D model has been run for conditions and locations of the observations. The diurnal cycle features for the species investigated here are generally well reproduced by the model. The satellite observations and the model generally agree well in terms of absolute mixing ratios as well as differences between the day and night values. This confirms that gas phase chemistry of these species based on latest recommendations of reaction rate constants is fairly well understood.

scholarly journals Impact of reactive bromine chemistry in the troposphere

2004 ◽  
Vol 4 (4) ◽  
pp. 4877-4913 ◽  
Author(s):  
R. von Glasow ◽  
R. von Kuhlmann ◽  
M. G. Lawrence ◽  
U. Platt ◽  
P. J. Crutzen
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Changes ◽  
Dimethyl Sulfide ◽  
Transport Model ◽  
Satellite Observations ◽  
Mixing Ratio ◽  
Chemistry Transport Model ◽  
Bromine Oxide ◽  
Mixing Ratios ◽  
Field Campaigns

Abstract. Recently several field campaigns and satellite observations found strong indications for bromine oxide (BrO) in the free troposphere. Using a global atmospheric chemistry transport model we show that BrO measurements mixing ratios of a few tenths to 2 pmol mol−1 lead to a reduction in the zonal mean O3 mixing ratio of up to 18% in widespread areas and locally even up to 40% compared to a model run without bromine chemistry. For dimethyl sulfide (DMS) the effect is even larger with up to 60% decreases. This is accompanied by dramatic changes in DMS oxidation pathways, reducing its cooling effect on climate. Changes in the HO2:OH ratio also cause changes for NOx and PAN. These results imply that a very strong sink for O3 and DMS has so far been ignored in many studies of the chemistry of the troposphere.

scholarly journals Structural changes in the shallow and transition branch of the Brewer–Dobson circulation induced by El Niño

2018 ◽  
Author(s):  
Mohamadou Diallo ◽  
Paul Konopka ◽  
Michelle L. Santee ◽  
Rolf Müller ◽  
Mengchu Tao ◽  
...  
Keyword(s):  
El Niño ◽  
Structural Changes ◽  
Lower Stratosphere ◽  
Transport Model ◽  
El Nino ◽  
Southern Oscillation ◽  
Satellite Observations ◽  
Trace Gas ◽  
Residual Circulation ◽  
Mixing Ratios

Abstract. The stratospheric Brewer–Dobson circulation (BD-circulation) determines the transport and lifetime of key radiatively active trace gases and further impacts surface climate through downward coupling. Here, we quantify the variability in the lower stratospheric BD-circulation induced by the El Nino Southern Oscillation (ENSO), using satellite trace gas measurements and simulations with the Lagrangian chemistry transport model, CLaMS, driven by ERA-Interim and JRA-55 reanalyses. We show that despite discrepancies in the deseasonalised ozone (O3) mixing ratios between CLaMS simulations and satellite observations, the patterns of changes in the lower stratospheric O3 anomalies induced by ENSO agree remarkably well over the 2005–2016 period. Particularly during the most recent El Niño in 2015–2016, both satellite observations and CLaMS simulations show the largest negative tropical O3 anomaly in the record. Regression analysis of different metrics of the BD-circulation strength, including mean age of air, vertical velocity, residual circulation and age spectrum, shows clear evidence for structural changes of the BD-circulation in the lower stratosphere induced by El Niño, consistent with observed O3 anomalies. These structural changes during El Niño include a weakening of the transition branch of the BD-circulation between about 370–420 K (∼ 100–70 hPa) and equatorward of about 60° and, a strengthening of the shallow branch at the same latitudes and between about 420–500 K (∼ 70–30 hPa). The strengthening of the shallow branch induces negative tropical O3 anomalies due to enhanced tropical upwelling, while the weakening of the transition branch combined with enhanced downwelling due to the strengthening shallow branch leads to positive O3 anomalies in the extratropical upper troposphere-lower stratosphere (UTLS). Our results suggest that a shift of the ENSO basic state toward more frequent El Niño-like conditions in a warming future climate will substantially alter UTLS trace gas distributions due to these changes in the vertical structure of the stratospheric circulation.

scholarly journals Global stratospheric fluorine inventory for 2004–2009 from Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements and SLIMCAT model simulations

2014 ◽  
Vol 14 (1) ◽  
pp. 267-282 ◽  
Author(s):  
A. T. Brown ◽  
M. P. Chipperfield ◽  
N. A. D. Richards ◽  
C. Boone ◽  
P. F. Bernath
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Transport Model ◽  
Similar Rate ◽  
Montreal Protocol ◽  
Negative Slope ◽  
Mixing Ratios ◽  
Inorganic Species ◽  
The Tropics ◽  
The Impact

Abstract. Fluorine-containing species can be extremely effective atmospheric greenhouse gases. We present fluorine budgets using organic and inorganic species retrieved by the ACE-FTS satellite instrument supplemented with output from the SLIMCAT 3-D chemical transport model. The budgets are calculated between 2004 and 2009 for a number of latitude bands: 70–30° N, 30–00° N, 00° N–30° S, and 30–70° S. At lower altitudes total fluorine profiles are dominated by the contribution from CFC-12, up to an altitude of 20 km in the extra-tropics and 29 km in the tropics; above these altitudes the profiles are dominated by hydrogen fluoride (HF). Our data show that total fluorine profiles at all locations have a negative slope with altitude, providing evidence that overall fluorine emissions (measured by their F content) have been increasing with time. Total stratospheric fluorine is increasing at a similar rate in the tropics: 32.5 ± 4.9 ppt yr−1 (1.31 ± 0.20% per year) in the Northern Hemisphere (NH) and 29.8 ± 5.3 ppt yr−1 (1.21 ± 0.22% per year) in the Southern Hemisphere (SH). Extra-tropical total stratospheric fluorine is also increasing at a similar rate in both the NH and SH: 28.3 ± 2.7 ppt per year (1.12 ± 0.11% per year) in the NH and 24.3 ± 3.1 ppt per year (0.96 ± 0.12% per year) in the SH. The calculation of radiative efficiency-weighted total fluorine allows the changes in radiative forcing between 2004 and 2009 to be calculated. These results show an increase in radiative forcing of between 0.23 ± 0.11% per year and 0.45 ± 0.11% per year, due to the increase in fluorine-containing species during this time. The decreasing trends in the mixing ratios of halons and chlorofluorocarbons (CFCs), due to their prohibition under the Montreal Protocol, have suppressed an increase in total fluorine caused by increasing mixing ratios of hydrofluorocarbons (HFCs). This has reduced the impact of fluorine-containing species on global warming.

scholarly journals Which processes drive observed variations of HCHO columns over India?

2018 ◽  
Vol 18 (7) ◽  
pp. 4549-4566 ◽  
Author(s):  
Luke Surl ◽  
Paul I. Palmer ◽  
Gonzalo González Abad
Keyword(s):  
Atmospheric Chemistry ◽  
Seasonal Cycle ◽  
Transport Model ◽  
Monsoon Season ◽  
Gangetic Plain ◽  
Model Calculations ◽  
Propene Oxidation ◽  
Meridional Gradient ◽  
Northeastern India ◽  
Continental Scale

Abstract. We interpret HCHO column variations observed by the Ozone Monitoring Instrument (OMI), aboard the NASA Aura satellite, over India during 2014 using the GEOS-Chem atmospheric chemistry and transport model. We use a nested version of the model with a horizontal resolution of approximately 25 km. HCHO columns are related to local emissions of volatile organic compounds (VOCs) with a spatial smearing that increases with the VOC lifetime. Over India, HCHO has biogenic, pyrogenic, and anthropogenic VOC sources. Using a 0-D photochemistry model, we find that isoprene has the largest molar yield of HCHO which is typically realized within a few hours. We also find that forested regions that neighbour major urban conurbations are exposed to high levels of nitrogen oxides. This results in depleted hydroxyl radical concentrations and a delay in the production of HCHO from isoprene oxidation. We find that propene is the only anthropogenic VOC emitted in major Indian cities that produces HCHO at a comparable (but slower) rate to isoprene. The GEOS-Chem model reproduces the broad-scale annual mean HCHO column distribution observed by OMI (r = 0.6), which is dominated by a distinctive meridional gradient in the northern half of the country, and by localized regions of high columns that coincide with forests. Major discrepancies are noted over the Indo-Gangetic Plain (IGP) and Delhi. We find that the model has more skill at reproducing observations during winter (JF) and pre-monsoon (MAM) months with Pearson correlations r > 0.5 but with a positive model bias of  ≃ 1×1015 molec cm−2. During the monsoon season (JJAS) we reproduce only a diffuse version of the observed meridional gradient (r = 0.4). We find that on a continental scale most of the HCHO column seasonal cycle is explained by monthly variations in surface temperature (r = 0.9), suggesting a role for biogenic VOCs, in agreement with the 0-D and GEOS-Chem model calculations. We also find that the seasonal cycle during 2014 is not significantly different from the 2008 to 2015 mean seasonal variation. There are two main loci for biomass burning (the states of Punjab and Haryana, and northeastern India), which we find makes a significant contribution (up to 1×1015 molec cm−2) to observed HCHO columns only during March and April over northeastern India. The slow production of HCHO from propene oxidation results in a smeared hotspot over Delhi that we resolve only on an annual mean timescale by using a temporal oversampling method. Using a linear regression model to relate GEOS-Chem isoprene emissions to HCHO columns we infer seasonal isoprene emissions over two key forest regions from the OMI HCHO column data. We find that the a posteriori emissions are typically lower than the a priori emissions, with a much stronger reduction of emissions during the monsoon season. We find that this reduction in emissions during monsoon months coincides with a large drop in satellite observations of leaf phenology that recovers in post monsoon months. This may signal a forest-scale response to monsoon conditions.

scholarly journals Which processes drive observed variations of HCHO columns over India?

2017 ◽  
Author(s):  
Luke Surl ◽  
Paul I. Palmer ◽  
Gonzalo González Abad
Keyword(s):  
Atmospheric Chemistry ◽  
Seasonal Cycle ◽  
Transport Model ◽  
Monsoon Season ◽  
Gangetic Plain ◽  
Model Calculations ◽  
Propene Oxidation ◽  
Meridional Gradient ◽  
Northeastern India ◽  
Continental Scale

Abstract. We interpret HCHO column variations observed by the Ozone Monitoring Instrument (OMI), aboard the NASA Aura satellite, over India during 2014 using the GEOS-Chem atmospheric chemistry and transport model. We use a nested version of the model with a spatial resolution of approximately 25 km. HCHO columns are related to local emissions of volatile organic compounds (VOCs) with a spatial smearing that increases with the VOC lifetime. Over India, HCHO has biogenic, pyrogenic, and anthropogenic VOC sources. Using a 0-D photochemistry model, we find that isoprene has the largest molar yield of HCHO that is typically realized within a few hours. We find that forested regions that neighbours major urban conurbations are exposed to high levels of nitrogen oxides. This results in depleted hydroxyl radical concentrations and a delay in the production of HCHO from isoprene oxidation. We find that propene is the only anthropogenic VOC emitted in major Indian cities that produces HCHO at a comparable (slower) rate to isoprene. The GEOS-Chem model reproduces the broadscale annual mean HCHO column distribution observed by OMI (r = 0.6), which is dominated by a distinctive meridional gradient in the northern half of the country, and by localized regions of high columns that coincide with forests. Major discrepancies are over the Indo-Gangetic Plain and Delhi. We find that the model has more skill at reproducing observations during winter (JF) and pre-monsoon (MAM) months with Pearson correlations r > 0.5 but with a positive model bias of 1 × 1015 molec/cm2. During the monsoon season (JJAS) we reproduce only a diffuse version of the observed meridional gradient (r = 0.4). Generally, we find that on a continental scale most of the seasonal cycle is explained by monthly variations in surface temperature (r = 0.9), suggesting a strong role for biogenic VOCs, in agreement with the 0-D and GEOS-Chem model calculations. We also find that the seasonal cycle during 2014 is not significantly different from the 2008–2015 mean seasonal variation but there are large year to year variations. There are two main loci for biomass burning (states of Punjab and Haryana, and northeastern India), which we find only contributes a significant contribution (up to 1 × 1015 molec/cm2) to observed HCHO columns during March to April over northeastern India. The slow production of HCHO from propene oxidation results in a smeared hotspot over Delhi that we resolve only on an annual mean timescale by using a temporal oversampling method. Using a linear regression model to relate GEOS-Chem isoprene emissions to HCHO columns we infer seasonal isoprene emissions over two key forest regions from the OMI HCHO column data. We find that the a posteriori emissions are typically lower than the a priori emissions, with a much stronger reduction of emissions during the monsoon season. We find that this reduction in emissions during monsoon months coincides with a large drop in satellite observations of leaf phenology that recovers in post monsoon months. This may signal a forest-scale response to monsoon conditions.

scholarly journals Stratospheric lifetime ratio of CFC-11 and CFC-12 from satellite and model climatologies

2014 ◽  
Vol 14 (11) ◽  
pp. 16865-16906 ◽  
Author(s):  
L. Hoffmann ◽  
C. M. Hoppe ◽  
R. Müller ◽  
G. S. Dutton ◽  
J. C. Gille ◽  
...  
Keyword(s):  
Global Warming ◽  
Atmospheric Chemistry ◽  
Climate Model ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Michelson Interferometer ◽  
Coupled Model ◽  
Model System ◽  
Satellite Observations ◽  
The Impact

Abstract. Chlorofluorocarbons (CFCs) play a key role in stratospheric ozone loss and are strong infrared absorbers that contribute to global warming. The stratospheric lifetimes of CFCs are a measure of their global loss rates that are needed to determine global warming and ozone depletion potentials. We applied the tracer-tracer correlation approach to zonal mean climatologies from satellite measurements and model data to assess the lifetimes of CFCl3 (CFC-11) and CF2Cl2 (CFC-12). We present estimates of the CFC-11/CFC-12 lifetime ratio and the absolute lifetime of CFC-12, based on a reference lifetime of 52 yr for CFC-11. We analyzed climatologies from three satellite missions, the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS), the HIgh Resolution Dynamics Limb Sounder (HIRDLS), and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). We found a CFC-11/CFC-12 lifetime ratio of 0.47±0.08 and a CFC-12 lifetime of 111(96–132) yr for ACE-FTS, a ratio of 0.46±0.07 and a lifetime of 112(97–133) yr for HIRDLS, and a ratio of 0.46±0.08 and a lifetime of 112(96–135) yr for MIPAS. The error-weighted, combined CFC-11/CFC-12 lifetime ratio is 0.47±0.04 and the CFC-12 lifetime estimate is 112(102–123) yr. These results agree with the recent Stratosphere-troposphere Processes And their Role in Climate (SPARC) reassessment, which recommends lifetimes of 52(43–67) yr and 102(88–122) yr, respectively. Having smaller uncertainties than the results from other recent studies, our estimates can help to better constrain CFC-11 and CFC-12 lifetime recommendations in future scientific studies and assessments. Furthermore, the satellite observations were used to validate first simulation results from a new coupled model system, which integrates a Lagrangian chemistry transport model into a climate model. For the coupled model we found a CFC-11/CFC-12 lifetime ratio of 0.48±0.07 and a CFC-12 lifetime of 110(95–129) yr, based on a ten-year perpetual run. Closely reproducing the satellite observations, the new model system will likely become a useful tool to assess the impact of advective transport, mixing, and photochemistry as well as climatological variability on the stratospheric lifetimes of long-lived tracers.

scholarly journals Development of the global atmospheric chemistry general circulation model BCC-GEOS-Chem v1.0: model description and evaluation

2020 ◽  
Vol 13 (9) ◽  
pp. 3817-3838
Author(s):  
Xiao Lu ◽  
Lin Zhang ◽  
Tongwen Wu ◽  
Michael S. Long ◽  
Jun Wang ◽  
...  
Keyword(s):  
General Circulation Model ◽  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
General Circulation ◽  
Climate Models ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Circulation Model ◽  
Satellite Observations ◽  
Model Description

Abstract. Chemistry plays an indispensable role in investigations of the atmosphere; however, many climate models either ignore or greatly simplify atmospheric chemistry, limiting both their accuracy and their scope. We present the development and evaluation of the online global atmospheric chemical model BCC-GEOS-Chem v1.0, coupling the GEOS-Chem chemical transport model (CTM) as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model (BCC-AGCM). The GEOS-Chem atmospheric chemistry component includes detailed tropospheric HOx–NOx–volatile organic compounds–ozone–bromine–aerosol chemistry and online dry and wet deposition schemes. We then demonstrate the new capabilities of BCC-GEOS-Chem v1.0 relative to the base BCC-AGCM model through a 3-year (2012–2014) simulation with anthropogenic emissions from the Community Emissions Data System (CEDS) used in the Coupled Model Intercomparison Project Phase 6 (CMIP6). The model captures well the spatial distributions and seasonal variations in tropospheric ozone, with seasonal mean biases of 0.4–2.2 ppbv at 700–400 hPa compared to satellite observations and within 10 ppbv at the surface to 500 hPa compared to global ozonesonde observations. The model has larger high-ozone biases over the tropics which we attribute to an overestimate of ozone chemical production. It underestimates ozone in the upper troposphere which is likely due either to the use of a simplified stratospheric ozone scheme or to biases in estimated stratosphere–troposphere exchange dynamics. The model diagnoses the global tropospheric ozone burden, OH concentration, and methane chemical lifetime to be 336 Tg, 1.16×106 molecule cm−3, and 8.3 years, respectively, which is consistent with recent multimodel assessments. The spatiotemporal distributions of NO2, CO, SO2, CH2O, and aerosol optical depth are generally in agreement with satellite observations. The development of BCC-GEOS-Chem v1.0 represents an important step for the development of fully coupled earth system models (ESMs) in China.

Sign in / Sign up

Export Citation Format

Share Document