scholarly journals First space-based observations of formic acid (HCOOH): Atmospheric Chemistry Experiment austral spring 2004 and 2005 Southern Hemisphere tropical-mid-latitude upper tropospheric measurements

2006 ◽  
Vol 33 (23) ◽  
Author(s):  
Curtis P. Rinsland ◽  
Chris D. Boone ◽  
Peter F. Bernath ◽  
Emmanuel Mahieu ◽  
Rodolphe Zander ◽  
...  
Keyword(s):  
Formic Acid ◽  
Southern Hemisphere ◽  
Atmospheric Chemistry ◽  
Austral Spring ◽  
Tropospheric Measurements ◽  
Chemistry Experiment

scholarly journals Global distribution of upper tropospheric formic acid from the ACE-FTS

2009 ◽  
Vol 9 (20) ◽  
pp. 8039-8047 ◽  
Author(s):  
G. González Abad ◽  
P. F. Bernath ◽  
C. D. Boone ◽  
S. D. McLeod ◽  
G. L. Manney ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Formic Acid ◽  
Atmospheric Chemistry ◽  
South American ◽  
Fourier Transform Spectrometer ◽  
Vegetation Growth ◽  
Solar Occultation ◽  
The Fourier Transform ◽  
Chemistry Experiment ◽  
Seasonal Dependence

Abstract. We present the first near global upper tropospheric distribution of formic acid (HCOOH) observed from space using solar occultation measurements from the Fourier transform spectrometer (FTS) on board the Atmospheric Chemistry Experiment (ACE) satellite. Using a new set of spectroscopic line parameters recently published for formic acid by Vander Auwera et al. (2007) and Perrin and Vander Auwera (2007), we have retrieved the concentrations of HCOOH between 5 km and the tropopause for ACE-FTS observations from February 2004 to September 2007. We observe a significant seasonal dependence for the HCOOH concentrations related to vegetation growth and biomass burning. We estimate an emission ratio of 0.0051±0.0015 for HCOOH relative to CO for tropical South American fires using a selected set of data for September 2004. Results from the balloon-borne MkIV Fourier transform spectrometer are also presented and compared with the ACE measurements.

scholarly journals Global distribution of upper tropospheric formic acid from the ACE-FTS

2009 ◽  
Vol 9 (3) ◽  
pp. 12465-12482
Author(s):  
G. González Abad ◽  
P. F. Bernath ◽  
C. D. Boone ◽  
S. D. McLeod ◽  
G. L. Manney ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Formic Acid ◽  
Atmospheric Chemistry ◽  
South American ◽  
Fourier Transform Spectrometer ◽  
Vegetation Growth ◽  
Solar Occultation ◽  
The Fourier Transform ◽  
Chemistry Experiment ◽  
Seasonal Dependence

Abstract. We present the first near global upper tropospheric distribution of formic acid (HCOOH) observed from the space using solar occultation measurements from the Fourier transform spectrometer (FTS) on board the Atmospheric Chemistry Experiment (ACE) satellite. Using a new set of spectroscopic line parameters recently published for formic acid, we have retrieved the concentrations of HCOOH between 5 km and the tropopause for ACE-FTS observations from February 2004 to September 2007. We observe a significant seasonal dependence for the HCOOH concentrations related to vegetation growth and biomass burning. We estimate an emission ratio of 0.0051±0.0015 for HCOOH relative to CO for tropical South American fires using a selected set of data for September 2004. Results from the balloon-borne MkIV Fourier transform spectrometer are also presented and used to validate the ACE measurements.

scholarly journals Global stratospheric chlorine inventories for 2004–2009 from Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements

2013 ◽  
Vol 13 (9) ◽  
pp. 23491-23548 ◽  
Author(s):  
A. T. Brown ◽  
M. P. Chipperfield ◽  
S. Dhomse ◽  
C. Boone ◽  
P. F. Bernath
Keyword(s):  
Southern Hemisphere ◽  
Northern Hemisphere ◽  
Atmospheric Chemistry ◽  
Transport Model ◽  
Montreal Protocol ◽  
Chemical Transport Model ◽  
Mixing Ratios ◽  
Ozone Depleting Substances ◽  
The Tropics ◽  
Chemistry Experiment

Abstract. We present chlorine budgets calculated between 2004 and 2009 for four latitude bands (70° N–30° N, 30° N–0° N, 0° N–30° S, and 30° S–70° S). The budgets were calculated using ACE-FTS version 3.0 retrievals of the volume mixing ratios (VMRs) of 9 chlorine-containing species: CCl4, CFC-12 (CCl2F2), CFC-11 (CCl3F), COCl2, COClF, HCFC-22 (CHF2Cl), CH3Cl, HCl and ClONO2. These data were supplemented with calculated VMRs from the SLIMCAT 3-D chemical transport model (CFC-113, CFC-114, CFC-115, H-1211, H-1301, HCFC-141b, HCFC-142b, ClO and HOCl). The total chlorine profiles are dominated by chlorofluorocarbons (CFCs) and halons up to 24 km in the tropics and 19 km in the extra-tropics. In this altitude range CFCs and halons account for 58% of the total chlorine VMR. Above this altitude HCl increasingly dominates the total chlorine profile, reaching a maximum of 95% of total chlorine at 54 km. All total chlorine profiles exhibit a positive slope with altitude, suggesting that the total chlorine VMR is now decreasing with time. This conclusion is supported by the time series of the mean stratospheric total chlorine budgets which show mean decreases in total stratospheric chlorine of 0.38 ± 0.03% per year in the Northern Hemisphere extra-tropics, 0.35 ± 0.07% per year in the Northern Hemisphere tropical stratosphere, 0.54 ± 0.16% per year in the Southern Hemisphere tropics and 0.53 ± 0.12% per year in the Southern Hemisphere extra-tropical stratosphere for 2004–2009. Globally stratospheric chlorine is decreasing by 0.46 ± 0.02% per year. Both global warming potential-weighted chlorine and ozone depletion potential-weighted chlorine are decreasing at all latitudes. These results show that the Montreal Protocol has had a significant effect in reducing emissions of both ozone-depleting substances and greenhouse gases.

scholarly journals The high Arctic in extreme winters: vortex, temperature, and MLS and ACE-FTS trace gas evolution

2008 ◽  
Vol 8 (3) ◽  
pp. 505-522 ◽  
Author(s):  
G. L. Manney ◽  
W. H. Daffer ◽  
K. B. Strawbridge ◽  
K. A. Walker ◽  
C. D. Boone ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
High Arctic ◽  
Trace Gas ◽  
Satellite Measurements ◽  
Broadband Emission ◽  
Gas Measurements ◽  
Chemistry Experiment ◽  
Very High ◽  
Good Agreement

Abstract. The first three Arctic winters of the ACE mission represented two extremes of winter variability: Stratospheric sudden warmings (SSWs) in 2004 and 2006 were among the strongest, most prolonged on record; 2005 was a record cold winter. Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Campaigns were conducted at Eureka (80° N, 86° W) during each of these winters. New satellite measurements from ACE-Fourier Transform Spectrometer (ACE-FTS), Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), and Aura Microwave Limb Sounder (MLS), along with meteorological analyses and Eureka lidar temperatures, are used to detail the meteorology in these winters, to demonstrate its influence on transport, and to provide a context for interpretation of ACE-FTS and validation campaign observations. During the 2004 and 2006 SSWs, the vortex broke down throughout the stratosphere, reformed quickly in the upper stratosphere, and remained weak in the middle and lower stratosphere. The stratopause reformed at very high altitude, near 75 km. ACE measurements covered both vortex and extra-vortex conditions in each winter, except in late-February through mid-March 2004 and 2006, when the strong, pole-centered vortex that reformed after the SSWs resulted in ACE sampling only inside the vortex in the middle through upper stratosphere. The 2004 and 2006 Eureka campaigns were during the recovery from the SSWs, with the redeveloping vortex over Eureka. 2005 was the coldest winter on record in the lower stratosphere, but with an early final warming in mid-March. The vortex was over Eureka at the start of the 2005 campaign, but moved away as it broke up. Disparate temperature profile structure and vortex evolution resulted in much lower (higher) temperatures in the upper (lower) stratosphere in 2004 and 2006 than in 2005. Satellite temperatures agree well with lidar data up to 50–60 km, and ACE-FTS, MLS and SABER show good agreement in high-latitude temperatures throughout the winters. Consistent with a strong, cold upper stratospheric vortex and enhanced radiative cooling after the SSWs, MLS and ACE-FTS trace gas measurements show strongly enhanced descent in the upper stratospheric vortex in late January through March 2006 compared to that in 2005.

scholarly journals Global stratospheric measurements of the isotopologues of methane from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer

2015 ◽  
Vol 8 (10) ◽  
pp. 11171-11207
Author(s):  
E. M. Buzan ◽  
C. A. Beale ◽  
C. D. Boone ◽  
P. F. Bernath
Keyword(s):  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Climate Model ◽  
Fourier Transform Spectrometer ◽  
Atmospheric Methane ◽  
Community Climate Model ◽  
Atmospheric Sinks ◽  
Chemistry Experiment ◽  
Methane Concentrations ◽  
Balloon Measurements

Abstract. This paper presents an analysis of observations of methane and its two major isotopologues, CH3D and 13CH4 from the Atmospheric Chemistry Experiment (ACE) satellite between 2004 and 2013. Additionally, atmospheric methane chemistry is modeled using the Whole Atmospheric Community Climate Model (WACCM). ACE retrievals of methane extend from 6 km for all isotopologues to 75 km for 12CH4, 35 km for CH3D, and 50 km for 13CH4. While total methane concentrations retrieved from ACE agree well with the model, values of δD–CH4 and δ13C–CH4 show a bias toward higher δ compared to the model and balloon-based measurements. Calibrating δD and δ13C from ACE using WACCM in the troposphere gives improved agreement in δD in the stratosphere with the balloon measurements, but values of δ13C still disagree. A model analysis of methane's atmospheric sinks is also performed.

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 Ethane, ethyne and carbon monoxide concentrations in the upper troposphere and lower stratosphere from ACE and GEOS-Chem: a comparison study

2011 ◽  
Vol 11 (4) ◽  
pp. 13099-13139 ◽  
Author(s):  
G. González Abad ◽  
N. D. C. Allen ◽  
P. F. Bernath ◽  
C. D. Boone ◽  
S. D. McLeod ◽  
...  
Keyword(s):  
Carbon Monoxide ◽  
Atmospheric Chemistry ◽  
Transport Model ◽  
Chemical Mechanism ◽  
Chemical Transport Model ◽  
Spectrometer Data ◽  
Chemistry Experiment ◽  
Global Mean ◽  
Tropospheric Concentrations ◽  
Good Agreement

Abstract. Near global upper tropospheric concentrations of carbon monoxide (CO), ethane (C2H6) and ethyne (C2H2) from ACE (Atmospheric Chemistry Experiment) Fourier transform spectrometer on board the Canadian satellite SCISAT-1 are presented and compared with the output from the Chemical Transport Model (CTM) GEOS-Chem. The retrievals of ethane and ethyne from ACE have been improved for this paper by using new sets of microwindows compared with those for previous versions of ACE data. With the improved ethyne retrieval we have been able to produce a near global upper tropospheric distribution of C2H2 from space. Carbon monoxide, ethane and ethyne concentrations retrieved using ACE spectra show the expected seasonality linked to variations in the anthropogenic emissions and destruction rates as well as seasonal biomass burning activity. The GEOS-Chem model was run using the dicarbonyl chemistry suite, an extended chemical mechanism in which ethyne is treated explicitly. Seasonal cycles observed from satellite data are well reproduced by the model output, however the simulated CO concentrations are found to be systematically biased low over the Northern Hemisphere. An average negative global mean bias of 12% and 7% of the model relative to the satellite observations has been found for CO and C2H6 respectively and a positive global mean bias of 1% has been found for C2H2. ACE data are compared for validation purposes with MkIV spectrometer data and Global Tropospheric Experiment (GTE) TRACE-A campaign data showing good agreement with all of them.

scholarly journals Sunset–sunrise difference in solar occultation ozone measurements (SAGE II, HALOE, and ACE–FTS) and its relationship to tidal vertical winds

2014 ◽  
Vol 14 (11) ◽  
pp. 16043-16083
Author(s):  
T. Sakazaki ◽  
M. Shiotani ◽  
M. Suzuki ◽  
D. Kinnison ◽  
J. M. Zawodny ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Seasonal Variations ◽  
Climate Model ◽  
Transport Model ◽  
Stratospheric Aerosol ◽  
Chemical Transport Model ◽  
Latitude Range ◽  
Solar Occultation ◽  
Vertical Winds ◽  
Chemistry Experiment

Abstract. This paper contains a comprehensive investigation of the sunset–sunrise difference (SSD; i.e., the sunset-minus-sunrise value) of the ozone mixing ratio in the latitude range of 10° S–10° N. SSD values were determined from solar occultation measurements based on data obtained from the Stratospheric Aerosol and Gas Experiment (SAGE) II, the Halogen Occultation Experiment (HALOE), and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The SSD was negative at altitudes of 20–30 km (–0.1 ppmv at 25 km) and positive at 30–50 km (+0.2 ppmv at 40–45 km) for HALOE and ACE–FTS data. SAGE II data also showed a qualitatively similar result, although the SSD in the upper stratosphere was two times larger than those derived from the other datasets. On the basis of an analysis of data from the Superconducting Submillimeter Limb Emission Sounder (SMILES), and a nudged chemical-transport model (the Specified Dynamics version of the Whole Atmosphere Community Climate Model: SD–WACCM), we conclude that the SSD can be explained by diurnal variations in the ozone concentration, particularly those caused by vertical transport by the atmospheric tidal winds. All datasets showed significant seasonal variations in the SSD; the SSD in the upper stratosphere is greatest from December through February, while that in the lower stratosphere reaches a maximum twice: during the periods March–April and September–October. Based on an analysis of SD–WACCM results, we found that these seasonal variations follow those associated with the tidal vertical winds.

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