scholarly journals First carbon dioxide atmospheric vertical profiles retrieved from space observation using ACE-FTS solar occultation instrument

2010 ◽  
Vol 10 (11) ◽  
pp. 26473-26512
Author(s):  
P. Y. Foucher ◽  
A. Chédin ◽  
R. Armante ◽  
C. Boone ◽  
C. Crevoisier ◽  
...  

Abstract. Major limitations of our present knowledge of the global distribution of CO2 in the atmosphere are the uncertainty in atmospheric transport and the sparseness of in situ concentration measurements. Limb viewing spaceborne sounders such as the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) offer a vertical resolution of a few kilometres for profiles, which is much better than currently flying or planned nadir sounding instruments can achieve. After having demonstrated the feasibility of obtaining CO2 vertical profiles in the 5–25 km altitude range with an accuracy of about 2 ppm in a previous study, we present here the results of five years of ACE-FTS observations in terms of monthly mean profiles of CO2 averaged over 10° latitude bands for northern mid-latitudes. These results are compared with in-situ aircraft measurements and with simulations from two different air transport models. Key features of the measured altitude distribution of CO2 are shown to be accurately reproduced by the ACE-FTS retrievals: variation in altitude of the seasonal cycle amplitude and extrema, seasonal change of the vertical gradient, and mean growth rate. We show that small but significant differences from model simulations could result from an over estimation of the model circulation strength during the northern hemisphere spring. Coupled with column measurements from a nadir viewing instrument, it is expected that occultation measurements will bring useful constraints to the surface carbon flux determination.

2011 ◽  
Vol 11 (6) ◽  
pp. 2455-2470 ◽  
Author(s):  
P. Y. Foucher ◽  
A. Chédin ◽  
R. Armante ◽  
C. Boone ◽  
C. Crevoisier ◽  
...  

Abstract. Major limitations of our present knowledge of the global distribution of CO2 in the atmosphere are the uncertainty in atmospheric transport and the sparseness of in situ concentration measurements. Limb viewing spaceborne sounders such as the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) offer a vertical resolution of a few kilometres for profiles, which is much better than currently flying or planned nadir sounding instruments can achieve. After having demonstrated the feasibility of obtaining CO2 vertical profiles in the 5–25 km altitude range with an accuracy of about 2 ppm in a previous study, we present here the results of five years of ACE-FTS observations in terms of monthly mean profiles of CO2 averaged over 10° latitude bands for northern mid-latitudes. These results are compared with in-situ aircraft measurements and with simulations from two different air transport models. Key features of the measured altitude distribution of CO2 are shown to be accurately reproduced by the ACE-FTS retrievals: variation in altitude of the seasonal cycle amplitude and extrema, seasonal change of the vertical gradient, and mean growth rate. We show that small but significant differences from model simulations could result from an over estimation of the model circulation strength during the northern hemisphere spring. Coupled with column measurements from a nadir viewing instrument, it is expected that occultation measurements will bring useful constraints to the surface carbon flux determination.


2009 ◽  
Vol 9 (19) ◽  
pp. 7449-7459 ◽  
Author(s):  
N. D. C. Allen ◽  
P. F. Bernath ◽  
C. D. Boone ◽  
M. P. Chipperfield ◽  
D. Fu ◽  
...  

Abstract. The first study of the global atmospheric distribution of carbon tetrachloride (CCl4), as a function of altitude and latitude, was performed using solar occultation measurements obtained by the Atmospheric Chemistry Experiment (ACE) mission using Fourier transform spectroscopy. A total of 8703 profile measurements were taken in the upper troposphere and lower stratosphere between February 2004 and August 2007. The zonal distribution of carbon tetrachloride displays a slight hemispheric asymmetry and decreasing concentration with increasing altitude at all latitudes. Maximum carbon tetrachloride concentrations are situated below 10 km in altitude with VMR (Volume Mixing Ratio) values of 100–130 ppt (parts per trillion). The highest concentrations are located about the Equator and at mid-latitudes, particularly for latitudes in heavily industrialised regions (20–45° N), with values declining towards the poles. Global distributions obtained from ACE were compared with predictions from three chemistry transport models showing good agreement in terms of the vertical gradient despite an overall offset. The ACE dataset gives unique global and temporal coverage of carbon tetrachloride and its transport through the atmosphere. An estimated lifetime for carbon tetrachloride of 34±5 years was determined through correlation with CFC-11.


2009 ◽  
Vol 9 (8) ◽  
pp. 2873-2890 ◽  
Author(s):  
P. Y. Foucher ◽  
A. Chédin ◽  
G. Dufour ◽  
V. Capelle ◽  
C. D. Boone ◽  
...  

Abstract. Major limitations of our present knowledge of the global distribution of CO2 in the atmosphere are the uncertainty in atmospheric transport mixing and the sparseness of in situ concentration measurements. Limb viewing space-borne sounders, observing the atmosphere along tangential optical paths, offer a vertical resolution of a few kilometers for profiles, which is much better than currently flying or planned nadir sounding instruments can achieve. In this paper, we analyse the feasibility of obtaining CO2 vertical profiles in the 5–25 km altitude range from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS, launched in August 2003), high spectral resolution solar occultation measurements. Two main difficulties must be overcome: (i) the accurate determination of the instrument pointing parameters (tangent heights) and pressure/temperature profiles independently from an a priori CO2 profile, and (ii) the potential impact of uncertainties in the temperature knowledge on the retrieved CO2 profile. The first difficulty has been solved using the N2 collision-induced continuum absorption near 4 μm to determine tangent heights, pressure and temperature from the ACE-FTS spectra. The second difficulty has been solved by a careful selection of CO2 spectral micro-windows. Retrievals using synthetic spectra made under realistic simulation conditions show a vertical resolution close to 2.5 km and accuracy of the order of 2 ppm after averaging over 25 profiles. These results open the way to promising studies of transport mechanisms and carbon fluxes from the ACE-FTS measurements. First CO2 vertical profiles retrieved from real ACE-FTS occultations shown in this paper confirm the robustness of the method and applicability to real measurements.


2011 ◽  
Vol 11 (1) ◽  
pp. 1429-1455 ◽  
Author(s):  
S.-M. Salmi ◽  
P. T. Verronen ◽  
L. Thölix ◽  
E. Kyrölä ◽  
L. Backman ◽  
...  

Abstract. We use the 3-D FinROSE chemistry transport model (CTM) and ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations to study the connection between atmospheric dynamics and NOx descent during early 2009 in the northern polar region. We force the model NOx at 80 km poleward of 60° N with ACE-FTS observations and then compare the model results with observations at lower altitudes. Low geomagnetic indices indicate absence of local NOx production in early 2009, which gives a good opportunity to study the effects of atmospheric transport on polar NOx. No in-situ production of NOx by energetic particle precipitation is therefore included. This is the first model study using ECMWF (The European Centre for Medium-Range Weather Forecasts) data up to 80 km and simulating the exceptional winter of 2009 with one of the strongest major sudden stratospheric warmings (SSW). The model results show a strong NOx descent in February–March 2009 from the upper mesosphere to the stratosphere after the major SSW. Both observations and model results suggest an increase of NOx to 150–200 ppb (i.e. by factor of 50) at 65 km due to the descent following the SSW. The model, however, underestimates the amount of NOx around 55 km by 40–60 ppb. The results also show that the chemical loss of NOx was insignificant i.e. NOx was mainly controlled by the dynamics. Both ACE-FTS observations and FinROSE show a decrease of ozone of 20–30% at 30–50 km after mid-February to mid-March. However, these changes are not related to the NOx descent, but are due to activation of the halogen chemistry.


2009 ◽  
Vol 9 (3) ◽  
pp. 13299-13325 ◽  
Author(s):  
N. D. C. Allen ◽  
P. F. Bernath ◽  
C. D. Boone ◽  
M. P. Chipperfield ◽  
D. Fu ◽  
...  

Abstract. The first study of the global atmospheric distribution of carbon tetrachloride (CCl4), as a function of altitude and latitude, was performed using solar occultation measurements obtained by the Atmospheric Chemistry Experiment (ACE) mission using Fourier transform spectroscopy. A total of 8703 profile measurements were used in the study taken between February 2004 and August 2007. The zonal distribution of carbon tetrachloride displays a slight hemispheric asymmetry and decreasing concentration with increasing altitude at all latitudes. Maximum carbon tetrachloride concentrations are situated below 10 km in altitude with VMR (Volume Mixing Ratio) values of 100–130 ppt (parts per trillion). The highest concentrations are located about the equator and at mid-latitudes, particularly for latitudes in heavily industrialised regions (20–45° N), with values declining towards the poles. Global distributions obtained from ACE were compared with predictions from three chemistry transport models. The ACE dataset gives unique global and temporal coverage of carbon tetrachloride and its transport through the atmosphere. An estimated lifetime for carbon tetrachloride of 34±5 years was determined through correlation with CFC-11.


2008 ◽  
Vol 8 (2) ◽  
pp. 4499-4559 ◽  
Author(s):  
M. R. Carleer ◽  
C. D. Boone ◽  
K. A. Walker ◽  
P. F. Bernath ◽  
K. Strong ◽  
...  

Abstract. The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Water vapour (H2O), one of the most important molecules for climate and atmospheric chemistry, is one of the key species provided by the two principal instruments, the infrared Fourier Transform Spectrometer (ACE-FTS) and the MAESTRO UV-Visible spectrometer (ACE-MAESTRO). The first instrument performs measurements on several lines in the 1362–2137 cm−1 range, from which vertically resolved H2O concentration profiles are retrieved, from 7 to 90 km altitude. ACE-MAESTRO measures profiles using the water absorption band in the near infrared part of the spectrum at 926.0–969.7 nm. This paper presents a comprehensive validation of the ACE-FTS profiles. We have compared the H2O volume mixing ratio profiles with space-borne (SAGE II, HALOE, POAM III, MIPAS, SMR) observations and measurements from balloon-borne frostpoint hygrometers and a ground based lidar. We show that the ACE-FTS measurements provide H2O profiles with small retrieval uncertainties in the stratosphere (better than 5% from 15 to 70 km, gradually increasing above). The situation is unclear in the upper troposphere, due mainly to the high variability of the water vapour volume mixing ratio in this region. A new water vapour data product from the ACE-MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) is also presented and initial comparisons with ACE-FTS are discussed.


2016 ◽  
Author(s):  
Andreas Ostler ◽  
Ralf Sussmann ◽  
Prabir K. Patra ◽  
Sander Houweling ◽  
Marko De Bruine ◽  
...  

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.


Author(s):  
D. D. Lucas ◽  
C. Yver Kwok ◽  
P. Cameron-Smith ◽  
H. Graven ◽  
D. Bergmann ◽  
...  

Abstract. Emission rates of greenhouse gases (GHGs) entering into the atmosphere can be inferred using mathematical inverse approaches that combine observations from a network of stations with forward atmospheric transport models. Some locations for collecting observations are better than others for constraining GHG emissions through the inversion, but the best locations for the inversion may be inaccessible or limited by economic and other non-scientific factors. We present a method to design an optimal GHG observing network in the presence of multiple objectives that may be in conflict with each other. As a demonstration, we use our method to design a prototype network of six stations to monitor summertime emissions in California of the potent GHG 1,1,1,2-tetrafluoroethane (CH2FCF3, HFC-134a). We use a multiobjective genetic algorithm to evolve network configurations that seek to jointly maximize the scientific accuracy of the inferred HFC-134a emissions and minimize the associated costs of making the measurements. The genetic algorithm effectively determines a set of "optimal" observing networks for HFC-134a that satisfy both objectives (i.e., the Pareto frontier). The Pareto frontier is convex, and clearly shows the tradeoffs between performance and cost, and the diminishing returns in trading one for the other. Without difficulty, our method can be extended to design optimal networks to monitor two or more GHGs with different emissions patterns, or to incorporate other objectives and constraints that are important in the practical design of atmospheric monitoring networks.


2014 ◽  
Vol 14 (11) ◽  
pp. 16043-16083
Author(s):  
T. Sakazaki ◽  
M. Shiotani ◽  
M. Suzuki ◽  
D. Kinnison ◽  
J. M. Zawodny ◽  
...  

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.


2020 ◽  
Vol 13 (5) ◽  
pp. 2379-2392 ◽  
Author(s):  
Michael Jähn ◽  
Gerrit Kuhlmann ◽  
Qing Mu ◽  
Jean-Matthieu Haussaire ◽  
David Ochsner ◽  
...  

Abstract. Emission inventories serve as crucial input for atmospheric chemistry transport models. To make them usable for a model simulation, they have to be pre-processed and, traditionally, provided as input files at discrete model time steps. In this paper, we present an “online” approach, which produces a minimal number of input data read-in at the beginning of a simulation and which handles essential processing steps online during the simulation. For this purpose, a stand-alone Python package “emiproc” was developed, which projects the inventory data to the model grid and generates temporal and vertical scaling profiles for individual emission categories. The package is also able to produce “offline” emission files if desired. Furthermore, we outline the concept of the online emission module (written in Fortran 90) and demonstrate its implementation in two different atmospheric transport models: COSMO-GHG and COSMO-ART. Simulation results from both modeling systems show the equivalence of the online and offline procedure. While the model run time is very similar for both approaches, input size and pre-processing time are greatly reduced when online emissions are utilized.


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