scholarly journals Validation of HNO<sub>3</sub>, ClONO<sub>2</sub>, and N<sub>2</sub>O<sub>5</sub> from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS)

2008 ◽  
Vol 8 (13) ◽  
pp. 3529-3562 ◽  
Author(s):  
M. A. Wolff ◽  
T. Kerzenmacher ◽  
K. Strong ◽  
K. A. Walker ◽  
M. Toohey ◽  
...  

Abstract. The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra in the ultraviolet/visible and infrared wavelength regions. The reservoir gases HNO3, ClONO2, and N2O5 are three of the key species provided by the primary instrument, the ACE Fourier Transform Spectrometer (ACE-FTS). This paper describes the ACE-FTS version 2.2 data products, including the N2O5 update, for the three species and presents validation comparisons with available observations. We have compared volume mixing ratio (VMR) profiles of HNO3, ClONO2, and N2O5 with measurements by other satellite instruments (SMR, MLS, MIPAS), aircraft measurements (ASUR), and single balloon-flights (SPIRALE, FIRS-2). Partial columns of HNO3 and ClONO2 were also compared with measurements by ground-based Fourier Transform Infrared (FTIR) spectrometers. Overall the quality of the ACE-FTS v2.2 HNO3 VMR profiles is good from 18 to 35 km. For the statistical satellite comparisons, the mean absolute differences are generally within ±1 ppbv ±20%) from 18 to 35 km. For MIPAS and MLS comparisons only, mean relative differences lie within±10% between 10 and 36 km. ACE-FTS HNO3 partial columns (~15–30 km) show a slight negative bias of −1.3% relative to the ground-based FTIRs at latitudes ranging from 77.8° S–76.5° N. Good agreement between ACE-FTS ClONO2 and MIPAS, using the Institut für Meteorologie und Klimaforschung and Instituto de Astrofísica de Andalucía (IMK-IAA) data processor is seen. Mean absolute differences are typically within ±0.01 ppbv between 16 and 27 km and less than +0.09 ppbv between 27 and 34 km. The ClONO2 partial column comparisons show varying degrees of agreement, depending on the location and the quality of the FTIR measurements. Good agreement was found for the comparisons with the midlatitude Jungfraujoch partial columns for which the mean relative difference is 4.7%. ACE-FTS N2O5 has a low bias relative to MIPAS IMK-IAA, reaching −0.25 ppbv at the altitude of the N2O5 maximum (around 30 km). Mean absolute differences at lower altitudes (16–27 km) are typically −0.05 ppbv for MIPAS nighttime and ±0.02 ppbv for MIPAS daytime measurements.

2008 ◽  
Vol 8 (1) ◽  
pp. 2429-2512 ◽  
Author(s):  
M. A. Wolff ◽  
T. Kerzenmacher ◽  
K. Strong ◽  
K. A. Walker ◽  
M. Toohey ◽  
...  

Abstract. The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra in the ultraviolet/visible and infrared wavelength regions. The reservoir gases HNO3, ClONO2, and N2O5 are three of the key species provided by the primary instrument, the ACE Fourier Transform Spectrometer (ACE-FTS). This paper describes the ACE-FTS version 2.2 data products, including the N2O5 update, for the three species and presents validation comparisons with available observations. We have compared volume mixing ratio (VMR) profiles of HNO3, ClONO2, and N2O5 with measurements by other satellite instruments (SMR, MLS, MIPAS), aircraft measurements (ASUR), and single balloon-flights (SPIRALE, FIRS-2). Partial columns of HNO3 and ClONO2 were also compared with measurements by ground-based Fourier Transform Infrared (FTIR) spectrometers. Overall the quality of the ACE-FTS v2.2 HNO3 VMR profiles is good from 18 to 35 km. For the statistical satellite comparisons, the mean absolute differences are generally within ±1 ppbv (±20%) from 18 to 35 km. For MIPAS and MLS comparisons only, mean relative differences lie within ±10% between 10 and 36 km. ACE-FTS HNO3 partial columns (~15–30 km) show a slight negative bias of −1.3% relative to the ground-based FTIRs at latitudes ranging from 77.8° S–76.5° N. Good agreement between ACE-FTS ClONO2 and MIPAS, using the Institut für Meteorologie und Klimaforschung and Instituto de Astrofísica de Andalucía (IMK-IAA) data processor is seen. Mean absolute differences are typically within ±0.01 ppbv between 16 and 27 km and less than +0.09 ppbv between 27 and 34 km. The ClONO2 partial column comparisons show varying degrees of agreement, depending on the location and the quality of the FTIR measurements. Good agreement was found for the comparisons with the midlatitude Jungfraujoch partial columns for which the mean relative difference is 4.7%. ACE-FTS N2O5 has a low bias relative to MIPAS IMK-IAA, reaching −0.25 ppbv at the altitude of the N2O5 maximum (around 30 km). Mean absolute differences at lower altitudes (16–27 km) are typically −0.05 ppbv for MIPAS nighttime and ±0.02 ppbv for MIPAS daytime measurements.


2008 ◽  
Vol 8 (16) ◽  
pp. 4759-4786 ◽  
Author(s):  
K. Strong ◽  
M. A. Wolff ◽  
T. E. Kerzenmacher ◽  
K. A. Walker ◽  
P. F. Bernath ◽  
...  

Abstract. The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N2O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3–4 km. In this study, the quality of the ACE-FTS version 2.2 N2O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between −42 ppbv and +17 ppbv, with most within ±20 ppbv. This corresponds to relative deviations from the mean that are within ±15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences for the satellite comparisons are generally within ±10 ppbv. From 30 to 60 km, the mean absolute differences are within ±4 ppbv, and are mostly between −2 and +1 ppbv. Given the small N2O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns (which cover a mean altitude range of 14 to 27 km) are within ±5.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation (R=0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of −0.20 on the line fitted to the data.


2008 ◽  
Vol 8 (1) ◽  
pp. 3597-3663 ◽  
Author(s):  
K. Strong ◽  
M. A. Wolff ◽  
T. E. Kerzenmacher ◽  
K. A. Walker ◽  
P. F. Bernath ◽  
...  

Abstract. The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N2O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3–4 km. In this study, the quality of the ACE-FTS version 2.2 N2O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Overall, the quality of the ACE-FTS version 2.2 N2O VMR profiles is good over the entire altitude range from 5 to 60 km. Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between −42 ppbv and +17 ppbv, with most within ±20 ppbv. This corresponds to relative deviations from the mean that are within ±15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences are generally within ±10 ppbv, again excluding the aircraft and balloon comparisons. From 30 to 60 km, the mean absolute differences are within ±4 ppbv, and are mostly between −2 and +1 ppbv. Given the small N2O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns are within ±6.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation (R=0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of −0.20 on the line fitted to the data.


2015 ◽  
Vol 8 (10) ◽  
pp. 11171-11207
Author(s):  
E. M. Buzan ◽  
C. A. Beale ◽  
C. D. Boone ◽  
P. F. Bernath

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.


2008 ◽  
Vol 8 (9) ◽  
pp. 2569-2594 ◽  
Author(s):  
C. Clerbaux ◽  
M. George ◽  
S. Turquety ◽  
K. A. Walker ◽  
B. Barret ◽  
...  

Abstract. The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Carbon monoxide (CO), a good tracer of pollution plumes and atmospheric dynamics, is one of the key species provided by the primary instrument, the ACE-Fourier Transform Spectrometer (ACE-FTS). This instrument performs measurements in both the CO 1-0 and 2-0 ro-vibrational bands, from which vertically resolved CO concentration profiles are retrieved, from the mid-troposphere to the thermosphere. This paper presents an updated description of the ACE-FTS version 2.2 CO data product, along with a comprehensive validation of these profiles using available observations (February 2004 to December 2006). We have compared the CO partial columns with ground-based measurements using Fourier transform infrared spectroscopy and millimeter wave radiometry, and the volume mixing ratio profiles with airborne (both high-altitude balloon flight and airplane) observations. CO satellite observations provided by nadir-looking instruments (MOPITT and TES) as well as limb-viewing remote sensors (MIPAS, SMR and MLS) were also compared with the ACE-FTS CO products. We show that the ACE-FTS measurements provide CO profiles with small retrieval errors (better than 5% from the upper troposphere to 40 km, and better than 10% above). These observations agree well with the correlative measurements, considering the rather loose coincidence criteria in some cases. Based on the validation exercise we assess the following uncertainties to the ACE-FTS measurement data: better than 15% in the upper troposphere (8–12 km), than 30% in the lower stratosphere (12–30 km), and than 25% from 30 to 100 km.


2013 ◽  
Vol 13 (14) ◽  
pp. 6921-6950 ◽  
Author(s):  
A. T. Brown ◽  
C. M. Volk ◽  
M. R. Schoeberl ◽  
C. D. Boone ◽  
P. F. Bernath

Abstract. Long lived halogen-containing compounds are important atmospheric constituents since they can act both as a source of chlorine radicals, which go on to catalyse ozone loss, and as powerful greenhouse gases. The long-term impact of these species on the ozone layer is dependent on their stratospheric lifetimes. Using observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) we present calculations of the stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O. The lifetimes were calculated using the slope of the tracer–tracer correlation of these species with CFC-11 at the tropopause. The correlation slopes were corrected for the changing atmospheric concentrations of each species based on age of air and CFC-11 measurements from samples taken aboard the Geophysica aircraft – along with the effective linear trend of the volume mixing ratio (VMR) from tropical ground based AGAGE (Advanced Global Atmospheric Gases Experiment) sites. Stratospheric lifetimes were calculated using a CFC-11 lifetime of 45 yr. These calculations produced values of 113 + (−) 26 (18) yr (CFC-12), 35 + (−) 11 (7) yr (CCl4), 69 + (−) 65 (23) yr (CH3Cl), 123 + (−) 53 (28) yr (N2O) and 195 + (−) 75 (42) yr (CH4). The errors on these values are the weighted 1σ non-systematic errors. Systematic errors were estimated by recalculating lifetimes using VMRs which had been modified to reflect differences between ACE-FTS retrieved VMRs and those from other instruments. The results of these calculations, including systematic errors, were as follows: 113 + (−) 32 (20) for CFC-12, 123 + (−) 83 (35) for N2O, 195 + (−) 139 (57) for CH4, 35 + (−) 14 (8) for CCl4 and 69 + (−) 2119 (34) yr for CH3Cl. For CH3Cl &amp; CH4 this represents the first calculation of the stratospheric lifetime using data from a space based instrument.


2009 ◽  
Vol 9 (20) ◽  
pp. 8039-8047 ◽  
Author(s):  
G. González Abad ◽  
P. F. Bernath ◽  
C. D. Boone ◽  
S. D. McLeod ◽  
G. L. Manney ◽  
...  

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.


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