global hcfc-22 measurements with mipas: retrieval, validation, global distribution and its evolution over 2005–2012
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ID: 227730
2016
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Abstract
We report on HCFC-22 data acquired by the Michelson Interferometer for
Passive Atmospheric Sounding (MIPAS) in the reduced spectral resolution
nominal observation mode. The data cover the period from January 2005 to
April 2012 and the altitude range from the upper troposphere (above cloud top
altitude) to about 50 km. The profile retrieval was performed by constrained
nonlinear least squares fitting of modelled spectra to the measured limb
spectral radiances. The spectral ν4-band at
816.5 ± 13 cm−1 was used for the retrieval. A Tikhonov-type
smoothing constraint was applied to stabilise the retrieval. In the lower
stratosphere, we find a global volume mixing ratio of HCFC-22 of about
185 pptv in January 2005. The rate of linear growth in the lower latitudes
lower stratosphere was about 6 to 7 pptv year−1 in the period 2005–2012. The profiles obtained
were compared with ACE-FTS satellite data v3.5, as well as with MkIV balloon
profiles and cryosampler balloon measurements. Between 13 and 22 km, average
agreement within −3 to +5 pptv (MIPAS – ACE) with ACE-FTS v3.5 profiles
is demonstrated. Agreement with MkIV solar occultation balloon-borne
measurements is within 10–20 pptv below 30 km and worse above, while in
situ cryosampler balloon measurements are systematically lower over their
full altitude range by 15–50 pptv below 24 km and less than 10 pptv above
28 km. MIPAS HCFC-22 time series below 10 km altitude are shown to agree
mostly well to corresponding time series of near-surface abundances from the NOAA/ESRL and AGAGE networks, although a more pronounced seasonal cycle is
obvious in the satellite data. This is attributed to tropopause altitude
fluctuations and subsidence of polar winter stratospheric air into the
troposphere. A parametric model consisting of constant, linear,
quasi-biennial oscillation (QBO) and several sine and cosine terms with
different periods has been fitted to the temporal variation of stratospheric
HCFC-22 for all 10°-latitude/1-to-2-km-altitude bins. The relative
linear variation was always positive, with relative increases of
40–70 % decade−1 in
the tropics and global lower stratosphere, and up to 120 % decade−1
in the upper stratosphere of the northern polar region and the southern
extratropical hemisphere. Asian HCFC-22 emissions have become the major
source of global upper tropospheric HCFC-22. In the upper troposphere,
monsoon air, rich in HCFC-22, is instantaneously mixed into the tropics. In the
middle stratosphere, between 20 and 30 km, the observed trend is
inconsistent with the trend at the surface (corrected for the age of
stratospheric air), hinting at circulation changes. There exists a stronger
positive trend in HCFC-22 in the Southern Hemisphere and a more muted
positive trend in the Northern Hemisphere, implying a potential change in the
stratospheric circulation over the observation period.
| Reference Key |
chirkov2016atmosphericglobal
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|---|---|
| Authors | ;M. Chirkov;G. P. Stiller;A. Laeng;S. Kellmann;T. von Clarmann;C. D. Boone;J. W. Elkins;A. Engel;N. Glatthor;U. Grabowski;C. M. Harth;M. Kiefer;F. Kolonjari;P. B. Krummel;A. Linden;C. R. Lunder;B. R. Miller;S. A. Montzka;J. Mühle;S. O'Doherty;J. Orphal;R. G. Prinn;G. Toon;M. K. Vollmer;K. A. Walker;K. A. Walker;R. F. Weiss;A. Wiegele;D. Young |
| Journal | Journal of agricultural and food chemistry |
| Year | 2016 |
| DOI |
10.5194/acp-16-3345-2016
|
| URL | |
| Keywords |
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