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| Titel |
Acetone variability in the upper troposphere: analysis of CARIBIC observations and LMDz-INCA chemistry-climate model simulations |
| VerfasserIn |
T. Elias, S. Szopa, A. Zahn, T. Schuck, C. Brenninkmeijer, D. Sprung, F. Slemr |
| Medientyp |
Artikel
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| Sprache |
Englisch
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| ISSN |
1680-7316
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| Digitales Dokument |
URL |
| Erschienen |
In: Atmospheric Chemistry and Physics ; 11, no. 15 ; Nr. 11, no. 15 (2011-08-08), S.8053-8074 |
| Datensatznummer |
250009991
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| Publikation (Nr.) |
 copernicus.org/acp-11-8053-2011.pdf |
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| Zusammenfassung |
This paper investigates the acetone variability in the upper troposphere
(UT) as sampled during the CARIBIC airborne experiment and simulated by the
LMDz-INCA global chemistry climate model. The aim is to (1) describe spatial
distribution and temporal variability of acetone; (2) propose benchmarks
deduced from the observed data set; and (3) investigate the
representativeness of the observational data set.
According to the model results, South Asia (including part of the Indian
Ocean, all of India, China, and the Indochinese peninsula) and Europe
(including Mediterranean Sea) are net source regions of acetone, where
nearly 25 % of North Hemispheric (NH) primary emissions and nearly 40 %
of the NH chemical production of acetone take place. The impact of these net
source regions on continental upper tropospheric acetone is studied by
analysing CARIBIC observations of 2006 and 2007 when most flight routes
stretched between Frankfurt (Germany) and Manila (Philippines), and by
focussing over 3 sub-regions where acetone variability is strong:
Europe-Mediterranean, Central South China and South China Sea.
Important spatial variability was observed over different
scales: (1) east-west positive gradient of annually averaged
acetone vmr in UT over the Eurasian continent, namely a
factor two increase from east to west; (2) ocean/continent
contrast with 50 % enhancement over the continents;
(3) the acetone volume mixing ration (vmr) may vary in summer
by more than 1000 pptv within only 5 latitude-longitude degrees;
(4) the standard deviation for measurements acquired
during a short flight sequence over a sub-region may reach
40 %. Temporal variability is also important: (1) the acetone volume
mixing ratio (vmr) in the UT varies with the season, increasing from winter
to summer by a factor 2 to 4; (2) a difference as large as 200 pptv may be
observed between successive inbound and outbound flights over the same
sub-region due to different flight specifications (trajectory in relation to
the plume, time of day).
A satisfactory agreement for the abundance of acetone is found between model
results and observations, with e.g. only 30 % overestimation of the annual
average over Central-South China and the South China Sea (between 450 and
600 pptv), and an underestimation by less than 20 % over
Europe-Mediterranean (around 800 pptv). Consequently, annual budget terms
could be computed with LMDz-INCA, yielding a global atmospheric burden of
7.2 Tg acetone, a 127 Tg yr−1 global source/sink strength, and a 21-day mean
residence time.
Moreover the study shows that LMDz-INCA can reproduce the impact of summer
convection over China when boundary layer compounds are lifted to cruise
altitude of 10–11 km and higher. The consequent enhancement of acetone vmr
during summer is reproduced by LMDz-INCA, to reach agreement on an observed
maximum of 970 ± 400 pptv (average during each flight sequence over the
defined zone ± standard deviation). The summer enhancement of acetone
is characterized by a high spatial and temporal heterogeneity, showing the
necessity to increase the airborne measurement frequency over Central-South
China and the South China Sea in August and September, when the annual
maximum is expected (daily average model values reaching potentially 3000 pptv).
In contrast, the annual cycle in the UT over Europe-Mediterranean is
not reproduced by LMDz-INCA, in particular the observed summer enhancement
of acetone to 1400 ± 400 pptv after long-range transport of free
tropospheric air masses over North Atlantic Ocean is not reproduced. In view
of the agreement on the acetone annual cycle at surface level, this
disagreement in UT over Europe indicates misrepresentation of simulated
transport of primary acetone or biased spatial distribution of acetone
chemical sinks and secondary sources. The sink and source budget in
long-range transported free tropospheric air masses may be studied by
analysing atmospheric chemical composition observed by CARIBIC in summer
flights between North America and Europe. |
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