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10.5194/acpd-10-14771-2010
http://www.atmos-chem-phys-discuss.net/10/14771/2010/
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http://www.atmos-chem-phys-discuss.net/10/14771/2010/acpd-10-14771-2010.pdf
14771
14814
2010-06-16
Formic acid above the Jungfraujoch during 1985–2007: observed variability, seasonality, but no long-term background evolution
R. Zander
r.zander@ulg.ac.be
P. Duchatelet
E. Mahieu
P. Demoulin
G. Roland
C. Servais
J. Vander Auwera
A. Perrin
C. P. Rinsland
P. Crutzen
Institute of Astrophysics and Geophysics, University of Liège, 4000, Liège, Belgium
Service de Chimie Quantique et Photophysique, Université Libre de Bruxelles, 1050, Brussels, Belgium
Laboratoire Interuniversitaire de Systèmes Atmosphériques, CNRS, Université de Paris 12 et 7, 94010 Créteil cedex, France
NASA Langley Research Center, Hampton, VA 23681-2199, USA
Max Planck Institute for Chemistry, Airchemistry Division, Mainz, Germany
This paper reports on daytime total vertical column abundances
of formic acid (HCOOH) above the Northern mid-latitude, high
altitude Jungfraujoch station (Switzerland; 46.5° N,
8.0° E, 3580 m altitude). The columns were derived from
the analysis of infrared solar observations regularly
performed with high spectral resolution Fourier transform
spectrometers during over 1537 days between September 1985 and
September 2007. The investigation was based on the
spectrometric fitting of five spectral intervals, one
encompassing the HCOOH ν<sub>6</sub> band Q branch at
1105 cm<sup>−1</sup>, and four additional ones allowing to
optimally account for critical temperature-sensitive or timely
changing interferences by other atmospheric gases, in
particular HDO, CCl<sub>2</sub>F<sub>2</sub> and CHClF<sub>2</sub>. The
main results derived from the 22 yr long database indicate
that the free tropospheric burden of HCOOH above the
Jungfraujoch undergoes important short-term daytime
variability, diurnal and seasonal modulations, inter-annual
anomalies, but no statistically significant long-term
background change at the 1-sigma level.
<br><br>
A major progress in the remote determination of the
atmospheric HCOOH columns reported here has resulted from the
adoption of new, improved absolute spectral line intensities
for the infrared ν<sub>6</sub> band of trans-formic acid,
resulting in retrieved free tropospheric loadings being about
a factor two smaller than if derived with previous
spectroscopic parameters. Implications of this significant
change with regard to earlier remote measurements of
atmospheric formic acid and comparison with relevant Northern
mid-latitude in situ findings will be assessed
critically. Sparse HCOOH model predictions will also be
evoked.
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