Article (Scientific journals)
Diurnal cycle and multi-decadal trend of formaldehyde in the remote atmosphere near 46° N
Franco, Bruno; Marais, Eloise A.; Bovy, Benoît et al.
2016In Atmospheric Chemistry and Physics, 16, p. 4171-4189
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Keywords :
formaldehyde (HCHO); Fourier transform infrared spectroscopy; GEOS-Chem; diurnal cycle; long-term variation
Abstract :
[en] Only very few long-term records of formaldehyde (HCHO) exist that are suitable for trend analysis. Furthermore, many uncertainties remain as to its diurnal cycle, representing a large short-term variability superimposed on seasonal and inter-annual variations that should be accounted for when comparing ground-based observations to e.g., model results. In this study, we derive a multi-decadal time series (January 1988 – June 2015) of HCHO total columns from ground-based high-resolution Fourier transform infrared (FTIR) solar spectra recorded at the high-altitude station of Jungfraujoch (Swiss Alps, 46.5° N, 8.0° E, 3580 m a.s.l.), allowing for the characterization of the mid-latitudinal atmosphere for background conditions. First we investigate the HCHO diurnal variation, peaking around noontime and mainly driven by the intra-day insolation modulation and methane (CH4) oxidation. We also characterize quantitatively the diurnal cycles by adjusting a parametric model to the observations, which links the daytime to the HCHO columns according to the monthly intra-day regimes. It is then employed to scale all the individual FTIR measurements on a given daytime in order to remove the effect of the intra-day modulation for improving the trend determination and the comparison with HCHO columns simulated by the state-of-the-art chemical transport model GEOS-Chem v9-02. Such a parametric model will be useful to scale the Jungfraujoch HCHO columns on satellite overpass times in the framework of future calibration/validation efforts of space borne sensors. GEOS-Chem sensitivity tests suggest then that the seasonal and inter-annual HCHO column variations above Jungfraujoch are predominantly led by the atmospheric CH4 oxidation, with a maximum contribution of 25 % from the anthropogenic non-methane volatile organic compound precursors during wintertime. Finally, trend analysis of the so-scaled 27-year FTIR time series reveals a long-term evolution of the HCHO columns in the remote troposphere to be related with the atmospheric CH4 fluctuations and the short-term OH variability: +2.9 %/yr between 1988 and 1995, -3.7 %/yr over 1996-2002 and +0.8/% yr from 2003 onwards.
Disciplines :
Earth sciences & physical geography
Author, co-author :
Franco, Bruno ;  Université de Liège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Marais, Eloise A.;  Harvard University, Cambridge, MA, USA > School of Engineering and Applied Sciences
Bovy, Benoît ;  Université de Liège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Bader, Whitney ;  Université de Liège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Lejeune, Bernard ;  Université de Liège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Roland, Ginette;  Université de Liège - ULiège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Servais, Christian ;  Université de Liège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Mahieu, Emmanuel  ;  Université de Liège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Language :
English
Title :
Diurnal cycle and multi-decadal trend of formaldehyde in the remote atmosphere near 46° N
Publication date :
31 March 2016
Journal title :
Atmospheric Chemistry and Physics
ISSN :
1680-7316
eISSN :
1680-7324
Publisher :
Copernicus Publications, Katlenburg-Lindau, Germany
Volume :
16
Pages :
4171-4189
Peer reviewed :
Peer Reviewed verified by ORBi
European Projects :
FP7 - 284421 - NORS - Demonstration Network Of ground-based Remote Sensing Observations in support of the GMES Atmospheric Service
Funders :
PRODEX project ACROSAT funded by the Belgian Science Policy O ce (BELSPO)
Swiss GAW-CH program
F.R.S.-FNRS - Fonds de la Recherche Scientifique [BE]
CE - Commission Européenne [BE]
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