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See detailDiurnal cycle and multi-decadal trend of formaldehyde in the remote atmosphere near 46° N
Franco, Bruno ULg; Marais, Eloise A.; Bovy, Benoît ULg et al

in Atmospheric Chemistry & Physics Discussions (2015), 15

Only very few long-term trends of formaldehyde (HCHO) exist. Furthermore, many uncertainties remain as to its diurnal cycle, representing a large short-term variability superimposed on seasonal and inter ... [more ▼]

Only very few long-term trends of formaldehyde (HCHO) exist. 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. [less ▲]

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See detailTowards understanding the variability in biospheric CO2 fluxes: using FTIR spectrometry and a chemical transport model to investigate the sources and sinks of carbonyl sulfide and its link to CO2
Wang, Y.; Deutscher, N. M.; Palm, M. et al

in Atmospheric Chemistry & Physics Discussions (2015), 15(18), 26025--26065

Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and inter-annual variability of CO2 in the atmosphere. Atmospheric ... [more ▼]

Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and inter-annual variability of CO2 in the atmosphere. Atmospheric inversions based on CO2 concentration measurements alone can only determine net biosphere fluxes, but not differentiate between photosynthesis (uptake) and respiration (production). Carbonyl sulfide (OCS) could provide an important additional constraint: it is also taken up by plants during photosynthesis but not emitted during respiration, and therefore is a potential mean to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrievals of the atmospheric concentrations of both CO2 and OCS from measured solar absorption spectra. Here, we investigate co-located and quasi-simultaneous FTIR measurements of OCS and CO2 performed at three selected sites located in the Northern Hemisphere. These measurements are compared to simulations of OCS and CO2 using a chemical transport model (GEOS-Chem). The OCS simulations are driven by different land biospheric fluxes to reproduce the seasonality of the measurements. Increasing the plant uptake of Kettle et al. (2002a) by a factor of three resulted in the best comparison with FTIR measurements. However, there are still discrepancies in the latitudinal distribution when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. The coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study and compared to measurements. The CO2 simulation with SiB fluxes agrees with the measurements well, while the OCS simulation reproduced a weaker drawdown than FTIR measurements at selected sites, and a smaller latitudinal gradient in the Northern Hemisphere during growing season. An offset in the timing of the seasonal cycle minimum between SiB simulation and measurements is also seen. Using OCS as a photosynthesis proxy can help to understand how the biospheric processes are reproduced in models and to further understand the carbon cycle in the real world. [less ▲]

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See detailAnalysis of the global atmospheric methane budget using ECHAM-MOZ simulations for present-day, pre-industrial time and the Last Glacial Maximum
Basu, A.; Schultz, M. G.; Schröder, S. et al

in Atmospheric Chemistry & Physics Discussions (2014), 14

Atmospheric methane concentrations increased considerably from pre-industrial (PI) to present times largely due to anthropogenic emissions. However, firn and ice core records also document a notable rise ... [more ▼]

Atmospheric methane concentrations increased considerably from pre-industrial (PI) to present times largely due to anthropogenic emissions. However, firn and ice core records also document a notable rise of methane levels between the Last Glacial Maximum (LGM) and the pre-industrial era, the exact cause of which is not entirely clear. This study investigates these changes by analyzing the methane sources and sinks at each of these climatic periods. Wetlands are the largest natural source of methane and play a key role in determining methane budget changes in particular in the absence of anthropogenic sources. Here, a simple wetland parameterization suitable for coarse-scale climate simulations over long periods is introduced, which is derived from a high- resolution map of surface slopes together with various soil hydrology parameters from the CARAIB vegetation model. This parameterization was implemented in the chem- istry general circulation model ECHAM5-MOZ and multi-year time slices were run for LGM, PI and present-day (PD) climate conditions. Global wetland emissions from our parameterization are 72 Tg yr [less ▲]

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