Abstract
Abstract. We present a retrieval method for ammonia (NH3) total columns from ground-based Fourier transform infrared (FTIR) observations. Observations from Bremen (53.10° N, 8.85° E), Lauder (45.04° S, 169.68° E), Réunion (20.9° S, 55.50° E) and Jungfraujoch (46.55° N, 7.98° E) were used to illustrate the capabilities of the method. NH3 mean total columns ranging 3 orders of magnitude were obtained, with higher values at Bremen (mean of 13.47 × 1015 molecules cm−2) and lower values at Jungfraujoch (mean of 0.18 × 1015 molecules cm−2). In conditions with high surface concentrations of ammonia, as in Bremen, it is possible to retrieve information on the vertical gradient, as two layers can be distinguished. The retrieval there is most sensitive to ammonia in the planetary boundary layer, where the trace gas concentration is highest. For conditions with low concentrations, only the total column can be retrieved. Combining the systematic and random errors we have a mean total error of 26 % for all spectra measured at Bremen (number of spectra (N) = 554), 30 % for all spectra from Lauder (N = 2412), 25 % for spectra from Réunion (N = 1262) and 34 % for spectra measured at Jungfraujoch (N = 2702). The error is dominated by the systematic uncertainties in the spectroscopy parameters. Station-specific seasonal cycles were found to be consistent with known seasonal cycles of the dominant ammonia sources in the station surroundings. The developed retrieval methodology from FTIR instruments provides a new way of obtaining highly time-resolved measurements of ammonia burdens. FTIR-NH3 observations will be useful for understanding the dynamics of ammonia concentrations in the atmosphere and for satellite and model validation. It will also provide additional information to constrain the global ammonia budget.
Highlights
Nitrogen emissions in the form of ammonia (NH3), which largely derive from agriculture, have been associated with acidification and eutrophication of soils and surface waters (Krupa, 2003; Vitousek et al, 1997), which may reduce biodiversity in vulnerable ecosystems (Bobbink et al, 1998, 2010)
In this study we presented a new method to retrieve ammonia total columns from ground-based Fourier transform infrared (FTIR) solar spectra
Observations from four complementary stations were used to illustrate the capabilities of the retrieval method
Summary
Nitrogen emissions in the form of ammonia (NH3), which largely derive from agriculture, have been associated with acidification and eutrophication of soils and surface waters (Krupa, 2003; Vitousek et al, 1997), which may reduce biodiversity in vulnerable ecosystems (Bobbink et al, 1998, 2010). Recent advances in open-path remote sensing techniques, like (mini-)differential optical absorption spectroscopy (DOAS) systems and open-path quantum cascade laser (QCL) instruments, show great potential in overcoming part of these sampling issues (Volten et al, 2012; Miller et al, 2014), but are still in the development stage and not widely applied yet Another aspect is the lack of vertical information, as most instruments only measure surface concentrations (Erisman et al, 2007, 2008; Van Damme et al, 2015a).
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