We analyzed the precipitation chemistry for a maritime region in northern Germany (Schleswig-Holstein) from 1997 to 2017 in order to reveal temporal and spatial patterns and to evaluate the role of meteorological factors relative to emission reductions in Germany and Europe. Therefore, we applied several statistical methods such as time series decomposition, principal component, and redundancy analysis. We extracted two main groups: (i) a marine group (Cl, Na, Mg) that was related to natural processes like sea spray input and (ii) an anthropogenic group (Pb, Cd, As, Zn, and nitrogen species) with a terrestrial subgroup (Fe, Al, Mn), which were both related to emissions. These groups were valid for the spatial, seasonal, and annual trend data. Other elements, like Ca, K, total P, and sulfate, were influenced by natural and anthropogenic processes. The seasonal variation of ammonium deposition was caused primarily by ammonia emissions and ancillary by precipitation. Most heavy metals as well as sulfate, nitrate, and ammonium showed decreasing trends in concentrations and deposition fluxes. Only Hg did not show any trend. The decreasing depositions of sulfate and total nitrogen were correlated to emission reductions in Germany. The deposition of most heavy metals was influenced by emission reductions on European scale and meteorological factors such as wind speed and humidity. Hg did not show any correlation with the emission time series in Europe. Instead, it was correlated to the NAO index and wind, implying that global emissions and transport pathways determine the temporal development of Hg depositions. Overall, the study reveals that emission reductions positively influence regional depositions for most investigated substances. The regional spatial patterns of depositions were also influenced by local meteorological factors.
Keywords: Atmospheric deposition; Heavy metals; Multivariate statistics; Nutrients; Time series decomposition; Trend analysis.