Decreasing litterfall mercury deposition in central European coniferous forests and effects of bark beetle infestation.

We evaluated a 14-year trend (2003-2017) in mercury (Hg) concentrations and fluxes in six litterfall categories (needles, bark, twigs, cones, lichen, and a mixture of unidentified fragments) at six research plots situated in two central European unmanaged mountain forest stands, dominated by mature Norway spruce. One of the stands (catchment of Plešné Lake, PL) was infested by bark beetle and all mature spruces died at three of four research plots during the study. One PL plot and two plots in the second stand (catchment of Čertovo Lake, CT) were intact and used as a control. At the intact plots, the litterfall Hg deposition averaged 45 and 32 μg/m/year in the PL and CT catchments, respectively, while bulk precipitation Hg deposition was an order of magnitude lower (2.6 μg/m/year). In the individual litter categories, Hg concentrations averaged 223, 195, 126, 81, 79 and 30 μg/kg in lichen, unidentified fragments, bark, twigs, needles and cones, respectively. As a result of decreasing European Hg emissions, Hg concentrations in most litter categories decreased from 2003 to 2017. Consequently, the litter-associated Hg flux to the forest floor decreased from 66 to 23 μg/m/year during 2003-2017. The litterfall mass fluxes exhibited no trends at the intact plots. In contrast, the litter-associated Hg flux increased 5-fold after tree dieback due to elevated litterfall, averaging 218 μg/m/year Hg at the PL infested plots during 2004-2009. The relative contribution of individual litter categories to the total Hg flux shifted from needle to bark and twig dominance. Starting in 2010, Hg flux decreased to pre-disturbance levels for the following decade. The tree mortality in the PL catchment provided a unique opportunity to evaluate changes in litter-associated Hg fluxes to the forest floor during and after natural tree dieback.