Contrasting temporal trends and relationships of total organic carbon, black carbon, and polycyclic aromatic hydrocarbons in rural low-altitude and remote high-altitude lakes

Historical records of total organic carbon (TOC), black carbon (BC), and polycyclic aromatic hydrocarbons (PAHs) were reconstructed in dated sediment cores from four nearby lakes in central Switzerland. In the sub-Alpine Lake Thun, located at 558 m a.s.l., the proximity to anthropogenic emission sources is reflected in higher input of BC and PAHs into sediments with fluxes only slightly decreasing during the last decades. PAH/BC ratios are relatively high and correlation between levels of total PAHs and BC is almost inexistent in Lake Thun, probably due to the presence of less condensed forms of the BC spectrum (char BC) that is underestimated with the chemothermal oxidation method applied in this study. The sediment profiles of TOC, BC, and PAHs are noticeably different in the mountain lakes located around 2000 m a.s.l. In Lake Engstlen, the PAH/BC ratios, as well as the correlation between PAHs and BC, point towards appreciable amounts of predominantly light soot particles. Light soot particles have higher mobility and can, therefore, be efficiently transported to this remote site. The proglacial Lake Oberaar is shown to be a receptor of BC and PAHs released by the fast melting adjacent glacier acting as a secondary source for these conservative species temporarily stored in the glacier ice. Finally, Lake Stein is in strong contrast to all other lakes. High flux of BC into Lake Stein, combined with constant temporal evolutions of BC and PAHs, and in particular BC/TOC ratios approaching 100% are all strong indications for a geogenic presence of graphite in its catchment area.