Untangling the influence of in-lake productivity and terrestrial organic matter flux on 4,250 years of mercury accumulation in Lake Hambre, Southern Chile

There is ongoing debate about the relative influence of aquatic production, flux, and sedimentation of aquatic and terrestrial organic matter on mercury accumulation in lake sediments. In this study, lake sediments spanning the past 4,250 years, were collected from remote, organic-rich Lake Hambre, Patagonia (53A degrees A S) and investigated for changes in the accumulation of pre-anthropogenic mercury and organic matter of aquatic and terrestrial origin. Natural mercury accumulation varied by up to a factor of four, comparable to the recent anthropogenic forcing of the mercury cycle (factor 3-5). Hydrogen and Oxygen indices (HI and OI, Rock-EvalA (c)) and nitrogen/carbon ratios of the organic matter, combined with multi-element sediment data, reveal intense changes in aquatic productivity as well as influx of terrestrial organic matter into the lake. Evaluation of the multi-element dataset using Principal Component Analysis shows clear covariation of mercury with other soil-derived elements such as copper and yttrium. This covariance reflects a common transport mechanism, i.e. leaching of trace-element-bearing organic matter complexes from catchment soils. Correlation between changes in aquatic productivity and mercury concentrations occurs in some sections of the record, but we do not suggest they are linked by a direct causal relationship. Mass balance approaches suggest that mercury scavenging and accumulation in this organic-rich lake is controlled by the supply of mercury from catchment soils rather than the amount of organic material produced within the water column. A common controlling mechanism, i.e. changing climate, however, is thought to independently drive variations in both the flux of terrestrial organic matter mercury complexes and aquatic productivity.