Branched glycerol dialkyl glycerol tetraethers (GDGTs) are bacterial membrane lipids, ubiquitously present in soils and peat bogs, as well as in rivers, lakes and lake sediments. Their distribution in soil is controlled mainly by pH and mean annual air temperature, but the controls on their distribution in lake sediments are less well understood. Several studies have found a relationship between the distribution of branched GDGTs in lake sediments and average lake water pH, suggesting an aquatic source for them, besides that for soil transported to the lake via erosion. We sampled the surface water suspended particulate matter (SPM) from 23 lakes in Minnesota and Iowa (USA), that vary widely in pH, alkalinity and trophic state. The SPM was analyzed for the concentration and distributions of core lipid (presumed fossil origin) and intact polar lipid (IPL, presumed to derive from living cells) branched GDGTs. The presence of substantial amounts (18-48%) of IPL-derived branched GDGTs suggests that branched GDGTs are likely of autochthonous origin. Temperature estimates based on their distribution using lake-specific calibrations agree reasonably with water temperature at time of sampling and average air temperature of the season of sampling. Importantly, a strong correlation between the distribution of branched GDGTs and lake water pH was found (r2 0.72), in agreement with a predominant in situ production. An stronger correlation was found with lake water alkalinity (r2 0.83), although the underlying mechanism that controls the relationship is not understood. Our results raise the potential for reconstructing pH/alkalinity of past lake environments, which could provide important knowledge on past developments in lake water chemistry.
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We thank R. Smittenberg and an anonymous reviewer for constructive comments. We thank K. Poole, A. Erickson, D. Kendall, and J. Li, from the ISU Limnology Laboratory, and J. McGinnis from the lake survey in Grand Rapids, Itasca (MN), for technical support. Parts of the manuscript are based on work supported by the Iowa Department of Natural Resources and the National Science Foundation under Grant No. 005309844 . From the Royal NIOZ (Texel) we thank A. Mets, J. Ossebaar, M. Baas, M. Kienhuis, J. van Ooijen and K. Bakker for laboratory and analytical support. Partial funding for the project came from the Darwin Center of Biogeosciences (publication no. DW-2013-1003) and a VICI grant from the Netherlands Organisation for Scientific Research to S.S.