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Branched glycerol monoalkyl glycerol tetraethers (brGMGTs) are membrane-spanning lipids which were initially identified in marine settings and have more recently been found in peats and lake sediments . In the latter settings, their abundance relative to that of the branched glycerol dialkyl glycerol tetraethers (brGDGTs) appears to increase under warmer climate conditions. Furthermore, their relative distribution in bottom sediments from an altitudinal transect of East African lakes has been linked to local mean annual air temperature (MAAT). To shed light on their sources and identify potential environmental factors driving their production in lakes, we investigated their occurrence and distribution in the water column, surficial lake-bottom sediments, and catchment soils of Lake Chala, a permanently stratified (meromictic) tropical crater lake in East Africa. Data from the water column comprise both suspended particulate matter (SPM) collected monthly at eight depth intervals between 0 and 80 m for 17 consecutive months, and settling particles collected monthly at a depth of 35 m over a period of 53 months. In catchment soils, brGMGTs are either relatively scarce or absent. In the water column, their occurrence is dominated by four of the seven known brGMGTs and mostly limited to the anoxic zone. Whereas the spatial distribution and concentration of brGMGTs in SPM were strongly influenced by the seasonal cycle of strong water-column stratification alternating with deep mixing, this trend is not consistent on the multi-year timescale of the settling-particles record. Moreover, their relative distribution in both SPM and settling particles did not respond to temperature variation during the studied interval. In contrast to the water column, surficial lake-bottom sediments contain the full suite of known brGMGTs in a distinct and spatially uniform fractional abundance, strongly suggesting that the majority of brGMGT production takes place there. BrGMGT-inferred MAAT for the Chala area reasonably estimates measured MAAT and conforms to the East African lake brGMGT calibration. Our results have important implications for the use of brGMGTs as proxy for MAAT, in that outside of the equatorial zone the presumably greater offset between bottom-water temperature and MAAT may create a bias towards cold-season air temperature. Regardless, the more singular source of brGMGTs in lake sediments is an advantage for paleotemperature reconstruction compared to brGDGTs, which several studies now indicate to have a mixed aquatic and terrestrial source of which the relative contribution cannot easily be disentangled or assumed to have been constant through time.

Lake sediments are important archives of continental climate history, and their lipid biomarker content can be exploited to reconstruct paleoenvironmental conditions. Branched glycerol dialkyl glycerol tetraethers (brGDGTs) are bacterial membrane lipids widely used in paleoclimate studies to reconstruct past temperature. However, major gaps still exist in our understanding of the environmental controls on in situ (i.e. aquatic) production in lake systems. In Lake Chala, a permanently stratified tropical crater lake in East Africa, we determined the concentrations and fractional abundances of individual brGDGTs along depth profiles of suspended particulate matter collected monthly from September 2013 to January 2015 and in settling particles collected monthly at 35 m water depth from August 2010 to January 2015 and compared these brGDGT distributions with those in surficial lake bottom sediments and catchment soils. We find that brGDGTs are primarily produced within the water column and that their concentrations and distributions vary greatly with depth and over time. Comparison with concentration–depth profiles of the monthly distribution and abundance of bacterial taxa, based on 16S rRNA gene amplicon sequencing and quantification, indicates that Acidobacteria are likely not the main producers of brGDGTs in Lake Chala. Shallowing of the oxic–anoxic boundary during seasonal episodes of strong water column stratification promoted production of specific brGDGTs in the anoxic zone. BrGDGT distributions in the water column do not consistently relate with temperature, pH, or dissolved-oxygen concentration but do respond to transitions between episodes of strong stratification and deep (but partial) lake mixing, as does the aquatic bacterial community. Hence, the general link between brGDGT distributions and temperature in brGDGT-based paleothermometry is more likely driven by a change in bacterial community composition than by membrane adaptation of specific members of the bacterial community to changing environmental conditions. Although temperature is not the principal driver of distributional changes in aquatic brGDGTs in this system, at least not during the 17-month study period, abundance-weighted and time-integrated averages of brGDGT fractional abundance in the 53-month time series of settling particles reveal systematic variability over longer timescales that indirectly relates to temperature. Thus, although we do not as yet fully understand the drivers of modern-day brGDGT fluxes and distributions in Lake Chala, our data do support the application of brGDGT paleothermometry to time-integrated archives such as sediments. Highlights. BrGDGTs in the tropical African lake Chala are produced in situ. Acidobacteria are not the dominant source of aquatic brGDGTs. Stratification and mixing drive aquatic brGDGT production and their signature.

Non-hopanoid pentacyclic triterpenoids occur widely in lake sediments, but their biological sources and diagenetic pathways are not fully resolved. We tentatively identified a number of des-A-arborene isomers occurring in relatively high abundance in the 25,000 year (25 kyr) sedimentary record of Lake Chala, a deep crater lake in tropical East Africa. The mono-, di- and tri-unsaturated des-A-arborenes are transformation products of isoarborinol/arborinone. These precursors have an aquatic source and are most likely biosynthesized by algae or aerobic bacteria in the epilimnion. The relatively depleted delta C-13 values (on average - 32.3 parts per thousand +/- 1.3 parts per thousand) of des-A-arbor-9(11)-ene are consistent with an aquatic source (algae or aerobic bacteria). In general, isoarborinol and its microbially induced transformation products are found in present and ancient tropical lacustrine settings (typically crater lakes) with permanently anoxic bottom waters and sediments. Based on molecular mechanics calculations of des-A-arborenes, it is clear that these transformation products are not in thermodynamic equilibrium, strongly indicating that their formation is microbially mediated. Subtle temporal and spatial differences in the microbial community might therefore not only dictate the variable relative contributions of different des-A-arborenes found in the sediments of Lake Chala over the last 25 kyr, but also explain the distribution of arborane derivatives in comparable crater-lake settings elsewhere. (C) 2018 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND-license.