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The general warming trend of the last deglaciation was interrupted by the Younger Dryas, a period of abrupt cooling and widespread environmental change(1-10). Ice core records suggest the abrupt cooling began 12,846 years ago in Greenland(10), about 170 years before the significant environmental and vegetation change in western Europe(7) classically defined as the Younger Dryas. However, this difference in timing falls within age model uncertainties. Here we use the hydrogen isotope composition of lipid biomarkers from precisely dated varved sediments from Lake Meerfelder Maar to reconstruct hydroclimate over western Europe. We observe a decrease in the hydrogen isotope values of both aquatic and terrestrial lipids 12,850 years ago, indicating cooling climate in this region synchronous with the abrupt cooling in Greenland. A second drop occurs 170 years later, mainly in the hydrogen isotope record of aquatic lipids but to a lesser extent in the terrestrial lipids, which we attribute to aridification, as well as a change in moisture source and pathway. We thus confirm that there was indeed a lag between cooling and substantial hydrologic and environmental change in western Europe. We suggest the delay is related to the expansion of sea ice in the North Atlantic Ocean and the subsequent southward migration of the westerly wind system(9). We further suggest that these hydrological changes amplified environmental change in western Europe at the onset of the Younger Dryas.
Dinosterol delta D values in stratified tropical lakes (Cameroon) are affected by eutrophication
(2015)
In freshwater settings, dinosterol (4 alpha,23,24-trimethyl-5 alpha-cholest-22E-en-3 beta-ol) is produced primarily by dinoflagellates, which encompass various species including autotrophs, mixotrophs and heterotrophs. Due to its source specificity and occurrence in lake and marine sediments, its presence and hydrogen isotopic composition (delta D) should be valuable proxies for paleohydrological reconstruction. However, because the purity required for hydrogen isotope measurements is difficult to achieve using standard wet chemical purification methods, their potential as a paleohydrological proxy is rarely exploited. In this study, we tested delta D values of dinosterol in both particulate organic matter (POM) and sediments of stratified tropical freshwater lakes (from Cameroon) as a paleohydrological proxy, the lakes being characterized by variable degrees of eutrophication. In POM and sediment samples, the delta D values of dinosterol correlated with lake water delta D values, confirming a first order influence of source water delta D values. However, we observed that sedimentary dinosterol was D enriched from ca. 19 to 54% compared with POM dinosterol. The enrichment correlated with lake water column conditions, mainly the redox potential at the oxic-anoxic interface (E-h OAI). The observations suggest that paleohydrologic reconstruction from delta D values of dinosterol in the sediments of stratified tropical lakes ought to be sensitive to the depositional environment, in addition to lake water delta D values, with more positive dinosterol delta values potentially reflecting increasing lake eutrophication. Furthermore, in lake sediments, the concentration of partially reduced vs. non-reduced C-34 botryococcenes, stanols vs. stenols, and bacterial (diploptene, diplopterol and beta beta-bishomohopanol) vs. planktonic/terrestrial lipids (cholesterol, campesterol and dinosterol) correlated with Eh OAI. We suggest using such molecular proxies for lake redox conditions in combination with dinosterol delta D values to evaluate the effect of lake trophic status on sedimentary dinosterol delta D values, as a basis for accurately reconstructing tropical lake water delta D values. (C) 2015 Elsevier Ltd. All rights reserved.
A potential human footprint on Western Central African rainforests before the Common Era has become the focus of an ongoing controversy. Between 3,000 y ago and 2,000 y ago, regional pollen sequences indicate a replacement of mature rainforests by a forest-savannah mosaic including pioneer trees. Although some studies suggested an anthropogenic influence on this forest fragmentation, current interpretations based on pollen data attribute the "rainforest crisis" to climate change toward a drier, more seasonal climate. A rigorous test of this hypothesis, however, requires climate proxies independent of vegetation changes. Here we resolve this controversy through a continuous 10,500-y record of both vegetation and hydrological changes from Lake Barombi in Southwest Cameroon based on changes in carbon and hydrogen isotope compositions of plant waxes. delta C-13-inferred vegetation changes confirm a prominent and abrupt appearance of C-4 plants in the Lake Barombi catchment, at 2,600 calendar years before AD 1950 (cal y BP), followed by an equally sudden return to rainforest vegetation at 2,020 cal y BP. delta D values from the same plant wax compounds, however, show no simultaneous hydrological change. Based on the combination of these data with a comprehensive regional archaeological database we provide evidence that humans triggered the rainforest fragmentation 2,600 y ago. Our findings suggest that technological developments, including agricultural practices and iron metallurgy, possibly related to the large-scale Bantu expansion, significantly impacted the ecosystems before the Common Era.
The observation that the hydrogen isotope composition (delta D) of leaf wax lipids is determined mainly by precipitation delta D values, has resulted in the application of these biomarkers to reconstruct paleoclimate from geological records. However, because the delta D values of leaf wax lipids are additionally affected by vegetation type and ecosystem evapotranspiration, paleoclimatic reconstruction remains at best semi-quantitative. Here, we used published results for the carbon isotope composition (delta C-13) of n-alkanes in common plants along a latitudinal gradient in C-3/C-4 vegetation and relative humidity in Cameroon and demonstrated that pentacyclic triterpene methyl ethers (PTMEs) and n-C-29 and n-C-31 in the same soil, derived mainly from C-4 graminoids (e.g. grass) and C-3 plants (e.g. trees and shrubs), respectively. We found that the delta D values of soil n-C-27, n-C29 and n-C-31, and PTMEs correlated significantly with surface water delta D values, supporting previous observations that leaf wax lipid delta D values are an effective proxy for reconstructing precipitation delta D values even if plant types changed significantly. The apparent fractionation (epsilon(app)) between leaf wax lipid and precipitation delta D values remained relatively constant for C-3-derived long chain n-alkanes, whereas eapp of C-4-derived PTMEs decreased by 20 parts per thousand along the latitudinal gradient encompassing a relative humidity range from 80% to 45%. Our results indicate that PTME delta D values derived from C-4 graminoids may be a more reliable paleo-ecohydrological proxy for ecosystem evapotranspiration within tropical and sub-tropical Africa than n-alkane delta D values, the latter being a better proxy for surface water delta D values. We suggest that vegetation changes associated with different plant water sources and/or difference in timing of leaf wax synthesis between C-3 trees of the transitional class and C-3 shrubs of the savanna resulted in a D depletion in soil long chain n-alkanes, thereby counteracting the effect of evapotranspiration D enrichment along the gradient. In contrast, evaporative D enrichment of leaf and soil water was significant enough to be recorded in the delta D values of PTMEs derived from C-4 graminoids, likely because PTMEs recorded the hydrogen isotopic composition of the same vegetation type.
Leaf wax n-alkane H-2 values carry important information about environmental and ecophysiological processes in plants. However, the physiological and biochemical drivers that shape leaf wax n-alkane H-2 values are not completely understood. It is particularly unclear why n-alkanes in grasses are typically H-2-depleted compared with plants from other taxonomic groups such as dicotyledonous plants and why C3 grasses are H-2-depleted compared with C4 grasses. To resolve these uncertainties, we quantified the effects of leaf water evaporative H-2-enrichment and biosynthetic hydrogen isotope fractionation on n-alkane H-2 values for a range of C3 and C4 grasses grown in climate-controlled chambers. We found that only a fraction of leaf water evaporative H-2-enrichment is imprinted on the leaf wax n-alkane H-2 values in grasses. This is interesting, as previous studies have shown in dicotyledonous plants a nearly complete transfer of this H-2-enrichment to the n-alkane H-2 values. We thus infer that the typically observed H-2-depletion of n-alkanes in grasses (as opposed to dicots) is because only a fraction of the leaf water evaporative H-2-enrichment is imprinted on the H-2 values. Our experiments also show that differences in n-alkane H-2 values between C3 and C4 grasses are largely the result of systematic differences in biosynthetic fractionation between these two plant groups, which was on average -198 and-159 parts per thousand for C3 and C4 grasses, respectively. We present novel and exciting data on how leaf wax n-alkane 2H values from grasses are affected by plant physiological (leaf water evaporative 2H-enrichment) or biochemical processes (biosynthetic hydrogen isotope fractionation). These results are very interesting because they shed new light on how naturally observed differences between 2H values from C3 and C4 grasses and dicots can be explained by systematic differences in the biosynthesis of n-alkanes between these plant group (i.e. largely driven by NADPH origins).
Elevation-dependent changes in n-alkane delta D and soil GDGTs across the South Central Andes
(2016)
Surface uplift of large plateaus may significantly influence regional climate and more specifically precipitation patterns and temperature, sometimes complicating paleoaltimetry interpretations. Thus, understanding the topographic evolution of tectonically active mountain belts benefits from continued development of reliable proxies to reduce uncertainties in paleoaltimetry reconstructions. Lipid biomarker-based proxies provide a novel approach to stable isotope paleoaltimetry and complement authigenic or pedogenic mineral proxy materials, in particular outside semi-arid climate zones where soil carbonates are not abundant but (soil) organic matter has a high preservation potential. Here we present delta D values of soil-derived n-alkanes and mean annual air temperature (MAT) estimates based on branched glycerol dialkyl glycerol tetraether (brGDGT) distributions to assess their potential for paleoelevation reconstructions in the southern central Andes. We analyzed soil samples across two environmental and hydrological gradients that include a hillslope (26-28 degrees S) and a valley (22-24 degrees S) transect on the windward flanks of Central Andean Eastern Cordillera in NW Argentina. Our results show that present-day n-alkane delta D values and brGDGT-based MAT estimates are both linearly related with elevation and in good agreement with present-day climate conditions. Soil n-alkanes show a delta D lapse rate (A(delta D)) of -1.64 parts per thousand/100 m (R-2 = 0.91, p < 0.01) at the hillslope transect, within the range of delta D lapse rates from precipitation and surface waters in other tropical regions in the Andes like the Eastern Cordillera in Colombia and Bolivia and the Equatorial and Peruvian Andes. BrGDGT-derived soil temperatures are similar to monitored winter temperatures in the region and show a lapse rate of Delta T = -0.51 degrees C/100 m (R-2 = 0.91, p < 0.01), comparable with lapse rates from in situ soil temperature measurements, satellite derived land-surface temperatures at this transect, and weather stations from the Eastern Cordillera at similar latitude. As a result of an increasing leeward sampling position along the valley transect lapse rates are biased towards lower values and display higher scatter (Delta(delta D) = -0.9 parts per thousand/100 m, R-2 = 0.76, p < 0.01 and Delta T = -0.19 degrees C/100 m, R-2 = 0.48, p < 0.05). Despite this higher complexity, they are in line with lapse rates from stream-water samples and in situ soil temperature measurements along the same transect. Our results demonstrate that both soil n-alkane delta D values and MAT reconstructions based on brGDGTs distributions from the hillslope transect (Delta(delta D) = -1.64 parts per thousand/100 m, R-2 = 0.91, p < 0.01 and Delta T = -0.51 degrees C/100 m, R-2 = 0.91, p < 0.01) track the direct effects of orography on precipitation and temperature and hence the combined effects of local and regional hydrology as well as elevation. (C) 2016 Elsevier B.V. All rights reserved.
In this study, we evaluated the potential of the hydrogen isotopic composition of algal lipid biomarkers as a proxy for past hydroclimatic variability in hypersaline Isabel Lake, Mexico (Eastern Pacific). We compared rainfall variability recorded in the region over the last 65 years with changes in delta D values of the most abundant compounds preserved in the uppermost 16 cm of lake sediment. Changes in delta D values of the 1,15-C-32 diol (delta D-diol), a specific biomarker of algal populations, were related to rainfall variability; specifically, n-alkyl diols were more deuterium-enriched (depleted) during wetter (drier) periods. Strikingly, neither the magnitude of lipid biomarker isotopic changes over interannual timescales (of up to 70-80 parts per thousand) nor the direction of that variability can be explained by changes in delta D values of the water source or salinity fluctuations (approximately 30 on the practical salinity scale) controlled by seasonal rainfall. However, changes in sedimentary biomarker composition, higher total organic carbon content and less negative delta C-13 values of the 1,15-C-32 diol indicate enhanced algal growth during wetter periods. We find that these conditions result in less negative delta D values of n-alkyl diols. We hypothesize that due to higher lipid demand during enhanced algal growth, an increasing proportion of hydrogen for lipid synthesis is derived from the cytosol via oxidation of polysaccharides, which may cause a deuterium enrichment of the acetogenic compounds. This study has significant implications for paleohydrological reconstructions using algal lipid delta D values, particularly in highly seasonal environments such as Isabel Lake. In such environments, delta D values of specific algal lipid biomarkers may not record the full seasonal cycle in source water delta D but appear to be mainly controlled by the physiological state of algal populations. Our data provide the first evidence that changes in D/H fractionation due to algal growth conditions can be recorded in sediments. For paleoclimate reconstructions in such environments, algal growth conditions should be constrained with additional proxy data (delta C-13 values of the same biomarkers), as the net D/H fractionation between water and lipids may not have been constant over time.
The Central Asian Pamir Mountains (Pamirs) are a high-altitude region sensitive to climatic change, with only few paleoclimatic records available. To examine the glacial-interglacial hydrological changes in the region, we analyzed the geochemical parameters of a 31-kyr record from Lake Karakul and performed a set of experiments with climate models to interpret the results. delta D values of terrestrial biomarkers showed insolation-driven trends reflecting major shifts of water vapor sources. For aquatic biomarkers, positive delta D shifts driven by changes in precipitation seasonality were observed at ca. 31-30, 28-26, and 17-14 kyr BP. Multiproxy paleoecological data and modelling results suggest that increased water availability, induced by decreased summer evaporation, triggered higher lake levels during those episodes, possibly synchronous to northern hemispheric rapid climate events. We conclude that seasonal changes in precipitation-evaporation balance significantly influenced the hydrological state of a large waterbody such as Lake Karakul, while annual precipitation amount and inflows remained fairly constant.
Hydrogen isotope values (delta D) of sedimentary aquatic and terrestrial lipid biomarkers, originating from algae, bacteria, and leaf wax, have been used to record isotopic properties of ancient source water (i.e., precipitation and/or lake water) in several mid-and high-latitude lacustrine environments. In the tropics, however, where both processes associated with isotope fractionation in the hydrologic system and vegetation strongly differ from those at higher latitudes, calibration studies for this proxy are not yet available. To close this gap of knowledge, we sampled surface sediments from 11 lakes in Cameroon to identify those hydro-climatological processes and physiological factors that determine the hydrogen isotopic composition of aquatic and terrestrial lipid biomarkers. Here we present a robust framework for the application of compound-specific hydrogen isotopes in tropical Africa. Our results show that the delta D values of the aquatic lipid biomarker n-C(17) alkane were not correlated with the delta D values of lake water. Carbon isotope measurements indicate that the n-C(17) alkane was derived from multiple source organisms that used different hydrogen pools for biosynthesis. We demonstrate that the delta D values of the n-C(29) alkane were correlated with the delta D values of surface water (i.e., river water and groundwater), which, on large spatial scales, reflect the isotopic composition of mean annual precipitation. Such a relationship has been observed at higher latitudes, supporting the robustness of the leaf-wax lipid delta D proxy on a hemispheric spatial scale. In contrast, the delta D values of the n-C(31) alkane did not show such a relationship but instead were correlated with the evaporative lake water delta D values. This result suggests distinct water sources for both leaf-wax lipids, most likely originating from two different groups of plants. These new findings have important implications for the interpretation of long-chain n-alkane delta D records from ancient lake sediments. In particular, a robust interpretation of palaeohydrological data requires knowledge of the vegetation in the catchment area as different plants may utilise different water sources. Our results also suggest that the combination of carbon and hydrogen isotopes does help to differentiate between the metabolic pathway and/or growth form of organisms and therefore, the source of hydrogen used during lipid biosynthesis.