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High-resolution paleoclimate records from tropical continental settings are greatly needed to advance understanding of global climate dynamics. The International Continental Scientific Drilling Program (ICDP) project DeepCHALLA recovered a 214.8-meter long sediment sequence from Lake Chala, a deep and permanently stratified (meromictic) crater lake in equatorial East Africa, covering the past c. 250,000 years (250 kyr) of continuous lacustrine deposition since the earliest phase of lake-basin development. Lipid biomarker analyses on the sediments of this long-lived lake can provide much-needed records 5 of past climate variability from this currently poorly documented region. However, the degree to which climate proxies derived from aquatically produced biomarkers are affected by aspects of lake developmental history is rarely considered, even though it may critically influence their ability to consistently register a particular climate variable through time. Modern-system studies in Lake Chala revealed crucial information about the mechanisms underpinning relationships between proxies based on isoprenoid (iso-) and branched (br-) glycerol dialkyl glycerol tetraethers (GDGTs) and the targeted climate variables, but the 10 persistence of these relationships in the past remains unclear. To assess the reliability of long-term climate signals registered in the sediments of Lake Chala, we compared downcore variations in GDGT distributions with major phases in lake-system evolution as indicated by independent proxies of lake depth, mixing regime and nutrient dynamics: seismic reflection data, lithology and fossil diatom assemblages. Together, these records suggest that during early lake history (before c. 180-200 ka) the distinct mixing-related depth zones with which specific GDGT producers are associated in the modern-day lake were not 15 yet formed, likely due to more open lake hydrology and absence of chemical water-column stratification. Consequently during this early phase the absolute GDGT concentrations are relatively low, proxies sensitive to water-column stratification (e.g., BIT index) display highly irregular temporal variability, and correlations between proxies are dissimilar to expectations based on modern-system understanding. A sequence of lake-system changes between c. 180-200 ka and c. 80 ka first established and then strengthened the chemical density gradient, promoting meromictic conditions despite the overall decrease in lake depth due to sediment accumulation. From c. 180 ka onward some GDGTs and derived proxies (e.g., crenarchaeol concentration, BIT index and IR6Me) display strong 23-kyr periodicity, likely reflecting the predominantly precession-driven insolation forcing of Quaternary climate variability in low-latitude regions. Our results suggest that GDGT-based temperature and moisture-balance proxies in Lake Chala sediments reflect the climate history of eastern equatorial Africa from at least c. 160 ka onwards, i.e., covering the complete last glacial-interglacial cycle and the penultimate glacial maximum. This work confirms the potential of 25 lacustrine GDGTs for elucidating the climate history of tropical regions at Quaternary timescales, provided they are applied to suitably high-quality sediment archives. Additionally, their interpretation should incorporate a broader understanding of the extent to which lake-system evolution limits the extrapolation back in time of proxy-climate relationships established in the modern system. [ABSTRACT FROM AUTHOR]

Rivers play a key role in the global carbon cycle by transporting terrestrial organic matter (TerrOM) from land to the ocean. Upon burial in marine sediments, this TerrOM may be a significant long-term carbon sink, depending on its composition and properties. However, much remains unknown about the dispersal of different types of TerrOM in the marine realm upon fluvial discharge as the commonly used bulk OM parameters do not reach the required level of sourceand process-specific information. Here, we analysed bulk OM properties, lipid biomarkers (long-chain n-alkanes, sterols, long-chain diols, alkenones, branched and isoprenoid glycerol dialkyl glycerol tetraethers (GDGTs)), pollen, and dinoflagellate cysts in marine surface sediments along two transects offshore the Mississippi and Atchafalaya Rivers (MAR), as well as one along the 20 m isobath in the direction of the river plume. We use these biomarkers and palynological proxies to identify the dispersal patterns of soil-, fluvial, higher plant, and marine produced OM in the coastal sediments of the northern Gulf of Mexico (GoM). The Branched and Isoprenoid Tetraether (BIT) index and the relative abundance of C32 1,15-diols indicative for freshwater production show high contributions of soil and fluvial OC near the Mississippi River mouth (BIT = 0.6, FC32 1,15 >50%), which rapidly decrease further away from the river mouth (BIT <0.1, FC32 1,15 <20%). In contrast, concentrations of long- chain n-alkanes and pollen grains do not show this stark decrease along the path of transport, and especially n-alkanes are also found in sediments in deeper waters. Proxy indicators show that marine productivity is highest close to shore, and reveal that marine producers (diatoms, dinoflagellates, coccolithophorids) have different spatial distributions, indicating their preferential niches. Close to the coast, where food supply is high and waters are turbid, cysts of heterotrophic dinoflagellates dominate the assemblages. The dominance of heterotrophic taxa in shelf waters in combination with the rapid decrease in the relative contribution of TerrOM towards the deeper ocean, suggests that TerrOM input may trigger a priming effect that results in its rapid decomposition upon discharge. In the open ocean far away from the river plume, autotrophic/phototrophic dinoflagellates dominate the assemblages, indicating more oligotrophic conditions. Our multi-disciplinary approach reveals that different types of TerrOM have distinct dispersal patterns, suggesting that the initial composition of this particulate OM influences the burial efficiency of TerrOM on the continental shelf and open ocean. [ABSTRACT FROM AUTHOR]

Monsoonal rivers play an important role in the land-to-sea transport of soil-derived organic carbon (OC). However, spatial and temporal variation in the concentration, composition, and fate of OC in these rivers remains poorly understood. We investigate soil-to-sea transport of OC by the Godavari River in India using branched glycerol dialkyl glycerol tetraether (brGDGT) lipids in soils, river suspended particulate matter (SPM), riverbed sediments, and in a marine sediment core from the Bay of Bengal. The abundance and composition of brGDGTs in SPM and sediments in the Godavari River differs between the dry and wet season. In the dry season, 6-methyl brGDGTs dominate SPM and riverbed sediments in the whole basin. Currently, mobilisation and transport of soils from the upper basin is limited due to deficient rainfall and damming. This promotes aquatic brGDGT production in this part of the basin, which is reflected by a high relative abundance of 6-methyl brGDGTs in both seasons. In the wet season, brGDGT distributions in SPM from the lower basin closely resemble those in soils, mostly from the North and East Tributaries, corresponding to precipitation patterns. The brGDGT composition in SPM and sediments from the delta suggests that soil OC is only effectively transported to the Bay of Bengal in the wet season, when the river plume extends beyond the river mouth. The sediment geochemistry indicates that also the mineral particles exported by the Godavari River primarily originate from the lower basin, similar to the brGDGTs. River depth profiles of brGDGTs in the downstream Godavari reveal no hydrodynamic sorting effect in either season, indicating that brGDGTs are not associated with certain minerals. The similarity of brGDGT distributions in bulk and fine-grained sediments (≤63μm) further confirms the absence of selective transport mechanisms. Nevertheless, the composition of brGDGTs in a Holocene, marine sediment core near the river mouth appears substantially different from that in the modern Godavari basin, suggesting that terrestrial derived brGDGTs are rapidly lost upon discharge into the Bay of Bengal and/or overprinted by marine in situ production. The change in brGDGT distributions at the river-sea transition implies that this zone is key in the effective transfer of soil OC, as well as for the interpretation of paleorecords based on brGDGTs in coastal marine sediment archives. [ABSTRACT FROM AUTHOR]

The large difference in the fractionation of stable carbon isotopes between C3 and C4 plants is widely used in vegetation reconstructions, where the predominance of C3 plants suggests wetter and that of C4 plants drier conditions. The isotopic composition of organic carbon (OC) preserved in soils or sediments may be a valuable (paleo-)environmental indicator, based on the assumption that plant-derived material retains the carbon isotopic signature of its photosynthetic pathway during transfer from plant to sediment. In this study, we investigated the carbon isotopic signature of C3 and C4 plants (δ13C) and of organic carbon (δ13Corg) in soils, river Suspended Particulate Matter (SPM) and riverbed sediments, to gain insight in the control of precipitation on C3 and C4 plant δ13C values and to assess changes in δ13Corg values along the plant-soil-river continuum. This information allows us to elucidate the implications of different δ13C end-members on C3/C4 vegetation reconstructions. Our analysis was performed in the Godavari River basin, which has mixed C3 and C4 vegetation and is situated in the Core Monsoon Zone in peninsular India, a region that integrates the hydroclimatic and vegetation changes caused by variation in monsoonal strength. The Godavari C3 and C4 plants revealed more negative δ13C values than global average vegetation values, suggesting region-specific plant δ13C signatures. Godavari C3 plants confirmed a strong control by Mean Annual Precipitation (MAP) on their δ13C values, with an isotopic enrichment of ~2.2 �€� for the interval between ~500 and 1500 mm y-1. Tracing δ13Corg values from plant to soils and rivers revealed that soils and riverbed sediments reflected the transition from mixed C3 and C4 vegetation in the dry upper basin to more C3 vegetation in the humid lower basin. Soil degradation and stabilisation processes and hydrodynamic sorting within the river altered the plant-derived δ13C signal. Phytoplankton dominated the δ13Corg signal carried by SPM in the dry season and year-round in the upper basin. Our analysis revealed that the reconstructed C3/C4 vegetation composition was sensitive to the plant δ13C end-members used as mixing model input. The %C4 plants in the different subbasins was ~10-19 % higher using Godavari-specific end-members than using global averages, and including a correction for drought enrichment in Godavari C3 plants resulted in a 2-10 % lower estimated C4 plant cover. Hence, incorporating region-specific plant δ13C end-members and drought correction of the C3 end-member in mixing models need to be considered to determine C3 and C4 distributions of modern- and paleo-vegetation in monsoonal regions. [ABSTRACT FROM AUTHOR]

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 (SPM) 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 time scales 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. [ABSTRACT FROM AUTHOR]

Soils represent the largest reservoir of organic carbon (OC) on land. Upon mobilization, this OC is either returned to the atmosphere as carbon dioxide (CO2), or transported and ultimately locked into (marine) sediments, where it will act as a long-term sink of atmospheric CO2. These fluxes of soil OC are, however, poorly quantified, mostly due to the lack of a soil-specific tracer. In this study, a suite of branched glycerol dialkyl glycerol tetraethers (brGDGTs), which are membrane lipids of soil bacteria, is tested as specific tracers for soil OC from source (soils under arable land, ley, grassland and woodland) to sink (Lake Loe Pool sediments) considering a small catchment located in southwest England (i.e. Carminowe Creek draining into Lake Loe Pool). The analysis of brGDGTs in catchment soils reveals that their distribution is not significantly different across different land use types (p > 0.05), and thus does not allow tracing land use-specific soil contributions to Lake Loe Pool sediments. Furthermore, the significantly higher contribution of 6-methyl brGDGT isomers in creek sediments (isomerization ratio (IR) = 0.48 ± 0.10; mean ± s.d., standard deviation; p < 0.05) compared to that in catchment soils (IR = 0.28 ± 0.11) indicates that the initial soil signal is substantially altered by brGDGT produced in situ. Similarly, the riverine brGDGT signal appears to be overwritten by lacustrine brGDGTs in the lake sedimentary record, indicated by remarkably lower Methylation of Branched Tetraethers (MBT'5ME = 0.46 ± 0.02 in creek bed sediment and 0.38 ± 0.01 in lake core sediment; p < 0.05) and higher Degree of Cyclization (DC = 0.23 ± 0.02 in creek bed sediment and 0.32 ± 0.08 in lake core sediment). Thus, in this small catchment, brGDGTs do not allow us to trace soil OC transport. Nevertheless, the downcore changes in the degree of cyclization and the abundance of isoprenoid GDGTs produced by methanogens in the Lake Loe Pool sediment do reflect local environmental conditions over the past 100 years, and have recorded the eutrophication history of the lake. [ABSTRACT FROM AUTHOR]

Long chain diols (LCDs) occur widespread in marine environments and also in lakes and rivers. Transport of LCDs from rivers may impact the distribution of LCDs in coastal environments, however relatively little is known about the distribution and biological sources of LCDs in river systems. In this study, we investigated the distribution of LCDs in suspended particulate matter (SPM) of three river systems (Godavari, Danube, and Rhine) in relation with season, precipitation, temperature, and source catchments. The dominant long-chain diol is the C32 1,15-diol followed by the C30 1,15-diol in all studied river systems. In regions influenced by marine waters, such as delta systems, the fractional abundance of the C30 1,15-diol is substantially higher than in the river itself, suggesting different LCD producers in marine and freshwater environments. A change in the LCD distribution along the downstream transects of the rivers studied was not observed. However, an effect of river flow is observed, i.e. the concentration of the C32 1,15-diol is higher in stagnant waters, such as reservoirs and during seasons with river low stands. A seasonal change in the LCD distribution was observed in the Rhine, likely due to a change in the producers. Eukaryotic diversity analysis by 18S rRNA gene sequencing of SPM from the Rhine showed extremely low abundances of sequences (i.e. < 0.32 % of total reads) related to known algal LCD producers. Furthermore, incubation of the river water with 13C-labelled bicarbonate did not result in 13C incorporation into LCDs. This indicates that the LCDs present are mainly of fossil origin in the fast flowing part of the Rhine. Overall, our results suggest that the LCD-producers in rivers predominantly reside in lakes or side ponds that are part of the river system. [ABSTRACT FROM AUTHOR]

The modern-day Godavari River transports large amounts of sediment (170 Tg per year) and terrestrial organic carbon (OCterr; 1.5 Tg per year) from peninsular India to the Bay of Bengal. The flux and nature of OCterr is considered to have varied in response to past climate and human forcing. In order to delineate the provenance and nature of organic matter (OM) exported by the fluvial system and establish links to sedimentary records accumulating on its adjacent continental margin, the stable and radiogenic isotopic composition of bulk OC, abundance and distribution of long-chain fatty acids (LCFA), sedimentological properties (e.g. grain size, mineral surface area etc.) of fluvial (riverbed and riverbank) sediments and soils from the Godavari basin were analysed and these characteristics were compared to those of a sediment core retrieved from the continental slope depocenter. Results show that river sediments from the upper catchment exhibit higher total organic carbon (TOC) contents than those from the lower part of the basin. The general relationship between TOC and sedimentological parameters (i.e., mineral-specific surface area and grain size) of the sediments suggests that sediment mineralogy, largely driven by provenance, plays an important role in the stabilization of OM during transport along the river axis, and in preservation of OM exported by the Godavari to the Bay of Bengal. The stable carbon isotopic (δ13C) characteristics of river sediments and soils indicate that the upper mainstream and its tributaries drain catchments exhibiting more 13C enriched carbon than the lower stream resulting from the regional vegetation gradient and/or net balance between the upper (C4-dominated plants) and lower (C3-dominated plants) catchments. The radiocarbon contents of organic carbon (Δ14COC) in deep soils and eroding riverbanks suggests these are likely sources of “old” or pre-aged carbon to the Godavari River that increasingly dominates the late Holocene portion of the offshore sedimentary record. Reduced monsoonal rainfall and sediment transport impeded by recent dam constructions have drastically impacted the flux, loci and composition of OC exported from the modern Godavari basin, rendering it challenging to reconcile modern-day river geochemistry with that recorded in continental margin sediments. [ABSTRACT FROM AUTHOR]