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            Free, publicly-accessible full text available October 1, 2026
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            Abstract. Lipid remodeling, the modification of cell membrane chemistry via structural rearrangements within the lipid pool of an organism, is a common physiological response amongst all domains of life to alleviate environmental stress and maintain cellular homeostasis. Whereas culture experiments and environmental studies of phytoplankton have demonstrated the plasticity of lipids in response to specific abiotic stressors, few analyses have explored the impacts of multi-environmental stressors at the community-level scale. Here, we study changes in the pool of intact polar lipids (IPLs) of a phytoplanktonic community exposed to multi-environmental stressors during a ∼ 2-month-long mesocosm experiment deployed in the eastern tropical South Pacific off the coast of Callao, Peru. We investigate lipid remodeling of IPLs in response to changing nutrient stoichiometries, temperature, pH, and light availability in surface and subsurface water masses with contrasting redox potentials, using multiple linear regressions, classification and regression trees, and random forest analyses. We observe proportional increases in certain glycolipids (namely mono- and diglycosyldiacylglycerol – MGDG and DGDG, respectively) associated with higher temperatures and oxic conditions, consistent with previous observations of their utility to compensate for thermal stress and their degradation under oxygen stress. N-bearing (i.e., betaine lipids and phosphatidylethanolamine – BLs and PE) and non-N-bearing (i.e., MGDG; phosphatidylglycerol, PG; and sulfoquinovosyldiacylglycerol, SQDG) IPLs are anti-correlated and have strong positive correlations with nitrogen-replete and nitrogen-depleted conditions, respectively, which suggests a substitution mechanism for N-bearing IPLs under nitrogen limitation. Reduced CO2(aq) availability and increased pH levels are associated with greater proportions of DGDG and SQDG IPLs, possibly in response to the lower concentration of CO2(aq) and the overall lower availability of inorganic carbon for fixation. A higher production of MGDG in surface waters corresponds well with its established photoprotective and antioxidant mechanisms in thylakoid membranes. The observed statistical relationships between IPL distributions, physicochemical parameters, and the composition of the phytoplankton community suggest evidence of lipid remodeling in response to environmental stressors. These physiological responses may allow phytoplankton to reallocate resources from structural or extrachloroplastic membrane lipids (i.e., phospholipids and betaine lipids) under high-growth conditions to thylakoid and/or plastid membrane lipids (i.e., glycolipids and certain phosphatidylglycerols) under growth-limiting conditions. Further investigation of the exact mechanisms controlling the observed trends in lipid distributions is necessary to better understand how membrane reorganization under multi-environmental stressors can affect the pools of cellular C, N, P, and S, as well as their fluxes to higher trophic levels in marine environments subjected to increasing environmental pressure. Our results suggest that future studies addressing the biogeochemical consequences of climate change in the eastern tropical South Pacific Ocean must take into consideration the impacts of lipid remodeling in phytoplankton.more » « less
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            The distribution of brGDGT lipids produced by soil bacteria has been used to reconstruct temperatures in marine and terrestrial settings as far back as the Cretaceous period. However, modern calibrations of this proxy have primarily relied on air rather than in situ soil temperatures, which can differ by more than 10 ◦C. Furthermore, the influence of other parameters such as temperature seasonality and soil chemistry on brGDGT lipids is not fully understood. We measured brGDGT distributions, in situ soil temperatures, pH, soil water content, and electrical conductivity on soils from the Eastern Canadian Arctic and Iceland. We compiled our results with those of published soil brGDGT studies that also provide in situ soil temperatures and ancilliary measurements and generated global temperature and pH calibrations from the resulting dataset. Soil temperatures outperformed air temperatures in these calibrations, with mean summer soil temperature providing the highest-performing fit among the 10 tested soil temperature parameters. When applied to a loess/paleosol sequence from the Chinese Loess Plateau, these new calibrations produced paleotemperature and paleo-pH histories consistent with the results of previous studies, encouraging the application of our new calibrations on a broader scale. We also detected 7-methyl and IIIa’’ brGDGT isomers in our Eastern Canadian Arctic and Iceland soils, which have been shown in lakes to relate to salinity and anoxia, respectively. While neither correlated with bulk soil properties such as conductivity, soil water content, or pH, these brGDGT isomers did correlate with seasonality and winter soil temperature. We hypothesize that these compounds are generated in winter by bacteria in habitable niches of more saline, sometimes anoxic liquid water in the otherwise frozen soil matrix. Finally, we report the presence of overly branched GDGTs with m/z = 1064 and suggest that these heptamethylated tetraethers should be investigated as a potential tool for improving brGDGT calibrations. Overall, our results expand our understanding of the seasonality of brGDGT production, especially at high latitudes, and provide in situ soil temperature and pH calibrations for global use.more » « less
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            A Holocene history of climate, fire, landscape evolution, and human activity in northeastern IcelandAbstract. Paleoclimate reconstructions across Iceland provide a template for past changes in climate across the northern North Atlantic, a crucial region due to its position relative to the global northward heat transport system and its vulnerability to climate change. The roles of orbitally driven summer cooling, volcanism, and human impact as triggers of local environmental changes in the Holocene of Iceland remain debated. While there are indications that human impact may have reduced environmental resilience during late Holocene summer cooling, it is still difficult to resolve to what extent human and natural factors affected Iceland's late Holocene landscape instability. Here, we present a continuous Holocene fire record of northeastern Iceland from proxies archived in Stóra Viðarvatn sediment. We use pyrogenic polycyclic aromatic hydrocarbons (pyroPAHs) to trace shifts in fire regimes, paired with continuous biomarker and bulk geochemical records of soil erosion, lake productivity, and human presence. The molecular composition of pyroPAHs and a wind pattern reconstruction indicate a naturally driven fire signal that is mostly regional. Generally low fire frequency during most of the Holocene significantly increased at 3 ka and again after 1.5 ka BP before known human settlement in Iceland. We propose that shifts in vegetation type caused by cooling summers over the past 3 kyr, in addition to changes in atmospheric circulation, such as shifts in North Atlantic Oscillation (NAO) regime, led to increased aridity and biomass flammability. Our results show no evidence of faecal biomarkers associated with human activity during or after human colonisation in the 9th century CE. Instead, faecal biomarkers follow the pattern described by erosional proxies, pointing toward a negligible human presence and/or a diluted signal in the lake's catchment. However, low post-colonisation levels of pyroPAHs, in contrast to an increasing flux of erosional bulk proxies, suggest that farming and animal husbandry may have suppressed fire frequency by reducing the spread and flammability of fire-prone vegetation (e.g. heathlands). Overall, our results describe a fire frequency heavily influenced by long-term changes in climate through the Holocene. They also suggest that human colonisation had contrasting effects on the local environment by lowering its resilience to soil erosion while increasing its resilience to fire.more » « less
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            The generation of hydrogen and reduced carbon compounds during serpentinization provides sustained energy for microorganisms on Earth, and possibly on other extraterrestrial bodies (e.g., Mars, icy satellites). However, the geochemical conditions that arise from water-rock reaction also challenge the known limits of microbial physiology, such as hyperalkaline pH, limited electron acceptors and inorganic carbon. Because cell membranes act as a primary barrier between a cell and its environment, lipids are a vital component in microbial acclimation to challenging physicochemical conditions. To probe the diversity of cell membrane lipids produced in serpentinizing settings and identify membrane adaptations to this environment, we conducted the first comprehensive intact polar lipid (IPL) biomarker survey of microbial communities inhabiting the subsurface at a terrestrial site of serpentinization. We used an expansive, custom environmental lipid database that expands the application of targeted and untargeted lipodomics in the study of microbial and biogeochemical processes. IPLs extracted from serpentinite-hosted fluid communities were comprised of >90% isoprenoidal and non-isoprenoidal diether glycolipids likely produced by archaeal methanogens and sulfate-reducing bacteria. Phospholipids only constituted ~1% of the intact polar lipidome. In addition to abundant diether glycolipids, betaine and trimethylated-ornithine aminolipids and glycosphingolipids were also detected, indicating pervasive membrane modifications in response to phosphate limitation. The carbon oxidation state of IPL backbones was positively correlated with the reduction potential of fluids, which may signify an energy conservation strategy for lipid synthesis. Together, these data suggest microorganisms inhabiting serpentinites possess a unique combination of membrane adaptations that allow for their survival in polyextreme environments. The persistence of IPLs in fluids beyond the presence of their source organisms, as indicated by 16S rRNA genes and transcripts, is promising for the detection of extinct life in serpentinizing settings through lipid biomarker signatures. These data contribute new insights into the complexity of lipid structures generated in actively serpentinizing environments and provide valuable context to aid in the reconstruction of past microbial activity from fossil lipid records of terrestrial serpentinites and the search for biosignatures elsewhere in our solar system.more » « less
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            Abstract. As global warming progresses, changes in high-latitude precipitation are expected to impart long-lasting impacts on Earth systems, including glacier mass balance and ecosystem structures. Reconstructing past changes in high-latitude precipitation and hydroclimate from networks of continuous lake records offers one way to improve forecasts of precipitation and precipitation–evaporation balances, but these reconstructions are currently hindered by the incomplete understanding of controls on lake and soil water isotopes. Here, we study the distribution of modern water isotopes in Icelandic lakes, streams, and surface soils collected in 2002, 2003, 2004, 2014, 2019, and 2020 to understand the geographic, geomorphic, and environmental controls on their regional and interannual variability. We find that lake water isotopes in open-basin (through-flowing) lakes reflect local precipitation, with biases toward the cold season, particularly in lakes with sub-annual residence times. Closed-basin lakes have water isotope and deuterium excess values consistent with evaporative enrichment. Interannual and seasonal variabilities of lake water isotopes at repeatedly sampled sites are consistent with instrumental records of winter snowfall; summer relative humidity; and atmospheric circulation patterns, such as the North Atlantic Oscillation. Summer surface soil water isotopes span the entire range of seasonal precipitation values in Iceland and appear to be consistently overprinted by evaporative enrichment, which can occur throughout the year, although the sampling depths were shallower than rooting depths for many plant types. This dataset provides new insight into the functionality of water isotopes in Icelandic environments and offers renewed possibilities for optimized site selection and proxy interpretation in future paleohydrological studies on this North Atlantic outpost.more » « less
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            none (Ed.)As the Arctic continues to warm, woody shrubs are expected to expand northward. This process, known as ‘shrubification,’ has important implications for regional biodiversity, food web structure, and high-latitude temperature amplification. While the future rate of shrubification remains poorly constrained, past records of plant immigration to newly deglaciated landscapes in the Arctic may serve as useful analogs. We provide one new postglacial Holocene sedimentary ancient DNA (sedaDNA) record of vascular plants from Iceland and place a second Iceland postglacialsedaDNA record on an improved geochronology; both show Salicaceae present shortly after deglaciation, whereas Betulaceae first appears more than 1000 y later. We find a similar pattern of delayed Betulaceae colonization in eight previously published postglacialsedaDNA records from across the glaciated circum North Atlantic. In nearly all cases, we find that Salicaceae colonizes earlier than Betulaceae and that Betulaceae colonization is increasingly delayed for locations farther from glacial-age woody plant refugia. These trends in Salicaceae and Betulaceae colonization are consistent with the plant families’ environmental tolerances, species diversity, reproductive strategies, seed sizes, and soil preferences. As these reconstructions capture the efficiency of postglacial vascular plant migration during a past period of high-latitude warming, a similarly slow response of some woody shrubs to current warming in glaciated regions, and possibly non-glaciated tundra, may delay Arctic shrubification and future changes in the structure of tundra ecosystems and temperature amplification.more » « less
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            As the Arctic continues to warm, woody shrubs are expected to expand northward. This process, known as ‘shrubification,’ has important implications for regional biodiversity, food web structure, and high-latitude temperature amplification. While the future rate of shrubification remains poorly constrained, past records of plant immigration to newly deglaciated landscapes in the Arctic may serve as useful analogs. We provide one new postglacial Holocene sedimentary ancient DNA (sedaDNA) record of vascular plants from Iceland and place a second Iceland postglacialsedaDNA record on an improved geochronology; both show Salicaceae present shortly after deglaciation, whereas Betulaceae first appears more than 1000 y later. We find a similar pattern of delayed Betulaceae colonization in eight previously published postglacialsedaDNA records from across the glaciated circum North Atlantic. In nearly all cases, we find that Salicaceae colonizes earlier than Betulaceae and that Betulaceae colonization is increasingly delayed for locations farther from glacial-age woody plant refugia. These trends in Salicaceae and Betulaceae colonization are consistent with the plant families’ environmental tolerances, species diversity, reproductive strategies, seed sizes, and soil preferences. As these reconstructions capture the efficiency of postglacial vascular plant migration during a past period of high-latitude warming, a similarly slow response of some woody shrubs to current warming in glaciated regions, and possibly non-glaciated tundra, may delay Arctic shrubification and future changes in the structure of tundra ecosystems and temperature amplification.more » « less
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            Abstract Oceanic trenches are an important sink for organic matter (OM). However, little is known about how much of the OM reaching the hadal region derives from the sunlit surface ocean and other sources. We provide new insight into the OM sources in the Atacama Trench by examining the elemental and stable isotope composition of carbon and nitrogen in bulk OM throughout the entire water column and down to bathyal and hadal sediments. Moreover, we estimated the particulate organic carbon (POC) concentration and downward carbon flux. Our results, based on two‐way variance analysis, showed statistical differences in δ15NPONbetween the epipelagic zone and the deep zones. However, no statistical differences in δ13CPOCand C:N ratio between hadalpelagic and shallower pelagic zones were found, except for δ13CPOCin the oxygen‐deficient zone. On the contrary, whereas the isotopic signatures of hadal sediments were distinct from those over the entire water column, they were similar to the values in bathyal sediments. Thus, our results suggest that bathyal sediments could contribute more OM to hadal sediments than the different zones of the water column. Indeed, whereas POC flux estimates derived from remote sensing data indicate that ∼16%–27% of POC could evade surface remineralization within the top 200 m and potentially be exported to depths beyond the mesopelagic region, model estimates suggest that ∼3.3% of it could reach hadal depths. Our results provide a quantitative baseline of pelagic‐benthic coupling which can aid in assessment of carbon cycling changes in future climate scenarios.more » « less
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            Lake water chemistry was measured for lakes in Iceland. We used a multiparameter probe (HydroLab HL4, OTT HydroMet) to measure in situ temperature, pH, dissolved oxygen (DO), and electrical conductivity of the water column at 0.5-1 m resolution. These measurements were repeated during each field campaign, resulting in multiple years of summer water chemistry data for many lakes. For some lakes, profiles of the water column were additionally taken through the ice during a February field campaign. Additionally, 0.5-1L grab samples of surface and bottom waters were analyzed for Total Phosphorus (mg/L), Chloride (mg/L), Nitrate (mg/L), Sulfate (mg/L), TOC/DOC (mg/L), and Total Nitrogen (mg/L).more » « less
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