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Keywords: Black carbon, Dissolved organic carbon, BPCAs, Mackenzie River, Beaufort Sea, Climate changeClimate change is amplified in the arctic and boreal regions. This causes higher average temperatures and less precipitation in the summer months and is resulting in longer wildfire seasons, severity, frequency and extent. This increases the relies of carbon into the atmosphere as greenhouse gases and aerosols, amplifying climate change even further. Black carbon (BC) is a fraction of organic carbon, resulting from the incomplete combustion of biomass and fossil fuels. BC may be inaccessible for biodegradation, because of its highly condensed aromatic molecular structure and therefore stores carbon on long timescales on land and in the ocean. BC is produced on land, but is transported as dissolved BC (DBC) by the rivers to the oceans, where it cycles on millennial timescales, sequestering BC. Thus, it is important to understand the significance of BC in the context of increased fires in this vulnerable region in the face of climate change.The Mackenzie River is a major source of terrestrial dissolved organic carbon (DOC) and the largest source of sediments to the Arctic Ocean. Here, we resolve the cycling of riverine DBC from the Mackenzie River to its fate in the Beaufort Sea, and the influence of mixing with Pacific water masses entering from the Chukchi Sea. We present DBC concentration data in ocean water, which was collected on two cruises in the Beaufort Sea in 2021 and 2022 covering the outflow of the Mackenzie River.For DBC concentrations, we digested solid phase extracts of DOC with nitric acid to oxidize BC molecules into benzenepolycarboxylic acids (BPCAs), which were then quantified on High Performance Liquid Chromatography (HPLC). We compare the concentrations of the DBC and DOC to trace the mixing of DBC river outflow with the ocean water. Since DBC originates on land and is relatively stable to biodegradation we can resolve the pathways of DBC from the Mackenzie River to the Arctic Ocean.

The residence time of carbon in terrestrial ecosystems, such as soils and freshwater, sets the pace of the terrestrial carbon cycle. Understanding export pathways and turnover times of soil organic carbon (OCSoil) is crucial to assess responses to climate and land use changes. Our study aims to quantify the average turnover time of OCSoil in the catchment of perialpine Lake Constance. Lake sedimentary sequences integrate organic carbon from their catchment and aquatic primary productivity. They act as both burial sites of organic carbon (OC) and time series archives of catchment processes. Thus, they can bridge the gap between plot scale observations, e.g., on soil carbon turnover, and observations made at the outlet of major river systems.Sedimentary organic carbon sources include aquatic primary productivity, OCSoil, and rock-derived (petrogenic) OC. Stable carbon isotopes (δ13C) can be used to identify the relative contribution of these pools. The 5700-year half-life of radiocarbon (14C) coupled with the atmospheric nuclear bomb spike in the early 1960s can be used to infer the age and turnover rate of the OC pools on millennial to annual timescales. Bulk OC isotope analysis of a varved sediment core spanning the past ca. 110 years at quasi-annual resolution was used to constrain the age of soil carbon delivered to Lake Constance. We combined the geochemical data with a Markov-Chain-Monte-Carlo-based approach to identify the most probable age structure of aquatic and soil-derived OC components and to quantify their respective contributions in addition to petrogenic OC.Radiocarbon analysis of sedimentary bulk OC reveals a well-defined but muted bomb spike in the early 1960s. However, bulk Δ14COC values remain below 0‰, implying a predominance of aged OC. Based on the δ13C-based three-component linear mixing model, we found these values to be the result of an OC mixture containing approx. 40% pre-aged soil carbon and up to 20% fossil petrogenic carbon. Accounting for these inputs, we estimated that soil-derived OC delivered to Lake Constance is centennial in age, implying interim storage prior or subsequent to erosion from the landscape.

Radiocarbon measurements of dissolved organic carbon (DOC) can give us valuable information about origin and age of DOC, a major, yet little understood component in the global carbon cycle. One way to measure DOC in water is to remove dissolved inorganic carbon first, oxidize organic carbon with UV irradiation and ultimately analyses the formed inorganic CO2 for 14C. The main challenge of UV-Oxidation (UVox) methods is to extract the typically low concentrations of DOC with low blanks required for relatively high precision 14C measurements. A disadvantage of currently used UVox methods is that only one sample can be oxidized in a laborious process at the same time in large volume. Here we present a UV-Oxidation system where up to 12 water samples can be oxidized simultaneously in 12 separate quartz reactors arranged around a single UV lamp in a compact setup. The simple setup further uses helium instead of vacuum typically used by conventional extraction lines to speed up the extraction of the formed CO2 after oxidation. The key improvements of the new UVox setup are: 1) Reduced amount of water needed (30- 60 ml) as samples are measured for 14C with the Micadas gas ion source., 2) UV oxidation efficiency for standards is high (96%), 3) No KI trap is needed, 4) Required time for sample preparation of up to 12 samples is 4-6 h, 5) combined the CO2 from different reactors to one trap. We obtained 2.6 ± 0.6 µgC with F14C= 0.27±0.05 for processing blank. We will present the first measurments of DOC samples from Swiss lakes, Canadian Beaufort Sea and the reproducibility of the line.

Arctic rivers provide an integrated signature of the changing landscape and transmit signals of change to the ocean. Here, we use a decade of particulate organic matter (POM) compositional data to deconvolute multiple allochthonous and autochthonous pan-Arctic and watershed-specific sources. Constraints from carbon-to-nitrogen ratios (C:N), δ13C, and Δ14C signatures reveal a large, hitherto overlooked contribution from aquatic biomass. Separation in Δ14C age is enhanced by splitting soil sources into shallow and deep pools (mean ± SD: -228 ± 211 vs. -492 ± 173‰) rather than traditional active layer and permafrost pools (-300 ± 236 vs. -441 ± 215‰) that do not represent permafrost-free Arctic regions. We estimate that 39 to 60% (5 to 95% credible interval) of the annual pan-Arctic POM flux (averaging 4,391 Gg/y particulate organic carbon from 2012 to 2019) comes from aquatic biomass. The remainder is sourced from yedoma, deep soils, shallow soils, petrogenic inputs, and fresh terrestrial production. Climate change-induced warming and increasing CO2 concentrations may enhance both soil destabilization and Arctic river aquatic biomass production, increasing fluxes of POM to the ocean. Younger, autochthonous, and older soil-derived POM likely have different destinies (preferential microbial uptake and processing vs. significant sediment burial, respectively). A small (~7%) increase in aquatic biomass POM flux with warming would be equivalent to a ~30% increase in deep soil POM flux. There is a clear need to better quantify how the balance of endmember fluxes may shift with different ramifications for different endmembers and how this will impact the Arctic system., Proceedings of the National Academy of Sciences of the United States of America, 120 (12), ISSN:0027-8424, ISSN:1091-6490

We present new high-resolution pollen records combined with palaeoceanographic proxies from the same samples in deep-sea cores SHAK06-5K and MD01-2444 on the southwestern Iberian Margin, documenting regional vegetation responses to orbital and millennial-scale climate changes over the last 28 ka. The chronology of these records is based on high-resolution radiocarbon dates of monospecific samples of the planktonic foraminifera Globigerina bulloides, measured from SHAK06-5K and MD01-2444 and aligned using an automated stratigraphical alignment method. Changes in temperate and steppe vegetation during Marine Isotope Stage 2 are closely coupled with sea surface temperature (SST) and global ice-volume changes. The peak expansion of thermophilous woodland between similar to 10.1 and 8.4 cal ka BP lags behind the boreal summer insolation maximum by similar to 2 ka, possibly arising from residual high-latitude ice-sheets into the Holocene. Rapid changes in pollen percentages are coeval with abrupt transitions in SSTs, precipitation and winter temperature at the onset and end of Heinrich Stadial 2, the ice-rafted debris event and end of Heinrich Stadial 1, and the onset of the Younger Dryas, suggesting extrinsically forced southwestern Iberian ecosystem changes by abrupt North Atlantic climate events. In contrast, the abrupt decline in thermophilous elements at similar to 7.8 cal ka BP indicates an intrinsically mediated abrupt vegetation response to the gradually declining boreal insolation, potentially resulting from the crossing of a seasonality of precipitation threshold. (C) 2021 The Authors. Journal of Quaternary Science Published by John Wiley & Sons, Ltd., Journal of Quaternary Science, 37 (3), ISSN:0267-8179, ISSN:1099-1417

Lateral particle transport in shelf/slope settings of marginal sea systems may potentially supply allochthonous particulate organic carbon (POC) to the ocean interior. The magnitude and prevalence of such processes has implications for our understanding of the functioning and efficiency of modern biological carbon pump processes, as well as for interpretation of deep ocean sediment records. Yet, ages and relative contribution of POC from different sources to deep ocean basins are much less understood. Here, based on radiocarbon (F-m, fraction modern), stable carbon (delta C-13(org)), and other geochemical analysis of particles intercepted by time-series sediment traps deployed at three different depths (1,000, 2,150, and 3,200 m), we constrain the source of the sinking POC in the deep basin of northern South China Sea (SCS). The results show that the modern POC derived from surface ocean productivity, acting as the vertical vector, accounts for 87% +/- 4% of sinking POC on average, while the lateral vector (aged POC hosted on resuspended sediment) comprises the remainder (13%). The contribution of laterally supplied POC increases with depth and is composed of aged POC derived from several sources. The majority stems from sediment resuspension of the northeastern SCS slope, that entrains aged marine POC (dominant), fossil OC, and soil OC (least significant). The diminished proportion of fossil OC in deep basin sinking POC relative to Taiwan-proximal areas is likely due to its dispersion via resuspension-deposition loops and dilution by POC stemming from modern surface ocean productivity during the delivery., Journal of Geophysical Research: Oceans, 127 (8), ISSN:0148-0227, ISSN:2169-9275

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 (≤63 μm) 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.

Collapse of permafrost coasts delivers large quantities of particulate organic carbon (POC) to Arctic coastal areas. With rapidly changing environmental conditions, sediment and organic carbon (OC) mobilization and transport pathways are also changing. Here, we assess the sources and sinks of POC in the highly dynamic nearshore zone of Herschel Island‐Qikiqtaruk (Yukon, Canada). Our results show that POC concentrations sharply decrease, from 15.9 to 0.3 mg L−1, within the first 100–300 m offshore. Simultaneously, radiocarbon ages of POC drop from 16,400 to 3,600 14C years, indicating rapid settling of old permafrost POC to underlying sediments. This suggests that permafrost OC is, apart from a very narrow resuspension zone (, Key Points Suspended particulate organic carbon (POC) sharply decreases in age and concentration within the nearshore zoneBeyond a narrow resuspension zone, permafrost‐derived OC dominates surface sediments, whereas much younger OC is found in the water columnPermafrost‐derived POC is rapidly removed from the water column, showing the critical role of nearshore dynamics for OC transport

The cycle of organic carbon through the atmosphere, oceans, continents and mantle reservoirs is a hallmark of Earth. Over geological time, chemical exchanges between those reservoirs have produced a diversity of reduced carbon materials that differ in their molecular structures and reactivity. This reactive complexity challenges the canonical dichotomy between the surface and deep, short-term and long-term organic carbon cycle. Old and refractory carbon materials are not confined to the lithosphere but are ubiquitous in the surface environment, and the lithosphere hosts various forms of reduced carbon that can be very reactive. The biological and geological pathways that drive the organic carbon cycle have changed through time; from a synthesis of these changes, it emerges that although a biosphere is required to produce organic carbon, mortality is required to ensure its export to the lithosphere, and graphitization is essential for its long-term stabilization in the solid Earth. Among the by-products of the organic carbon cycle are the accumulation of a massive lithospheric reservoir of organic carbon, the accumulation of dioxygen in the atmosphere and the rise of a terrestrial biosphere. Besides driving surface weathering reactions, free dioxygen has allowed the evolution of new metabolic pathways to produce and respire organic carbon. From the evolution of photosynthesis until the expansion of biomineralization in the Phanerozoic, inorganic controls on the organic carbon cycle have diversified, tightening the connection between the biosphere and geosphere. A review of the organic carbon cycle explores the interactions between the Earth’s surface and deeper reservoirs, the expanding inorganic controls on the organic carbon cycle, and how these links have strengthened through geological time.

The number of sedimentary records collected along the Brazilian continental margin has increased significantly in recent years, but relatively few are located in shallow waters and register paleoceanographic processes in the outer shelf–middle slope prior to 10–15 ka. For instance, the northward flow up to 23–24∘ S of cold and fresh shelf waters sourced from the Subantarctic region is an important feature of current hydrodynamics in the subtropical western South Atlantic Ocean, and yet limited information is available for the long-term changes of this system. Herein, we considered a suite of organic and inorganic proxies – alkenones-derived sea surface temperature (SST), δD-alkenones, δ18O of planktonic foraminifera, and ice-volume free seawater δ18OIVF−SW – in sediment from two cores (RJ-1501 and RJ-1502) collected off the Rio de Janeiro Shelf (SE Brazilian continental shelf) to shed light on SST patterns and relative salinity variations since the end of the last glacial cycle in the region and the implications of these processes over a broader spatial scale. The data indicate that, despite the proximity (∼40 km apart) of both cores, apparently contradictory climatic evolution occurred at the two sites, with the shallower (deeper) core RJ-1501 (RJ-1502) showing consistently cold (warm) and fresh (salt) conditions toward the Last Glacial Maximum (LGM) and last deglaciation. This can be reconciled by considering that the RJ-1501 core registered a signal from mid- to high latitudes on the upper slope off Rio de Janeiro represented by the influence of the cold and fresh waters composed of Subantarctic Shelf Water and La Plata Plume Water transported northward by the Brazilian Coastal Current (BCC). The data from core RJ-1502 and previous information for deep-cores from the same region support this interpretation. In addition, alkenone-derived SST and δ18OIVF−SW suggest a steep thermal and density gradient formed between the BCC and Brazil Current (BC) during the last climate transition which, in turn, may have generated perturbations in the air–sea heat flux with consequences for the regional climate of SE South America. In a scenario of future weakening of the Atlantic Meridional Overturning Circulation, the reconstructed gradient may become a prominent feature of the region., Climate of the Past, 16 (4), ISSN:1814-9324, ISSN:1814-9332

The storage of organic carbon in the terrestrial biosphere directly affects atmospheric concentrations of carbon dioxide over a wide range of timescales. Within the terrestrial biosphere, the magnitude of carbon storage can vary in response to environmental perturbations such as changing temperature or hydroclimate1, potentially generating feedback on the atmospheric inventory of carbon dioxide. Although temperature controls the storage of soil organic carbon at mid and high latitudes2,3, hydroclimate may be the dominant driver of soil carbon persistence in the tropics4,5; however, the sensitivity of tropical soil carbon turnover to large-scale hydroclimate variability remains poorly understood. Here we show that changes in Indian Summer Monsoon rainfall have controlled the residence time of soil carbon in the Ganges-Brahmaputra basin over the past 18,000 years. Comparison of radiocarbon ages of bulk organic carbon and terrestrial higher-plant biomarkers with co-located palaeohydrological records6 reveals a negative relationship between monsoon rainfall and soil organic carbon stocks on a millennial timescale. Across the deglaciation period, a depletion of basin-wide soil carbon stocks was triggered by increasing rainfall and associated enhanced soil respiration rates. Our results suggest that future hydroclimate changes in tropical regions are likely to accelerate soil carbon destabilization, further increasing atmospheric carbon dioxide concentrations.

Aged organic carbon (OC) is widely observed in surficial sediments deposited on continental margins, resulting from several factors including old OC input and sedimentological processes. While the supply of old OC to marine sediments has been examined and quantified in a range of continent margin settings, there have been few attempts to constrain the extent to which hydrodynamic processes, specifically lateral transport, contribute to the old age of sedimentary OC. Here, we propose a mathematical index, bAgedOC, to differentiate the causes of sedimentary aged OC, and apply this approach to two typical sediment transport pathways that follow the supply and dispersal of terrestrial OC in the marine environment, and further extrapolate it to submarine canyon, Arctic and deep-sea environments. The index, representing a modification of a widely used quantitative method, provides a novel approach to distinguish the contribution of lateral transport to the pre-depositional aging of OC in the oceanic region. ISSN:0094-8276 ISSN:1944-8007

Sources of dissolved and particulate carbon to the Fraser River system vary significantly in space and time. Tributaries in the northern interior of the basin consistently deliver higher concentrations of dissolved organic carbon (DOC) to the main stem than other tributaries. Based on samples collected near the Fraser River mouth throughout 2013, the radiocarbon age of DOC exported from the Fraser River does not change significantly across seasons despite a spike in DOC concentration during the freshet, suggesting modulation of heterogeneous upstream chemical and isotopic signals during transit through the river basin. Dissolved inorganic carbon (DIC) concentrations are highest in the Rocky Mountain headwater region where carbonate weathering is evident, but also in tributaries with high DOC concentrations, suggesting that DOC respiration may be responsible for a significant portion of DIC in this basin. Using an isotope and major ion mass balance approach to constrain the contributions of carbonate and silicate weathering and DOC respiration, we estimate that up to 33 +/- 11% of DIC is derived from DOC respiration in some parts of the Fraser River basin. Overall, these results indicate close coupling between the cycling of DOC and DIC, and that carbon is actively processed and transformed during transport through the river network., Biogeochemistry, 164 (1), ISSN:0168-2563, ISSN:1573-515X

Arctic rivers will be increasingly affected by the hydrological and biogeochemical consequences of thawing permafrost. During transport, permafrost-derived organic carbon (OC) can either accumulate in floodplain and shelf sediments or be degraded into greenhouse gases prior to final burial. Thus, the net impact of permafrost OC on climate will ultimately depend on the interplay of complex processes that occur along the source-to-sink system. Here, we focus on the Kolyma River, the largest watershed completely underlain by continuous permafrost, and marine sediments of the East Siberian Sea, as a transect to investigate the fate of permafrost OC along the land-ocean continuum. Three pools of riverine OC were investigated for the Kolyma main stem and five of its tributaries: dissolved OC (DOC), suspended particulate OC (POC), and riverbed sediment OC (SOC). They were compared with earlier findings in marine sediments. Carbon isotopes (δ13C, Δ14C), lignin phenol, and lipid biomarker proxies show a contrasting composition and degradation state of these different carbon pools. Dual C isotope source apportionment calculations imply that old permafrost-OC is mostly associated with sediments (SOC; contribution of 68±10%), and less dominant in POC (38±8%), whereas autochthonous primary production contributes around 44±10% to POC in the main stem and up to 79±11 % in tributaries. Biomarker degradation indices suggest that Kolyma DOC might be relatively degraded, regardless of its generally young age shown by previous studies. In contrast, SOC shows the lowest Δ14C value (oldest OC), yet relatively fresh compositional signatures. Furthermore, decreasing mineral surface area-normalised OC- and biomarker loadings suggest that SOC might be reactive along the land-ocean continuum and almost all parameters were subjected to rapid change when moving from freshwater to the marine environment. This suggests that sedimentary dynamics play a crucial role when targeting permafrost-derived OC in aquatic systems and support earlier studies highlighting the fact that the land-ocean transition zone is an efficient reactor and a dynamic environment. The prevailing inconsistencies between freshwater and marine research (i.e. targeting predominantly DOC and SOC respectively) need to be better aligned in order to determine to what degree thawed permafrost OC may be destined for long-term burial, thereby attenuating further global warming., Biogeosciences, 20 (1), ISSN:1726-4170

Erosion and riverine transport of organic carbon is an important component of the global carbon cycle, but the significance of this process for Earth's surface carbon budgets depends on the sources of carbon being mobilised. In this study, we aim to constrain how runoff-driven erosion modulates the contribution of different carbon source endmembers, i.e., bedrock, soil and vegetation, in three forested headwater catchments in the Swiss Prealps. The sources of organic carbon are determined using an inverse model based on bulk carbon isotope signatures and the abundances and distributions of long-chain n-alkane plant wax biomarkers in suspended sediments collected over a range of discharges. Despite landcover differences and contrasting bulk particulate organic carbon (POC) signatures, the increase of soil-sourced organic carbon with discharge is similar in all three studied catchments. This apparent existence of common processes implies that export fluxes of soil organic carbon may be extrapolated to similar catchments. Overall, our analysis shows that runoff-driven soil erosion in these alpine headwater streams is responsible for the export of ca. 0.3 to 0.8 gC m-2 a-1 as POC, which represents ca. 0.1 - 0.3 % of carbon fixed by NPP. Most of this soil OC export occurs during high-discharge events. Our study also shows that despite a significant variability in isotopic and molecular POC signatures at low discharge, all three catchments show a convergence of these signatures at higher discharges. Suspended sediment samples collected at above-average discharges are hence most representative of overall endmember contributions., Journal of Geophysical Research: Biogeosciences, 127 (3), ISSN:0148-0227, ISSN:2169-8953, ISSN:2169-8961

Identifying drivers of seasonal variations in fluvial particulate organic carbon (POC) composition can aid sediment provenance and biogeochemical cycling studies. We evaluate seasonal changes in POC composition in the Río Bermejo, Argentina, a lowland river running ∼1,270 km without tributaries. Weekly POC concentration and isotopic composition from 2016 to 2018 show that during the wet season, increased lateral channel migration generates an influx of 13C-enriched and 14C-enriched floodplain-sourced material, overprinting the 13C-depleted and 14C-depleted headwater signature that is observed during the dry season. These findings demonstrate how channel morphodynamics can drive variability of POC composition in lowland rivers, and may modulate the composition of POC preserved in sedimentary archives., Geophysical Research Letters, 48 (24), ISSN:0094-8276, ISSN:1944-8007

Interactions between organic and detrital mineral phases strongly influence both the dispersal and accumulation of terrestrial organic carbon (OC) in continental margin sediments. Yet the complex interplay among biological, chemical, and physical processes limits our understanding of how organo-mineral interactions evolve during sediment transfer and burial. In particular, diverse OC sources and complex hydrodynamic processes hinder the assessment of how the partnership of organic matter and its mineral host evolves during supply and dispersal over continental margins. In this study, we integrate new and compiled sedimentological (grain size, surface area), organic (%OC, OC-δ13C, OC-F14C), and inorganic isotopic (εNd, 87Sr/86Sr) geochemical data for a broad suite of surface sediments spanning the Western Arctic Ocean from the Bering Sea to the Mackenzie River Delta that capture diverse sources and ages of both terrestrial and marine material deposited in contrasting shelf and slope settings. Spatial gradients in sediment properties were used to delineate regional sources and transport processes influencing the dispersion and persistence of OC-mineral particle associations during export and burial. We found strong relationships between physical parameters, aluminum content, and OC-14C suggesting that terrestrial OC remains tightly associated with its detrital mineral carrier during source-to-sink transport. Notably, carbon and neodymium isotopic data yield consistent information regarding organic matter provenance. Results obtained highlight the potential for coupled organic-inorganic tracer measurements to elucidate sediment sources and to constrain physical and geochemical processes during sediment mobilization and transport in the Western Arctic Ocean. Tandem measurements of carbon and Nd isotopes may provide a new way to identify large-scale biogeochemical and ecological changes in the sources, nature, and fate of OC stemming from predicted increases in sea ice loss and fluvial inputs of dissolved and particulate OC to this complex and dynamic high latitude marginal sea. ISSN:0016-7037 ISSN:1872-9533

Rivers transfer terrestrial organic carbon (OC) from mountains to ocean basins, playing a key role in the global carbon cycle. During fluvial transit, OC may be oxidized and emitted to the atmosphere as CO2 or preserved and transported to downstream depositional sinks. The balance between oxidation and preservation determines the amount of particulate OC (POC) that can be buried long term, but the factors regulating this balance are poorly constrained. Here, we quantify the effects of fluvial transit on POC fluxes along an ~1,300 km lowland channel with no tributaries. We show that sediment transit time and mineral protection regulate the magnitude and rate of POC oxidation, respectively. Using a simple turnover model, we estimate that annual POC oxidation is a small percentage of the POC delivered to the river. Modelling shows that lateral erosion into POC-rich floodplains can increase POC fluxes to downstream basins, thereby offsetting POC oxidation. Consequently, rivers with high channel mobility can enhance CO2 drawdown while management practices that stabilize river channels may reduce the potential for CO2 drawdown., Nature Geoscience, 14 (11), ISSN:1752-0908, ISSN:1752-0894

The erosion and weathering of mountain ranges exert a key control on the long-term (105–106 yr) cycling of carbon between Earth’s surface and crust. The net carbon budget of a mountain range reflects the co-existence of multiple carbon sources and sinks, with corresponding fluxes remaining difficult to quantify. Uncertain responses of these carbon fluxes due to the stochastic nature of erosional processes further complicate the extrapolation of short-term observations to longer, climatically relevant timescales. Here, we quantify the evolution of the organic and inorganic carbon fluxes in response to the 2015 Gorkha earthquake (Mw 7.8) in the central Himalaya. We find that the Himalayan erosion acts as a net carbon sink due mainly to efficient biospheric organic carbon export. Our high-resolution time series encompassing four monsoon seasons before and after the Gorkha earthquake reveal that coseismic landslides did not significantly perturb large-scale Himalayan sediment and carbon fluxes. This muted response of the central Himalaya to a geologically frequent perturbation such as the Gorkha earthquake further suggests that our estimates are representative of at least interglacial timescales. Carbon fluxes in the central Himalaya did not change after the 2015 Gorkha earthquake and its accompanying landslides, according to observations of riverine sediment and carbon fluxes over four monsoon seasons spanning the event.

Burial of terrestrial organic carbon (OCterr) in marginal sea sediments is a key component of the carbon cycle, exerting long-term influence on atmospheric CO2 and climate. Assessment of the burial efficiency of OCterr is of key importance, yet remains poorly constrained due to current gaps in our knowledge of mechanistic controls, including the influence of organic matter composition and age on the fate of OCterr in marine sediments. We measured bulk characteristics (δ13C and Δ14C of OC; mineral surface area, SA; grain size; n = 98 samples) and biomarker carbon isotopic compositions (fatty acid δ13C and Δ14C; n = 11) of a suite of surface sediment samples from the Bohai Sea and Yellow Sea (BS-YS). Combining with published results, bulk OC (n = 234) and biomarker (n = 19) carbon isotopic data are used to examine spatial variability in the sources and ages of OCterr in this shallow marginal sea system. Biomarker carbon isotopic values are used to constrain endmember values, and a dual carbon isotope mixing model was applied to all bulk samples to develop a spatially explicit assessment of contributions of different pools of OCterr. Although highly spatially variable, pre-aged OC (OCpre-aged) and fossil OC (OCfossil) when combined (i.e., “non-modern OC”) on average accounted for 51 ± 10% of the OC in BS-YS surface sediments. This was equivalent to the proportion of OCterr (ave., 51 ± 14%) estimated from a δ13COC binary mixing model, suggesting OCterr in the mixed layer of BS-YS sediments is predominantly composed of millennial-aged OC. The burial potential of pool-specific OCterr was then evaluated through comparison of corresponding mineral SA-normalized loadings of surface sediments with those of Yellow River suspended particulate matter. Both the regression slope and the arithmetic mean value approaches reveal high burial potential for all terrestrial OC pools delivered by Yellow River, which is attributed to the aged and refractory nature of OC exported from the Yellow River. However, differing relationships of pool-specific OCterr loadings between BS-YS and Yellow River sediments imply contrasting fates. In particular, we find that the burial potential of OCpre-aged is consistently greater than that of OCfossil. This surprising observation suggests either enhanced degradation of OCfossil during lateral transport (possibly as a consequence of different mineral associations and hydrodynamic sorting effects), or additional sources for OCpre-aged, such as from small rivers or aerosol deposition. Overall, OC age, mineralogical composition and hydrological settings contribute to the complex patterns of OC residing in northern China marginal sea surface sediments. This novel molecular-isotopic approach reveals significant spatial variability in proportions, contents and burial potential among terrestrial OC pools, and underlines the importance of considering organic matter age and composition in understanding and constraining the fate of OCterr in marine sedimentary environments., Geochimica et Cosmochimica Acta, 309, ISSN:0016-7037, ISSN:1872-9533

Alkenone signatures preserved in marine sedimentary records are considered one of the most robust paleothermometers available and are often used as a proxy for paleoproductivity. However, important gaps remain regarding the provenance and fate of alkenones, as well as their impact on derived environmental signals in marine sediments. Here, we analyze the abundance, distribution and radiocarbon (14C) age of alkenones in bulk sediments and corresponding grain-size fractions in surficial sediments from seven continental margin settings in the Pacific and Atlantic oceans to evaluate the impact of organo-mineral associations and hydrodynamic sorting on sedimentary alkenone signals. We find that alkenones preferentially reside within fine-grained mineral fractions of continental margin sediments, with the preponderance of alkenones residing within the fine-silt fraction (2–10 µm) and most strongly influencing alkenone-14C age and sea surface temperature (SST) signals from bulk sediments as a consequence of their proportional abundance and higher degree of organic matter protection relative to other fractions. Our results provide further evidence for the key role of selective association of alkenones with mineral surfaces and associated hydrodynamic mineral sorting processes on the reliability of alkenone signals encoded in marine sediments (14C age, content and distribution) and the fidelity of corresponding proxy records (productivity and sea SST) in the spatial and temporal domain., Biogeosciences, 19 (3), ISSN:1726-4170

Estuaries are action zones for organic carbon (OC) degradation and aging. These processes influence the nature of terrestrial OC (OCterr) export and the magnitude of OCterr burial in marginal seas, with important environmental implications such as CO2 release and hypoxia. In this study, we determined the contents and carbon isotopic compositions (C-13 and C-14) of bulk OC and fatty acids (FAs) as well as the sedimentological characteristics of suspended particulate matter (SPM) samples collected from two sites over four seasons and of surface sediment samples from three sites in the Pearl River estuary (PRE) to evaluate processes controlling OCterr degradation and aging along an estuarine gradient. We found that the abundance-weighted average C(24-32)FA C-14 ages increased by an average of similar to 1170 years for SPM and by an average of similar to 3440 years in PR/PRE sediments, along the similar to 60 km PRE transect. These increases in the FA age coincided with an 86% decrease in the corresponding mineral surface area-normalized FA loading along the sediment transport pathway, implying that selective degradation of labile and younger OC resulted in apparent OC aging. These measurements reveal an important shift in the nature of OC, with implications for biogeochemical cycling within estuaries and for regional environmental changes. ISSN:0013-936X ISSN:1520-5851

Glycerol Dialkyl Glycerol Tetraethers (GDGTs) are ubiquitous biomolecules whose structural diversity or isotopic composition is increasingly used to reconstruct environmental changes such as air temperature or pCO2. Isoprenoid GDGTs (iGDGT), in particular GDGT-0, are biosynthesized by a large range of Archaea. To assess the potential of GDGT-0 as a tracer of past methane cycle variations, three sediment cores from the Mackenzie River Delta have been studied for iGDGT and diploptene concentration, distribution and stable carbon signature. The absence of crenarchaeol, high GDGT-0 vs crenarchaeol ratio values, and 13C-enriched carbon signature of GDGT-0 indicate production by acetoclastic methanogens as well as heterotrophic Archaea. The oxidation of methane seems to be dominated by bacteria as indicated by the high abundance of 13C-depleted diploptene. Branched GDGTs (brGDGT), thought to be produced by heterotrophic bacteria, are dominated by hexa- and penta-methylated 5- and 6-methyl compounds. The presence of 5,6-methyl isomer IIIa’’ points towards in situ production of brGDGTs, with only a minor input from soil branched GDGT brought by the Mackenzie River. Carbon isotopic compositions of brGDGTs are in agreement with heterotrophic producers, likely living during summer. The reconstructed temperatures using a global lake calibration reflect recorded summer air temperature (± 2 °C) during the last 60 years, and further highlight the absence of warming in summer in this region during the last 200 years. Oxygen availability and connection time to the Mackenzie River also seem to control the distribution of brGDGT with an increase in 6-methyl and 5,6-methyl isomers during periods of increased anoxia., Organic Geochemistry, 157, ISSN:0146-6380

Tropical rivers deliver ∼60% of particulate organic carbon to the world ocean. However, compositions and loadings of sedimentary organic matter (OM) from tropical small mountainous rivers are largely unknown. Here, we provide an initial constrain on sources of sedimentary OM from 28 fluvial systems across Luzon in the Philippines by measuring total organic carbon (TOC), total nitrogen (TN), stable carbon isotope (δ13C) and radiocarbon activity of TOC (expressed as fraction modern—Fm), as well as grain size and mineral surface area (SA) of sediments. Results indicate that sediments in Luzon rivers contain both contemporary and 14C-depleted OM (Fm: 0.71–1.06, mean 0.97 ± 0.07) with a wide range of δ13C values (−28.3‰ to −17.7‰, −24.9 ± 2.2‰). This is attributed to the OM sources originated from modern surface soil and 14C-depleted subsoil and deep soil vegetated by C3 and C4 plants, with mean fraction of C3 plant at 80% ± 11%. Minor input from bedrock may also contribute to the 14C-depleted OM in sediments, accounting for 6% ± 6%. Sediments in most rivers are featured by low OC loadings (OC/SA ratio < 0.4 mg C m−2), owing either to a less OM input or intensive OM degradation. The estimated yields of particulate OC from Luzon vary between 3.2 and 3.7 t km−2 yr−1, which is higher than most tropical large rivers. © 2021 American Geophysical Union ISSN:0148-0227 ISSN:2169-8953 ISSN:2169-8961

Bound to rock Organic matter binds to phyllosilicates, a process which affects both its transport and chemical stability. How does that affect the fate of terrestrial organic carbon that enters the ocean? Blattmann et al. show that organic carbon derived from soils is stripped from mineral surfaces upon discharge and dispersal into the ocean, whereas organic matter derived from ancient rocks is preserved there. Their results show that preservation of continentally derived organic matter in marine sediments is controlled largely by phyllosilicate mineralogy. Science , this issue p. 742

Hydrodynamic sorting has been shown to strongly influence the composition and age of organic carbon (OC) during sediment transport and burial in the marine environment, yet sorting effects on terrestrial OC (OCterr) in fluvial systems remain poorly understood. We conducted size fractionation of suspended particle samples from the lower Yellow River, China, and examined variations in mass distribution and carbon isotopic (δ13C and Δ14C) composition of bulk OC and specific biomarkers among grain size fractions in order to investigate the influence of hydrodynamic sorting and selective transport on organic matter export. In general, the 16–32 μm and 32–63 μm fractions contributed the most of sediment mass while the majority of the OC resided in the 16–32 μm fraction. Over 80% of OC and n-fatty acids (FAs) were concentrated in 32 μm), characterized by relatively low SA, OC%, and Δ14COC values, but higher Δ14C values of C26+28+30 FAs, are inferred to reflect a combination of bedrock-derived detrital sediment and fresh vascular-plant material (e.g., plant fragments). In contrast, finer particles (

ISSN:0148-0227 ISSN:2169-8953 ISSN:2169-8961

Perylene is a frequently abundant, and sometimes the only polycyclic aromatic hydrocarbon (PAH) in aquatic sediments, but its origin has been subject of a longstanding debate in geochemical research and pollutant forensics because its historical record differs markedly from typical anthropogenic PAHs. Here we investigate whether perylene serves as a source-specific molecular marker of fungal activity in forest soils. We use a well-characterized sedimentary record (1735-1999) from the anoxic-bottom waters of the Pettaquamscutt River basin, RI to examine mass accumulation rates and isotope records of perylene, and compare them with total organic carbon and the anthropogenic PAH fluoranthene. We support our arguments with radiocarbon (