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Dissolved organic matter (DOM) in soils drives biogeochemical cycling and soil functions in different directions depending on its molecular signature. Notably, there is a distinct paucity of information concerning how the molecular signatures of soil DOM vary with different degrees of weathering across wide geographic scales. Herein, we resolved the DOM molecular signatures from 22 diverse Chinese reference soils and linked them with soil organic matter and weathering-related mineralogical properties. The mixed-effects models revealed that the yields of DOM were determined by soil organic carbon content, whereas the molecular signature of DOM was primarily constrained by the weathering-related dimension. The soil weathering index showed a positive effect on the lability and a negative effect on the aromaticity of DOM. Specifically, DOM in highly weathered acidic soils featured more amino sugars, carbohydrates, and aliphatics, as well as less O-rich polyphenols and condensed aromatics, thereby conferring a higher DOM biolability and lower DOM aromaticity. This study highlights the dominance of the weathering-related dimension in constraining the molecular signatures and potential functions of DOM in soils across a wide geographic scale.

Dissolved organic matter (DOM) in soils drives biogeochemical cycling and soil functions in different directions depending on its molecular signature. Notably, there is a distinct paucity of information concerning how the molecular signatures of soil DOM vary with different degrees of weathering across wide geographic scales. Herein, we resolved the DOM molecular signatures from 22 diverse Chinese reference soils and linked them with soil organic matter and weathering-related mineralogical properties. The mixed-effects models revealed that the yields of DOM were determined by soil organic carbon content, whereas the molecular signature of DOM was primarily constrained by the weathering-related dimension. The soil weathering index showed a positive effect on the lability and a negative effect on the aromaticity of DOM. Specifically, DOM in highly weathered acidic soils featured more amino sugars, carbohydrates, and aliphatics, as well as less O-rich polyphenols and condensed aromatics, thereby conferring a higher DOM biolability and lower DOM aromaticity. This study highlights the dominance of the weathering-related dimension in constraining the molecular signatures and potential functions of DOM in soils across a wide geographic scale.

Humid tropical forests play a dominant role in the functioning of Earth but are under increasing threat from changes in land use and climate. How forest vulnerability varies across space and time and what level of stress forests can tolerate before facing a tipping point are poorly understood. Here, we develop a tropical forest vulnerability index (TFVI) to detect and evaluate the vulnerability of global tropical forests to threats across space and time. We show that climate change together with land-use change have slowed the recovery rate of forest carbon cycling. Temporal autocorrelation, as an indicator of this slow recovery, increases substantially for above-ground biomass, gross primary production, and evapotranspiration when climate stress reaches a critical level. Forests in the Americas exhibit extensive vulnerability to these stressors, while in Africa, forests show relative resilience to climate, and in Asia reveal more vulnerability to land use and fragmentation. TFVI can systematically track the response of tropical forests to multiple stressors and provide early-warning signals for regions undergoing critical transitions.

Humid tropical forests play a dominant role in the functioning of Earth but are under increasing threat from changes in land use and climate. How forest vulnerability varies across space and time and what level of stress forests can tolerate before facing a tipping point are poorly understood. Here, we develop a tropical forest vulnerability index (TFVI) to detect and evaluate the vulnerability of global tropical forests to threats across space and time. We show that climate change together with land-use change have slowed the recovery rate of forest carbon cycling. Temporal autocorrelation, as an indicator of this slow recovery, increases substantially for above-ground biomass, gross primary production, and evapotranspiration when climate stress reaches a critical level. Forests in the Americas exhibit extensive vulnerability to these stressors, while in Africa, forests show relative resilience to climate, and in Asia reveal more vulnerability to land use and fragmentation. TFVI can systematically track the response of tropical forests to multiple stressors and provide early-warning signals for regions undergoing critical transitions.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

The cycling of carbon on Earth exerts a fundamental influence upon the greenhouse gas content of the atmosphere, and hence global climate over millennia. Until recently, ice sheets were viewed as inert components of this cycle and largely disregarded in global models. Research in the past decade has transformed this view, demonstrating the existence of uniquely adapted microbial communities, high rates of biogeochemical/physical weathering in ice sheets and storage and cycling of organic carbon (>104 Pg C) and nutrients. Here we assess the active role of ice sheets in the global carbon cycle and potential ramifications of enhanced melt and ice discharge in a warming world.

The cycling of carbon on Earth exerts a fundamental influence upon the greenhouse gas content of the atmosphere, and hence global climate over millennia. Until recently, ice sheets were viewed as inert components of this cycle and largely disregarded in global models. Research in the past decade has transformed this view, demonstrating the existence of uniquely adapted microbial communities, high rates of biogeochemical/physical weathering in ice sheets and storage and cycling of organic carbon (>104 Pg C) and nutrients. Here we assess the active role of ice sheets in the global carbon cycle and potential ramifications of enhanced melt and ice discharge in a warming world.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Evaluating the collective impact of small source inputs to larger rivers is a constant challenge in riverine biogeochemistry. In this study, we investigated the generation of dissolved organic matter (DOM) in a small oak woodland catchment in the foothills of northern California, the subsequent transformation in lignin biomarkers and chromophoric DOM (CDOM) parameters during transport through the landscape to an exporting stream, and finally the overall compositional impact on the larger receiving stream and river. Our study included a natural leaching experiment in which precipitation passing through oak, pine, and grass litter and duff samples was collected after each of a series of storms. Also included were soil trench samples to capture subsurface lateral flow, stream samples along with point-source reservoir inputs, and samples of canopy throughfall, stemflow, and gopher hole (bypass) flow. The litter/duff leaching study demonstrated changing DOM fractionation patterns throughout the season, as evidenced by changing lignin compositions in the leachates with each successive storm. This adds a necessary seasonal component to interpreting lignin compositions in streams, as the source signatures are constantly changing. Released DOM from leaching was modified extensively during transit through the subsurface to the stream, with preferential increases in aromaticity as evidenced by increases in carbon-normalized absorbance at 254 nm, yet preferential decreases in lignin phenols, as evidence by carbon-normalized lignin yields in the headwater stream that was less than half that of the litter/duff leachates. Our extensive number of lignin measurements for source materials reveals a much more complex perspective on using lignin as a source indicator, as many riverine values for syringyl:vanillyl and cinnamyl:vanillyl ratios that have previously been interpreted as degraded lignin signatures are also possible as unmodified source signatures. Finally, this study demonst

Evaluating the collective impact of small source inputs to larger rivers is a constant challenge in riverine biogeochemistry. In this study, we investigated the generation of dissolved organic matter (DOM) in a small oak woodland catchment in the foothills of northern California, the subsequent transformation in lignin biomarkers and chromophoric DOM (CDOM) parameters during transport through the landscape to an exporting stream, and finally the overall compositional impact on the larger receiving stream and river. Our study included a natural leaching experiment in which precipitation passing through oak, pine, and grass litter and duff samples was collected after each of a series of storms. Also included were soil trench samples to capture subsurface lateral flow, stream samples along with point-source reservoir inputs, and samples of canopy throughfall, stemflow, and gopher hole (bypass) flow. The litter/duff leaching study demonstrated changing DOM fractionation patterns throughout the season, as evidenced by changing lignin compositions in the leachates with each successive storm. This adds a necessary seasonal component to interpreting lignin compositions in streams, as the source signatures are constantly changing. Released DOM from leaching was modified extensively during transit through the subsurface to the stream, with preferential increases in aromaticity as evidenced by increases in carbon-normalized absorbance at 254 nm, yet preferential decreases in lignin phenols, as evidence by carbon-normalized lignin yields in the headwater stream that was less than half that of the litter/duff leachates. Our extensive number of lignin measurements for source materials reveals a much more complex perspective on using lignin as a source indicator, as many riverine values for syringyl:vanillyl and cinnamyl:vanillyl ratios that have previously been interpreted as degraded lignin signatures are also possible as unmodified source signatures. Finally, this study demonst

The Siberian Arctic contains a globally significant pool of organic carbon (OC) vulnerable to enhanced warming and subsequent release by both fluvial and coastal erosion processes. However, the rate of release, its behaviour in the Arctic Ocean and vulnerability to remineralisation is poorly understood. Here we combine new measurements of microbial biohopanoids including adenosylhopane, a lipid associated with soil microbial communities, with published glycerol dialkyl glycerol tetraethers (GDGTs) and bulk δ13C measurements to improve knowledge of the fate of OC transported to the East Siberian Arctic Shelf (ESAS). The microbial hopanoid-based soil OC proxy R'soil ranges from 0.0 to 0.8 across the ESAS, with highest values nearshore and decreases offshore. Across the shelf R'soil displays a negative linear correlation with bulk δ13C measurements (r2 Combining double low line -0.73, p Combining double low line < 0.001). When compared to the GDGT-based OC proxy, the branched and isoprenoid tetraether (BIT) index, a decoupled (non-linear) behaviour on the shelf was observed, particularly in the Buor-Khaya Bay, where the R'soil shows limited variation, whereas the BIT index shows a rapid decline moving away from the Lena River outflow channels. This reflects a balance between delivery and removal of OC from different sources. The good correlation between the hopanoid and bulk terrestrial signal suggests a broad range of hopanoid sources, both fluvial and via coastal erosion, whilst GDGTs appear to be primarily sourced via fluvial transport. Analysis of ice complex deposits (ICDs) revealed an average R'soil of 0.5 for the Lena Delta, equivalent to that of the Buor-Khaya Bay sediments, whilst ICDs from further east showed higher values (0.6-0.85). Although R'soil correlates more closely with bulk OC than the BIT, our understanding of the endmembers of this system is clearly still incomplete, with variations between the different East Siberian Arctic regions potentially

The Siberian Arctic contains a globally significant pool of organic carbon (OC) vulnerable to enhanced warming and subsequent release by both fluvial and coastal erosion processes. However, the rate of release, its behaviour in the Arctic Ocean and vulnerability to remineralisation is poorly understood. Here we combine new measurements of microbial biohopanoids including adenosylhopane, a lipid associated with soil microbial communities, with published glycerol dialkyl glycerol tetraether (GDGTs) and bulk δ13C 5 measurements to improve knowledge of the fate of OC transported to the East Siberian Arctic Shelf (ESAS). The microbial hopanoid-based soil OC proxy R'soil ranges from 0.0 to 0.8 across the ESAS, with highest values near shore and decreases offshore. Across the shelf R'soil displays a negative linear correlation with bulk δ13C measurements (r2 = −0.73, p = < 0.001). When compared to the GDGT based OC proxy, the Branched and Isoprenoid tetraether (BIT) index, a decoupled (non-linear) behaviour on the shelf was observed, particularly in the Buor-Khaya Bay where the R'soil shows limited 10 variation, whereas the BIT index shows a rapid decline moving away from the Lena River outflow channels. This reflects a balance between delivery and removal of OC from different sources. The good correlation between the hopanoid and bulk terrestrial signal suggests a broad range of hopanoid sources, both fluvial and via coastal erosion whilst GDGTs appear to be primarily sourced via fluvial transport. Analysis of ice complex deposits (ICDs) revealed an average R'soil of 0.5 for the Lena delta, equivalent to that of the Buor-Khaya Bay sediments, whilst ICDs from further East showed higher values (0.6–0.85). Al15 though R'soil correlates more closely with bulk OC than the BIT, our understanding of the endmembers of this system is clearly still incomplete with east-west variations potentially reflecting differences in environmental conditions (e.g. temperature, pH) but other ph

Rivers play a major role in the transport and processing of dissolved organic matter (DOM). Disturbances that impact DOM dynamics, such as river impoundments and flow regulation, have consequences for biogeochemical cycling and aquatic ecosystems. In this study we examined how river impoundments and hydrologic regulation impact DOM quantity and quality by tracking spatial and seasonal patterns of DOM in a large, regulated river (Klamath River, USA). Dissolved organic carbon (DOC) concentrations decreased downstream and longitudinal patterns in DOC load varied by season. Export of DOM (as DOC) was largely driven by river flow, while DOM composition was strongly influenced by impoundments. Seasonal algal blooms in upstream lentic reaches provided a steady source of algal DOM that was processed in downstream reaches. DOM at upstream sites had an average spectral slope ratio (SR) > 1, indicating algal-derived material, but decreased downstream to an average SR < 1, more indicative of terrestrial-derived material. The increasingly terrestrial nature of DOM exported from reservoirs likely reflects degraded algal material that becomes increasingly more recalcitrant with distance from upstream source and additional processing. As a result, DOM delivered to free-flowing river reaches below impoundments was less variable in composition. Downstream of impoundments, tributary influences resulted in increasing contributions of terrestrial DOM from the surrounding watershed. Removal of the four lower dams on the Klamath River is scheduled to proceed in the next decade. These results suggest that management should consider the role of impoundments on altering DOM dynamics, particularly in the context of dam removal.

Rivers play a major role in the transport and processing of dissolved organic matter (DOM). Disturbances that impact DOM dynamics, such as river impoundments and flow regulation, have consequences for biogeochemical cycling and aquatic ecosystems. In this study we examined how river impoundments and hydrologic regulation impact DOM quantity and quality by tracking spatial and seasonal patterns of DOM in a large, regulated river (Klamath River, USA). Dissolved organic carbon (DOC) concentrations decreased downstream and longitudinal patterns in DOC load varied by season. Export of DOM (as DOC) was largely driven by river flow, while DOM composition was strongly influenced by impoundments. Seasonal algal blooms in upstream lentic reaches provided a steady source of algal DOM that was processed in downstream reaches. DOM at upstream sites had an average spectral slope ratio (SR) > 1, indicating algal-derived material, but decreased downstream to an average SR < 1, more indicative of terrestrial-derived material. The increasingly terrestrial nature of DOM exported from reservoirs likely reflects degraded algal material that becomes increasingly more recalcitrant with distance from upstream source and additional processing. As a result, DOM delivered to free-flowing river reaches below impoundments was less variable in composition. Downstream of impoundments, tributary influences resulted in increasing contributions of terrestrial DOM from the surrounding watershed. Removal of the four lower dams on the Klamath River is scheduled to proceed in the next decade. These results suggest that management should consider the role of impoundments on altering DOM dynamics, particularly in the context of dam removal.

Lignin has been analysed as a proxy for vegetation change in the Quaternary science literature since the early 1990s in archives such as peat, lakes, and intertidal and marine sediment cores. Historically, it has been regarded as comparatively resistant to various types of degradation in comparison to other plant components. However, studies of modern biogeochemical processes affecting organic carbon have demonstrated significant degradation and alteration of lignin as it is transported through the terrestrial biosphere, including phase changes from particulate to dissolved organic matter, mineral binding and decay due to biotic and abiotic processes. The literature of such topics is vast, however it is not particularly useful to Quaternary research without a comprehensive review to link our understanding of modern processes involving lignin to Quaternary environments. This review will outline the current state of the art in lignin phenol research that is relevant to the Quaternary scientist, and highlight the potential future applications for this important biomarker for vegetation change and terrestrial organic carbon cycling. © 2014 Elsevier Ltd.