Early land use and centennial scale changes in lake-water organic carbon prior to contemporary monitoring.

Organic carbon concentrations have increased in surface waters across parts of Europe and North America during the past decades, but the main drivers causing this phenomenon are still debated. A lack of observations beyond the last few decades inhibits a better mechanistic understanding of this process and thus a reliable prediction of future changes. Here we present past lake-water organic carbon trends inferred from sediment records across central Sweden that allow us to assess the observed increase on a centennial to millennial time scale. Our data show the recent increase in lake-water carbon but also that this increase was preceded by a landscape-wide, long-term decrease beginning already A.D. 1450-1600. Geochemical and biological proxies reveal that these dynamics coincided with an intensification of human catchment disturbance that decreased over the past century. Catchment disturbance was driven by the expansion and later cessation of widespread summer forest grazing and farming across central Scandinavia. Our findings demonstrate that early land use strongly affected past organic carbon dynamics and suggest that the influence of historical landscape utilization on contemporary changes in lake-water carbon levels has thus far been underestimated. We propose that past changes in land use are also a strong contributing factor in ongoing organic carbon trends in other regions that underwent similar comprehensive changes due to early cultivation and grazing over centuries to millennia.

The Arctic in the Twenty-First Century: Changing Biogeochemical Linkages across a Paraglacial Landscape of Greenland.

The Kangerlussuaq area of southwest Greenland encompasses diverse ecological, geomorphic, and climate gradients that function over a range of spatial and temporal scales. Ecosystems range from the microbial communities on the ice sheet and moisture-stressed terrestrial vegetation (and their associated herbivores) to freshwater and oligosaline lakes. These ecosystems are linked by a dynamic glacio-fluvial-aeolian geomorphic system that transports water, geological material, organic carbon and nutrients from the glacier surface to adjacent terrestrial and aquatic systems. This paraglacial system is now subject to substantial change because of rapid regional warming since 2000. Here, we describe changes in the eco- and geomorphic systems at a range of timescales and explore rapid future change in the links that integrate these systems. We highlight the importance of cross-system subsidies at the landscape scale and, importantly, how these might change in the near future as the Arctic is expected to continue to warm.

Boreal Forests Sequester Large Amounts of Mercury over Millennial Time Scales in the Absence of Wildfire.

Alterations in fire activity due to climate change and fire suppression may have profound effects on the balance between storage and release of carbon (C) and associated volatile elements. Stored soil mercury (Hg) is known to volatilize due to wildfires and this could substantially affect the land-air exchange of Hg; conversely the absence of fires and human disturbance may increase the time period over which Hg is sequestered. Here we show for a wildfire chronosequence spanning over more than 5000 years in boreal forest in northern Sweden that belowground inventories of total Hg are strongly related to soil humus C accumulation (R2 = 0.94, p < 0.001). Our data clearly show that northern boreal forest soils have a strong sink capacity for Hg, and indicate that the sequestered Hg is bound in soil organic matter pools accumulating over millennia. Our results also suggest that more than half of the Hg stock in the sites with the longest time since fire originates from deposition predating the onset of large-scale anthropogenic emissions. This study emphasizes the importance of boreal forest humus soils for Hg storage and reveals that this pool is likely to persist over millennial time scales in the prolonged absence of fire.

Inferring Past Trends in Lake Water Organic Carbon Concentrations in Northern Lakes Using Sediment Spectroscopy.

Changing lake water total organic carbon (TOC) concentrations are of concern for lake management because of corresponding effects on aquatic ecosystem functioning, drinking water resources and carbon cycling between land and sea. Understanding the importance of human activities on TOC changes requires knowledge of past concentrations; however, water-monitoring data are typically only available for the past few decades, if at all. Here, we present a universal model to infer past lake water TOC concentrations in northern lakes across Europe and North America that uses visible-near-infrared (VNIR) spectroscopy on lake sediments. In the orthogonal partial least-squares model, VNIR spectra of surface-sediment samples are calibrated against corresponding surface water TOC concentrations (0.5-41 mg L-1) from 345 Arctic to northern temperate lakes in Canada, Greenland, Sweden and Finland. Internal model-cross-validation resulted in a R2 of 0.57 and a prediction error of 4.4 mg TOC L-1. First applications to lakes in southern Ontario and Scotland, which are outside of the model's geographic range, show the model accurately captures monitoring trends, and suggests that TOC dynamics during the 20th century at these sites were primarily driven by changes in atmospheric deposition. Our results demonstrate that the lake water TOC model has multiregional applications and is not biased by postdepositional diagenesis, allowing the identification of past TOC variations in northern lakes of Europe and North America over time scales of decades to millennia.

The contribution of intra- and interspecific tolerance variability to biodiversity changes along toxicity gradients.

The worldwide distribution of toxicants is an important yet understudied driver of biodiversity, and the mechanisms relating toxicity to diversity have not been adequately explored. Here, we present a community model integrating demography, dispersal and toxicant-induced effects on reproduction driven by intraspecific and interspecific variability in toxicity tolerance. We compare model predictions to 458 species abundance distributions (SADs) observed along concentration gradients of toxicants to show that the best predictions occur when intraspecific variability is five and ten times higher than interspecific variability. At high concentrations, lower settings of intraspecific variability resulted in predictions of community extinction that were not supported by the observed SADs. Subtle but significant species losses at low concentrations were predicted only when intraspecific variability dominated over interspecific variability. Our results propose intraspecific variability as a key driver for biodiversity sustenance in ecosystems challenged by environmental change.

Mining, metallurgy and the historical origin of mercury pollution in lakes and watercourses in Central Sweden.

In Central Sweden an estimated 80% of the lakes contain fish exceeding health guidelines for mercury. This area overlaps extensively with the Bergslagen ore region, where intensive mining of iron ores and massive sulfide ores occurred over the past millennium. Although only a few mines still operate today, thousands of mineral occurrences and mining sites are documented in the region. Here, we present data on long-term mercury pollution in 16 sediment records from 15 lakes, which indicate that direct release of mercury to lakes and watercourses was already significant prior to industrialization (

Norway spruce postglacial recolonization of Fennoscandia.

Contrasting theories exist regarding how Norway spruce (Picea abies) recolonized Fennoscandia after the last glaciation and both early Holocene establishments from western microrefugia and late Holocene colonization from the east have been postulated. Here, we show that Norway spruce was present in southern Fennoscandia as early as 14.7 ± 0.1 cal. kyr BP and that the millennia-old clonal spruce trees present today in central Sweden likely arrived with an early Holocene migration from the east. Our findings are based on ancient sedimentary DNA from multiple European sites (N = 15) combined with nuclear and mitochondrial DNA analysis of ancient clonal (N = 135) and contemporary spruce forest trees (N = 129) from central Sweden. Our other findings imply that Norway spruce was present shortly after deglaciation at the margins of the Scandinavian Ice Sheet, and support previously disputed finds of pollen in southern Sweden claiming spruce establishment during the Lateglacial.

Contaminated lead environments of man: reviewing the lead isotopic evidence in sediments, peat, and soils for the temporal and spatial patterns of atmospheric lead pollution in Sweden.

Clair Patterson and colleagues demonstrated already four decades ago that the lead cycle was greatly altered on a global scale by humans. Moreover, this change occurred long before the implementation of monitoring programs designed to study lead and other trace metals. Patterson and colleagues also developed stable lead isotope analyses as a tool to differentiate between natural and pollution-derived lead. Since then, stable isotope analyses of sediment, peat, herbaria collections, soils, and forest plants have given us new insights into lead biogeochemical cycling in space and time. Three important conclusions from our studies of lead in the Swedish environment conducted over the past 15 years, which are well supported by extensive results from elsewhere in Europe and in North America, are: (1) lead deposition rates at sites removed from major point sources during the twentieth century were about 1,000 times higher than natural background deposition rates a few thousand years ago (~10 mg Pb m(-2) year(-1) vs. 0.01 mg Pb m(-2) year(-1)), and even today (~1 mg Pb m(-2) year(-1)) are still almost 100 times greater than natural rates. This increase from natural background to maximum fluxes is similar to estimated changes in body burdens of lead from ancient times to the twentieth century. (2) Stable lead isotopes ((206)Pb/(207)Pb ratios shown in this paper) are an effective tool to distinguish anthropogenic lead from the natural lead present in sediments, peat, and soils for both the majority of sites receiving diffuse inputs from long range and regional sources and for sites in close proximity to point sources. In sediments >3,500 years and in the parent soil material of the C-horizon, (206)Pb/(207)Pb ratios are higher, 1.3 to >2.0, whereas pollution sources and surface soils and peat have lower ratios that have been in the range 1.14-1.18. (3) Using stable lead isotopes, we have estimated that in southern Sweden the cumulative anthropogenic burden of atmospherically deposited lead is ~2-5 g Pb m(-2) and ~1 g Pb m(-2) in the "pristine" north. Half of this cumulative total was deposited before industrialization. (4) In the vicinity of the Rönnskär smelter in northern Sweden, a major point source during the twentieth century, there is an isotopic pattern that deviates from the general trends elsewhere, reflecting the particular history of ore usage at Rönnskär, which further demonstrates the chronological record of lead loading recorded in peat and in soil mor horizons.

Landscape Setting Drives the Microbial Eukaryotic Community Structure in Four Swedish Mountain Lakes over the Holocene.

On the annual and interannual scales, lake microbial communities are known to be heavily influenced by environmental conditions both in the lake and in its terrestrial surroundings. However, the influence of landscape setting and environmental change on shaping these communities over a longer (millennial) timescale is rarely studied. Here, we applied an 18S metabarcoding approach to DNA preserved in Holocene sediment records from two pairs of co-located Swedish mountain lakes. Our data revealed that the microbial eukaryotic communities were strongly influenced by catchment characteristics rather than location. More precisely, the microbial communities from the two bedrock lakes were largely dominated by unclassified Alveolata, while the peatland lakes showed a more diverse microbial community, with Ciliophora, Chlorophyta and Chytrids among the more predominant groups. Furthermore, for the two bedrock-dominated lakes-where the oldest DNA samples are dated to only a few hundred years after the lake formation-certain Alveolata, Chlorophytes, Stramenopiles and Rhizaria taxa were found prevalent throughout all the sediment profiles. Our work highlights the importance of species sorting due to landscape setting and the persistence of microbial eukaryotic diversity over millennial timescales in shaping modern lake microbial communities.

Late glacial (17,060-13,400 cal yr BP) sedimentary and paleoenvironmental evolution of the Sekhokong Range (Drakensberg), southern Africa.

Southern Africa sits at the junction of tropical and temperate systems, leading to the formation of seasonal precipitation zones. Understanding late Quaternary paleoclimatic change in this vulnerable region is hampered by a lack of available, reliably-dated records. Here we present a sequence from a well-stratified sedimentary infill occupying a lower slope basin which covers 17,060 to 13,400 cal yr BP with the aim to reconstruct paleoclimatic variability in the high Drakensberg during the Late Glacial. We use a combination of pollen, total organic carbon and nitrogen, δ13C, Fourier transform infrared spectroscopy attenuated total reflectance (FTIR-ATR) spectral and elemental data on contiguous samples with high temporal resolution (10 to 80 years per sample). Our data support a relatively humid environment with considerable cold season precipitation during what might have been the final stage of niche-glaciation on the adjoining southern aspects around 17,000 cal yr BP. Then, after an initial warmer and drier period starting ~15,600 cal yr BP, we identify a return to colder and drier conditions with more winter precipitation starting ~14,380 cal yr BP, which represents the first local evidence for the Antarctic Cold Reversal (ACR) in this region. On decadal to centennial timescales, the Late Glacial period was one marked by considerable climatic fluctuation and bi-directional environmental change, which has not been identified in previous studies for this region. Our study shows complex changes in both moisture and thermal conditions providing a more nuanced picture of the Late Glacial for the high Drakensburg.

Structural equation modeling of long-term controls on mercury and bromine accumulation in Pinheiro mire (Minas Gerais, Brazil).

The application of statistical modeling is still infrequent in mercury research in peat, despite the ongoing debate on the weight of the diverse factors (climate, peat decomposition, vegetation changes, etc.) that may affect mercury accumulation. One of the few exceptions is the Hg record of Pinheiro mire (souheast Brazil). Previous studies on this mire modeled mercury using principal components regression and partial least squares. These methods assume independence between factors, which is seldom the case in natural systems, thus hampering the identification of mediating effects and interactions. To overcome these limitations, in this reserach we use structural equation modeling (PLS-SEM) to model mercury and bromine peat records - bromine has been used in some investigations to normalize mercury accumuation. The mercury model explained 83% of the variance and suggested a complex control: increased peat decomposition, dust deposition and humid climates enhanced mercury accumulation, while increased mineral fluxes resulted in a decrease in mercury accumulation. The bromine model explained 90% of the variation in concentrations: increased dust deposition and peat decomposition promoted bromine accumulation, while time (i.e. peat age) promoted bromine depletion. Thus, although mercury and bromine are both organically bound elements with relevant atmospheric cycles the weights of the factors involved in their accumulation differed significantly. Our results suggest caution when using bromine to normalize mercury accumulation. PLS-SEM results indicate a large time dependence of peat decomposition, catchment mineral fluxes, long-term climate change, and atmospheric deposition; while atmospheric dust, mineral fluxes and peat decomposition showed high to moderate climate dependency. In particular, they also point to a relevant role of autogenic processes (i.e. the build up and expansion of the mire within the catchment), which controlled local mineral fluxes; an aspect that has seldom been considered.

Environmental archives of atmospheric Hg deposition - A review.

Environmental archives offer an opportunity to reconstruct temporal trends in atmospheric Hg deposition at various timescales. Lake sediment and peat have been the most widely used archives; however, new records from ice, tree rings, and the measurement of Hg stable isotopes, are offering new insights into past Hg cycling. Preindustrial Hg deposition has been studied over decadal to millennial timescales extending as far back as the late Pleistocene. Exploitation of mercury deposits (mainly cinnabar) first began during the mid to late Holocene in South America, Europe, and Asia, but increased dramatically during the Colonial era (1532-1900) for silver production. However, evidence for preindustrial Hg pollution is restricted to regions directly downwind or downstream of cinnabar or precious metal mining centers. Excluding these areas, there has been an approximately four-fold increase in atmospheric deposition globally over the industrial era (i.e., since 1800-1850), though regional differences exist, especially during the early 20th Century. Lake sediments, peat, ice, and tree rings are all influenced by (and integrate) a range of processes. For example, lake sediments are influenced by atmospheric deposition, sediment focusing, and the input of allochthonous material from the watershed, peat records reflect atmospheric deposition and biotic uptake, ice cores are a record of Hg scrubbed during precipitation, and tree rings record atmospheric concentrations. No archive represents an absolute record of past Hg deposition or concentrations, and post-depositional transformation of Hg profiles remains an important topic of research. However, natural archives continue to provide important insight into atmospheric Hg cycling over various timescales.

Human bones tell the story of atmospheric mercury and lead exposure at the edge of Roman World.

Atmospheric metal pollution is a major health concern whose roots pre-date industrialization. This study pertains the analyses of ancient human skeletons and compares them with natural archives to trace historical environmental exposure at the edge of the Roman Empire in NW Iberia. The novelty of our approach relies on the combination of mercury, lead and lead isotopes. We found over a 700-year period that rural Romans incorporated two times more mercury and lead into their bones than post-Romans inhabiting the same site, independent of sex or age. Atmospheric pollution sources contributed on average 57% (peaking at 85%) of the total lead incorporated into the bones in Roman times, which decreased to 24% after the decline of Rome. These values and accompanying changes in lead isotopic composition mirror changes in atmospheric Pb deposition recorded in local peatlands. Thus, skeletons are a time-transgressive archive reflecting contaminant exposure.

Comment on "Next-Generation Ice Core Technology Reveals True Minimum Natural Levels of Lead (Pb) in the Atmosphere: Insights From the Black Death" by More et al.

Over the past four decades numerous studies of lake sediment, marine sediment, and peat from sites in close proximity to mining or metallurgical centers and in remote locations have detailed local and regional histories of lead (Pb) pollution in Europe. Contrary to More et al.'s (2017, https://doi.org/10.1002/2017GH000064) claim that "previous assumptions about preindustrial "natural" background lead levels in the atmosphere have been misleading," these studies have clearly shown that true natural background conditions occurred more than 2,500 or even 3,500 years ago, and Pb pollution has proceeded uninterrupted since. The implications of this have been discussed within the context of environmental policy, for example, European Water Framework Directive. Though these records reflect a common European narrative of mining, metallurgy, and pollution, each reflects a combination of local and regional events, leading to differences in the timing and intensity of changes in each Pb record. No one record-ice or otherwise-fully represents the three millennia Pb pollution history in Europe. While the resolution of the ice record is impressive, there are questions about its interpretation. First, the authors discount local and regional Pb sources, whereas there is a close connection between the mining history in an area 40 km from the glacier and changes in a nearby lake Pb record; second, significant changes in ice chemistry cooccurring with the lowest Pb values are overlooked. A sharp increase in Ca/Fe ratios occurs precisely with the steepest Pb declines during the Black Death and mid-1400s, suggesting additional processes influencing the Pb record.

Industrial-era lead and mercury contamination in southern Greenland implicates North American sources.

To study the long-range transport of atmospheric pollutants from lower latitude industrial areas to the Arctic, we analysed a peat core spanning the last ~700cal.yr (~1300-2000CE) from southern Greenland, an area sensitive to atmospheric pollution from North American and Eurasian sources. A previous investigation conducted in the same location recorded atmospheric lead (Pb) pollution after ~1845, with peak values recorded in the 1970s, and concluded that a North American source was most likely. To confirm the origin of the lead, we present new Pb isotope data from Sandhavn, together with a high-resolution record for mercury (Hg) deposition. Results demonstrate that the mercury accumulation rate has steadily increased since the beginning of the 19th century, with maximum values of 9.3µgm-2yr-1 recorded ~1940. Lead isotopic ratios show two mixing lines: one which represents inputs from local and regional geogenic sources, and another that comprises regional geogenic and pollution sources. Detrending the Pb isotopic ratio record (thereby extracting the effect of the geogenic mixing) has enabled us to reconstruct a detailed chronology of metal pollution. The first sustained decrease in Pb isotope signals is recorded as beginning ~1740-1780 with the lowest values (indicating the highest pollution signature) dated to ~1960-1970. The 206Pb/207Pb ratio of excess Pb (measuring 1.222, and reflecting pollution-generated Pb), when compared with the Pb isotopic composition of the Sandhavn peat record since the 19th century and the timing of Pb enrichments, clearly points to the dominance of pollution sources from North America, although it did not prove possible to further differentiate the emissions sources geographically.

Mineral dust as a driver of carbon accumulation in northern latitudes.

Peatlands in northern latitudes sequester one third of the world's soil organic carbon. Mineral dusts can affect the primary productivity of terrestrial systems through nutrient transport but this process has not yet been documented in these peat-rich regions. Here we analysed organic and inorganic fractions of an 8900-year-old sequence from Store Mosse (the "Great Bog") in southern Sweden. Between 5420 and 4550 cal yr BP, we observe a seven-fold increase in net peat-accumulation rates corresponding to a maximum carbon-burial rate of 150 g C m-2 yr-1 - more than six times the global average. This high peat accumulation event occurs in parallel with a distinct change in the character of the dust deposited on the bog, which moves from being dominated by clay minerals to less weathered, phosphate and feldspar minerals. We hypothesize that this shift boosted nutrient input to the bog and stimulated ecosystem productivity. This study shows that diffuse sources and dust dynamics in northern temperate latitudes, often overlooked by the dust community in favour of arid and semi-arid regions, can be important drivers of peatland carbon accumulation and by extension, global climate, warranting further consideration in predictions of future climate variability.

Mercury pollution trends in subarctic lakes in the northern Swedish mountains.

Despite many years of research about mercury pollution, data concerning high-latitude regions of Europe are limited, particularly studies of long-term temporal trends. It is not clear whether the mercury load at high latitudes follows the recent decreasing trends in European mercury emissions or whether the load is still high because of continuing global emissions. In this study we use sediments from 12 lakes, located above the Arctic Circle in the Swedish mountains, to assess the past and recent mercury pollution situation, especially for the last 200 y. The mercury load increased clearly in sediment deposited from the late 19th or early 20th century to a peak between 1960 and 1990. This peak represents an enrichment of 1.4 to 4.2 times over background concentrations. This enrichment is comparable with enrichments in sediments from lower latitudes as well as other Arctic regions. Since the 1990s mercury concentration has declined in 8 of the 12 lakes, i.e., similar to emission trends in Europe.

Early atmospheric metal pollution provides evidence for Chalcolithic/Bronze Age mining and metallurgy in Southwestern Europe.

Although archaeological research suggests that mining/metallurgy already started in the Chalcolithic (3rd millennium BC), the earliest atmospheric metal pollution in SW Europe has thus far been dated to ~3500-3200 cal.yr. BP in paleo-environmental archives. A low intensity, non-extensive mining/metallurgy and the lack of appropriately located archives may be responsible for this mismatch. We have analysed the older section (>2100 cal.yr. BP) of a peat record from La Molina (Asturias, Spain), a mire located in the proximity (35-100 km) of mines which were exploited in the Chalcolithic/Bronze Age, with the aim of assessing evidence of this early mining/metallurgy. Analyses included the determination of C as a proxy for organic matter content, lithogenic elements (Si, Al, Ti) as markers of mineral matter, and trace metals (Cr, Cu, Zn, Pb) and stable Pb isotopes as tracers of atmospheric metal pollution. From ~8000 to ~4980 cal.yr. BP the Pb composition is similar to that of the underlying sediments (Pb 15 ± 4 µg g(-1); (206)Pb/(207)Pb 1.204 ± 0.002). A sustained period of low (206)Pb/(207)Pb ratios occurred from ~4980 to ~2470 cal.yr. BP, which can be divided into four phases: Chalcolithic (~4980-3700 cal.yr. BP), (206)Pb/(207)Pb ratios decline to 1.175 and Pb/Al ratios increase; Early Bronze Age (~3700-3500 cal.yr. BP), (206)Pb/(207)Pb increase to 1.192 and metal/Al ratios remain stable; Late Bronze Age (~3500-2800 cal.yr. BP), (206)Pb/(207)Pb decline to their lowest values (1.167) while Pb/Al and Zn/Al increase; and Early Iron Age (~2800-2470 cal.yr. BP), (206)Pb/(207)Pb increase to 1.186, most metal/Al ratios decrease but Zn/Al shows a peak. At the beginning of the Late Iron Age, (206)Pb/(207)Pb ratios and metal enrichments show a rapid return to pre-anthropogenic values. These results provide evidence of regional/local atmospheric metal pollution triggered by the earliest phases of mining/metallurgy in the area, and reconcile paleo-environmental and archaeological records.

Downwash of atmospherically deposited trace metals in peat and the influence of rainfall intensity: an experimental test.

Accumulation records of pollutant metals in peat have been frequently used to reconstruct past atmospheric deposition rates. While there is good support for peat as a record of relative changes in metal deposition over time, questions remain whether peat archives represent a quantitative or a qualitative record. Several processes can potentially influence the quantitative record of which downwashing is particularly pertinent as it would have a direct influence on how and where atmospherically deposited metals are accumulated in peat. The aim of our study was two-fold: first, to compare and contrast the retention of dissolved Pb, Cu, Zn and Ni in peat cores; and second, to test the influence of different precipitation intensities on the potential downwashing of metals. We applied four 'rainfall' treatments to 13 peat cores over a 3-week period, including both daily (2 or 5.3 mm day(-1)) and event-based additions (37 mm day(-1), added over 1h or over a 10h rain event). Two main trends were apparent: 1) there was a difference in retention of the added dissolved metals in the surface layer (0-2 cm): 21-85% for Pb, 18-63% for Cu, 10-25% for Zn and 10-20% for Ni. 2) For all metals and both peat types (sphagnum lawn and fen), the addition treatments resulted in different downwashing depths, i.e., as the precipitation-addition increased so did the depth at which added metals could be detected. Although the largest fraction of Pb and Cu was retained in the surface layer and the remainder effectively immobilized in the upper peat (≤ 10 cm), there was a smearing effect on the overall retention, where precipitation intensity exerts an influence on the vertical distribution of added trace metals. These results indicate that the relative position of a deposition signal in peat records would be preserved, but it would be quantitatively attenuated.

High-throughput characterization of sediment organic matter by pyrolysis-gas chromatography/mass spectrometry and multivariate curve resolution: A promising analytical tool in (paleo)limnology.

Molecular-level chemical information about organic matter (OM) in sediments helps to establish the sources of OM and the prevalent degradation/diagenetic processes, both essential for understanding the cycling of carbon (C) and of the elements associated with OM (toxic trace metals and nutrients) in lake ecosystems. Ideally, analytical methods for characterizing OM should allow high sample throughput, consume small amounts of sample and yield relevant chemical information, which are essential for multidisciplinary, high-temporal resolution and/or large spatial scale investigations. We have developed a high-throughput analytical method based on pyrolysis-gas chromatography/mass spectrometry and automated data processing to characterize sedimentary OM in sediments. Our method consumes 200 µg of freeze-dried and ground sediment sample. Pyrolysis was performed at 450°C, which was found to avoid degradation of specific biomarkers (e.g., lignin compounds, fresh carbohydrates/cellulose) compared to 650°C, which is in the range of temperatures commonly applied for environmental samples. The optimization was conducted using the top ten sediment samples of an annually resolved sediment record (containing 16-18% and 1.3-1.9% of total carbon and nitrogen, respectively). Several hundred pyrolytic compound peaks were detected of which over 200 were identified, which represent different classes of organic compounds (i.e., n-alkanes, n-alkenes, 2-ketones, carboxylic acids, carbohydrates, proteins, other N compounds, (methoxy)phenols, (poly)aromatics, chlorophyll and steroids/hopanoids). Technical reproducibility measured as relative standard deviation of the identified peaks in triplicate analyses was 5.5±4.3%, with 90% of the RSD values within 10% and 98% within 15%. Finally, a multivariate calibration model was calculated between the pyrolytic degradation compounds and the sediment depth (i.e., sediment age), which is a function of degradation processes and changes in OM source type. This allowed validation of the Py-GC/MS dataset against fundamental processes involved in OM cycling in aquatic ecosystems.