@article{YoungUedaGuehretal.2018, author = {Young, Linda and Ueda, Kiyoshi and G{\"u}hr, Markus and Bucksbaum, Philip H. and Simon, Marc and Mukamel, Shaul and Rohringer, Nina and Prince, Kevin C. and Masciovecchio, Claudio and Meyer, Michael and Rudenko, Artem and Rolles, Daniel and Bostedt, Christoph and Fuchs, Matthias and Reis, David A. and Santra, Robin and Kapteyn, Henry and Murnane, Margaret and Ibrahim, Heide and Legare, Francois and Vrakking, Marc and Isinger, Marcus and Kroon, David and Gisselbrecht, Mathieu and W{\"o}rner, Hans Jakob and Leone, Stephen R.}, title = {Roadmap of ultrafast x-ray atomic and molecular physics}, series = {Journal of physics : B, Atomic, molecular and optical physics}, volume = {51}, journal = {Journal of physics : B, Atomic, molecular and optical physics}, number = {3}, publisher = {IOP Publ. Ltd.}, address = {Bristol}, issn = {0953-4075}, doi = {10.1088/1361-6455/aa9735}, pages = {45}, year = {2018}, abstract = {X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (10(20) W cm(-2)) of x-rays at wavelengths down to similar to 1 Angstrom, and HHG provides unprecedented time resolution (similar to 50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of similar to 280 eV (44 Angstroms) and the bond length in methane of similar to 1 Angstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Angstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Angstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.}, language = {en} } @article{MonhonvalStraussMaucletetal.2021, author = {Monhonval, Arthur and Strauss, Jens and Mauclet, Elisabeth and Hirst, Catherine and Bemelmans, Nathan and Grosse, Guido and Schirrmeister, Lutz and Fuchs, Matthias and Opfergelt, Sophie}, title = {Iron redistribution upon thermokarst processes in the Yedoma domain}, series = {Frontiers in Earth Science}, volume = {9}, journal = {Frontiers in Earth Science}, publisher = {Frontiers Media}, address = {Lausanne}, issn = {2296-6463}, doi = {10.3389/feart.2021.703339}, pages = {18}, year = {2021}, abstract = {Ice-rich permafrost has been subject to abrupt thaw and thermokarst formation in the past and is vulnerable to current global warming. The ice-rich permafrost domain includes Yedoma sediments that have never thawed since deposition during the late Pleistocene and Alas sediments that were formed by previous thermokarst processes during the Lateglacial and Holocene warming. Permafrost thaw unlocks organic carbon (OC) and minerals from these deposits and exposes OC to mineralization. A portion of the OC can be associated with iron (Fe), a redox-sensitive element acting as a trap for OC. Post-depositional thaw processes may have induced changes in redox conditions in these deposits and thereby affected Fe distribution and interactions between OC and Fe, with knock-on effects on the role that Fe plays in mediating present day OC mineralization. To test this hypothesis, we measured Fe concentrations and proportion of Fe oxides and Fe complexed with OC in unthawed Yedoma and previously thawed Alas deposits. Total Fe concentrations were determined on 1,292 sediment samples from the Yedoma domain using portable X-ray fluorescence; these concentrations were corrected for trueness using a calibration based on a subset of 144 samples measured by inductively coupled plasma optical emission spectrometry after alkaline fusion (R (2) = 0.95). The total Fe concentration is stable with depth in Yedoma deposits, but we observe a depletion or accumulation of total Fe in Alas deposits, which experienced previous thaw and/or flooding events. Selective Fe extractions targeting reactive forms of Fe on unthawed and previously thawed deposits highlight that about 25\% of the total Fe is present as reactive species, either as crystalline or amorphous oxides, or complexed with OC, with no significant difference in proportions of reactive Fe between Yedoma and Alas deposits. These results suggest that redox driven processes during past thermokarst formation impact the present-day distribution of total Fe, and thereby the total amount of reactive Fe in Alas versus Yedoma deposits. This study highlights that ongoing thermokarst lake formation and drainage dynamics in the Arctic influences reactive Fe distribution and thereby interactions between Fe and OC, OC mineralization rates, and greenhouse gas emissions.}, language = {en} } @article{JongejansStraussLenzetal.2018, author = {Jongejans, Loeka Laura and Strauss, Jens and Lenz, Josefine and Peterse, Francien and Mangelsdorf, Kai and Fuchs, Matthias and Grosse, Guido}, title = {Organic matter characteristics in yedoma and thermokarst deposits on Baldwin Peninsula, west Alaska}, series = {Biogeosciences}, volume = {15}, journal = {Biogeosciences}, number = {20}, publisher = {Copernicus}, address = {G{\"o}ttingen}, issn = {1726-4170}, doi = {10.5194/bg-15-6033-2018}, pages = {6033 -- 6048}, year = {2018}, abstract = {As Arctic warming continues and permafrost thaws, more soil and sedimentary organic matter (OM) will be decomposed in northern high latitudes. Still, uncertainties remain in the quality of the OM and the size of the organic carbon (OC) pools stored in different deposit types of permafrost landscapes. This study presents OM data from deep permafrost and lake deposits on the Baldwin Peninsula which is located in the southern portion of the continuous permafrost zone in west Alaska. Sediment samples from yedoma and drained thermokarst lake basin (DTLB) deposits as well as thermokarst lake sediments were analyzed for cryostratigraphical and biogeochemical parameters and their lipid biomarker composition to identify the below-ground OC pool size and OM quality of ice-rich permafrost on the Baldwin Peninsula. We provide the first detailed characterization of yedoma deposits on Baldwin Peninsula. We show that three-quarters of soil OC in the frozen deposits of the study region (total of 68 Mt) is stored in DTLB deposits (52 Mt) and one-quarter in the frozen yedoma deposits (16 Mt). The lake sediments contain a relatively small OC pool (4 Mt), but have the highest volumetric OC content (93 kgm(-3)) compared to the DTLB (35 kgm(-3)) and yedoma deposits (8 kgm(-3)), largely due to differences in the ground ice content. The biomarker analysis indicates that the OM in both yedoma and DTLB deposits is mainly of terrestrial origin. Nevertheless, the relatively high carbon preference index of plant leaf waxes in combination with a lack of a degradation trend with depth in the yedoma deposits indi-cates that OM stored in yedoma is less degraded than that stored in DTLB deposits. This suggests that OM in yedoma has a higher potential for decomposition upon thaw, despite the relatively small size of this pool. These findings show that the use of lipid biomarker analysis is valuable in the assessment of the potential future greenhouse gas emissions from thawing permafrost, especially because this area, close to the discontinuous permafrost boundary, is projected to thaw substantially within the 21st century.}, language = {en} } @article{FuchsLenzJocketal.2019, author = {Fuchs, Matthias and Lenz, Josefine and Jock, Suzanne and Nitze, Ingmar and Jones, Benjamin M. and Strauss, Jens and G{\"u}nther, Frank and Grosse, Guido}, title = {Organic carbon and nitrogen stocks along a thermokarst lake sequence in Arctic Alaska}, series = {Journal of geophysical research : Biogeosciences}, volume = {124}, journal = {Journal of geophysical research : Biogeosciences}, number = {5}, publisher = {American Geophysical Union}, address = {Washington}, issn = {2169-8953}, doi = {10.1029/2018JG004591}, pages = {1230 -- 1247}, year = {2019}, abstract = {Thermokarst lake landscapes are permafrost regions, which are prone to rapid (on seasonal to decadal time scales) changes, affecting carbon and nitrogen cycles. However, there is a high degree of uncertainty related to the balance between carbon and nitrogen cycling and storage. We collected 12 permafrost soil cores from six drained thermokarst lake basins (DTLBs) along a chronosequence north of Teshekpuk Lake in northern Alaska and analyzed them for carbon and nitrogen contents. For comparison, we included three lacustrine cores from an adjacent thermokarst lake and one soil core from a non thermokarst affected remnant upland. This allowed to calculate the carbon and nitrogen stocks of the three primary landscape units (DTLB, lake, and upland), to reconstruct the landscape history, and to analyze the effect of thermokarst lake formation and drainage on carbon and nitrogen stocks. We show that carbon and nitrogen contents and the carbon-nitrogen ratio are considerably lower in sediments of extant lakes than in the DTLB or upland cores indicating degradation of carbon during thermokarst lake formation. However, we found similar amounts of total carbon and nitrogen stocks due to the higher density of lacustrine sediments caused by the lack of ground ice compared to DTLB sediments. In addition, the radiocarbon-based landscape chronology for the past 7,000years reveals five successive lake stages of partially, spatially overlapping DTLBs in the study region, reflecting the dynamic nature of ice-rich permafrost deposits. With this study, we highlight the importance to include these dynamic landscapes in future permafrost carbon feedback models. Plain Language Summary When permanently frozen soils (permafrost) contain ice-rich sediments, the thawing of this permafrost causes the surface to sink, which may result in lake formation. This process, the thaw of ice-rich permafrost and melting of ground ice leads to characteristic landforms-known as thermokarst. Once such a thaw process is initiated in ice-rich sediments, a thaw lake forms and grows by shoreline erosion, eventually expanding until a drainage pathway is encountered and the lake eventually drains, resulting in a drained thermokarst lake basin. In our study, we show that such a thermokarst-affected landscape north of Teshekpuk Lake in northern Alaska is shaped by repeated thaw lake formation and lake drainage events during the past 7,000years, highlighting the dynamic nature of these landscapes. These landscape-scale processes have a big effect on the carbon and nitrogen stored in permafrost soils. We show that large amounts of carbon (>45kg C/m(2)) and nitrogen (>2.6kg N/m(2)) are stored in unfrozen lake sediments and in frozen soil sediments. The findings are important when considering the potential effect that permafrost thaw has for the global climate through releasing carbon and nitrogen, which was frozen and therefore locked away for millennia, from the active carbon cycle.}, language = {en} } @article{FuchsGrosseStraussetal.2018, author = {Fuchs, Matthias and Grosse, Guido and Strauss, Jens and G{\"u}nther, Frank and Grigoriev, Mikhail N. and Maximov, Georgy M. and Hugelius, Gustaf}, title = {Carbon and nitrogen pools in thermokarst-affected permafrost landscapes in Arctic Siberia}, series = {Biogeosciences}, volume = {15}, journal = {Biogeosciences}, number = {3}, publisher = {Copernicus}, address = {G{\"o}ttingen}, issn = {1726-4170}, doi = {10.5194/bg-15-953-2018}, pages = {953 -- 971}, year = {2018}, abstract = {Ice-rich yedoma-dominated landscapes store considerable amounts of organic carbon (C) and nitrogen (N) and are vulnerable to degradation under climate warming. We investigate the C and N pools in two thermokarst-affected yedoma landscapes - on Sobo-Sise Island and on Bykovsky Peninsula in the north of eastern Siberia. Soil cores up to 3m depth were collected along geomorphic gradients and analysed for organic C and N contents. A high vertical sampling density in the profiles allowed the calculation of C and N stocks for short soil column intervals and enhanced understanding of within-core parameter variability. Profile-level C and N stocks were scaled to the landscape level based on landform classifications from 5 m resolution, multispectral RapidEye satellite imagery. Mean landscape C and N storage in the first metre of soil for Sobo-Sise Island is estimated to be 20.2 kg C m(-2) and 1.8 kg N m(-2) and for Bykovsky Peninsula 25.9 kg C m(-2) and 2.2 kg N m(-2). Radiocarbon dating demonstrates the Holocene age of thermokarst basin deposits but also suggests the presence of thick Holoceneage cover layers which can reach up to 2 m on top of intact yedoma landforms. Reconstructed sedimentation rates of 0.10-0.57 mm yr(-1) suggest sustained mineral soil accumulation across all investigated landforms. Both yedoma and thermokarst landforms are characterized by limited accumulation of organic soil layers (peat). We further estimate that an active layer deepening of about 100 cm will increase organic C availability in a seasonally thawed state in the two study areas by similar to 5.8 Tg (13.2 kg C m(-2)). Our study demonstrates the importance of increasing the number of C and N storage inventories in ice-rich yedoma and thermokarst environments in order to account for high variability of permafrost and thermokarst environments in pan-permafrost soil C and N pool estimates.}, language = {en} }