Exploring the pore fluid origin and methane-derived authigenic carbonate properties in response to changes in the methane flux at the southern Ulleung Basin, South Korea

We investigated the geochemistry of gas, pore fluid, and methane-derived authigenic carbonate (MDAC) from four sites in the southern Ulleung Basin, South Korea. In contrast to Sites 16GH-P1 and 16GH-P5, Sites 16GH-P3, and 16GH-P4 are characterized by acoustic chimney structures associated with gas flux. The composition of gas and isotopic signatures of methane (CH4) (C1/C2+ > 300, δ13CCH4 < -60‰, δDCH4 ≤ -190‰) indicate microbial source CH4 at all sites. The upward migration of CH4 can affect the chemical and isotopic properties of pore fluid and gas-related byproducts (e.g., gas hydrate (GH) and MDAC) within the shallow sediments including the current sulfate-methane transition (SMT) (< 5 meters below seafloor). Although no GH was found, elevated Cl- concentrations (maximum = 609 mM) with low δD and δ18O values in Site 16GH-P4 pore fluids delineate the influence of massive GH formation in deeper sediment. In contrast, relatively constant Cl-, δD, and δ18O values in fluids from Sites 16GH-P1, 16GH-P3, and 16GH-P5 indicate a predominant origin from seawater. Pore fluids also exhibit higher concentrations of H4SiO4, B, Mg2+, and K+, along with increasing alkalinity compared to seawater. These observations suggest that marine silicate weathering alters fluid chemistry within the sediment, affecting element and carbon cycles. High alkalinity (up to 60 mM) and Mg2+/Ca2+ ratios (> 6) alongside decreasing Ca2+ and Sr2+ concentrations imply carbonate precipitation. MDACs with diverse morphologies, mainly composed of aragonite and magnesian calcite, and characterized by low carbon isotopic values (δ13CMDAC < -31.3‰), were found at Sites 16GH-P3 and 16GH-P4. Interestingly, δ13CMDAC values at Site 16GH-P3 are clearly differentiated above and below the current SMT. High δ13CMDAC values above the SMT (> -34.3‰) suggest the combined influence of seawater and CH4 migrating upward on MDAC precipitation, whereas low δ13CMDAC values below it (< -41.6‰) indicate a predominant impact of CH4 on MDAC formation. Additionally, the vertical variation of δ18OMDAC values at Site 16GH-P4, compared to the theoretical values, reflects an association with GH dissociation and formation. Our findings improve the understanding of fluid, gas, and MDAC geochemistry in continental margin cold seeps, providing insights into global carbon and element cycles

Glacial history and depositional environments in little Storfjorden and Hambergbukta of Arctic Svalbard since the younger dryas

Geophysical and lithological data provide crucial information for the understanding of glacial history in Arctic Svalbard. In this study, we reconstructed the glacier-induced depositional environments of Little Storfjorden and its tributary, Hambergbukta, over the last 13 ka to better understand the glacial history of southeastern Svalbard. The combined uses of swath-bathymetry, high-resolution seismic stratigraphy, and multiple-proxy measurements of sediment cores allowed us to define five steps of glacier-induced depositional environments: 1) deposition of massive, semi-consolidated gravelly sandy mud (Facies 1) during re-advance or still-stand of the marine-based glaciers/ice streams in Little Storfjorden during Younger Dryas (13–12 ka); 2) deposition of massive mud to gravelly sandy mud (Facies 2A and B) during glacial retreat until the earliest Holocene (12–10.1 ka); 3) sediment winnowing by enhanced bottom currents during the early to middle Holocene (10.1–3.7 ka); 4) deposition of bioturbated sandy mud (Facies 3) with high productivity under seasonal sea ice conditions during the late Holocene (3.7–0.7 ka); and 5) deposition of (slightly) bioturbated sandy to gravelly mud (Facies 4) affected by glacier surges since Little Ice Age (LIA) (Facies 4). In addition to seismic stratigraphy, depositional patterns of IRD in Little Storfjorden indicate that the glacier surges in Hambergbukta occurred only after ∼0.7 ka. This suggests that the terminal moraine complex (TMC) represents the maximum extent of the LIA surges, which argues against the recent inference for the TMC formation during pre-LIA. This study shows the importance of multiple parameters to better understand the current behavior of tidewater glaciers in the Svalbard fjords in response to rapid climate change

A pulse of meteoric subsurface fluid discharging into the Chukchi Sea during the Early Holocene Thermal Maximum (EHTM)

This work was supported bythe Korea Ministry of Science and ICT (GP2020-038), by the Korea Ministry of Oceans and Fisheries (NP2011-040 and 1525011795), and by the Korea Polar Research Institute (Grants No. PE20350). W.-L.H. acknowledges the supports from the ArcticSGD, a project supported by the Norway Grants and the EEA Grants (2019/34/H/ST10/00645). Additional funds were contributed by the AWI Research Program PACES-II Workpackage 3.1 and 3.2.The response of Arctic Ocean biogeochemistry to subsurface flow driven by permafrost thaw is poorly understood. We present dissolved chloride and water isotopic data from the Chukchi Sea Shelf sediments that reveal the presence of a meteoric subsurface flow enriched in cations with a radiogenic Sr fingerprint. This subsurface fluid is also enriched in dissolved inorganic carbon and methane that bear isotopic compositions indicative of a carbon reservoir modified by reactions in a closed system. Such fluid characteristics are in stark contrast with those from other sites in the Chukchi Sea where the pore water composition shows no sign of meteoric input, but reflect typical biogeochemical reactions associated with early diagenetic sequences in marine sediment. The most likely source of the observed subsurface flow at the Chukchi Sea Shelf is from the degradation of permafrost that had extended to the shelf region during the Last Glacial Maximum. Our data suggest that the permafrost-driven subsurface flow most likely took place during the 2-3 oC warming in the Early Holocene Thermal Maximum (EHTM). This time scale is supported by numerical simulation of pore fluid profiles, which indicate that a minimum of several thousand years must have passed since the cessation of the subsurface methane-bearing fluid flow.Publisher PDFPeer reviewe

Influence of sedimentary deposition on the microbial assembly process in Arctic Holocene marine sediments

The sea-level rise during the Holocene (11–0 ky BP) and its resulting sedimentation and biogeochemical processes may control microbial life in Arctic sediments. To gain further insight into this interaction, we investigated a sediment core (up to 10.7 m below the seafloor) from the Chuckchi Shelf of the western Arctic Ocean using metabarcoding-based sequencing and qPCR to characterize archaeal and bacterial 16S rRNA gene composition and abundance, respectively. We found that Arctic Holocene sediments harbor local microbial communities, reflecting geochemical and paleoclimate separations. The composition of bacterial communities was more diverse than that of archaeal communities, and specifically distinct at the boundary layer of the sulfate–methane transition zone. Enriched cyanobacterial sequences in the Arctic middle Holocene (8–7 ky BP) methanogenic sediments remarkably suggest past cyanobacterial blooms. Bacterial communities were phylogenetically influenced by interactions between dispersal limitation and environmental selection governing community assembly under past oceanographic changes. The relative influence of stochastic and deterministic processes on the bacterial assemblage was primarily determined by dispersal limitation. We have summarized our findings in a conceptual model that revealed how changes in paleoclimate phases cause shifts in ecological succession and the assembly process. In this ecological model, dispersal limitation is an important driving force for progressive succession for bacterial community assembly processes on a geological timescale in the western Arctic Ocean. This enabled a better understanding of the ecological processes that drive the assembly of communities in Holocene sedimentary habitats affected by sea-level rise, such as in the shallow western Arctic shelves

Quantifying K, U, and Th contents of marine sediments using shipboard natural gamma radiation spectra measured on DV JOIDES Resolution

During International Ocean Discovery Program (IODP) expeditions, shipboard-generated data provide the first insights into the cored sequences. The natural gamma radiation (NGR) of the recovered material, for example, is routinely measured on the ocean drilling research vessel DV JOIDES Resolution. At present, only total NGR counts are readily available as shipboard data, although full NGR spectra (counts as a function of gamma-ray energy level) are produced and archived. These spectra contain unexploited information, as one can estimate the sedimentary contents of potassium (K), thorium (Th), and uranium (U) from the characteristic gamma-ray energies of isotopes in the ^(40)K, ^(232)Th, and ^(238)U radioactive decay series. Dunlea et al. [2013] quantified K, Th and U contents in sediment from the South Pacific Gyre by integrating counts over specific energy levels of the NGR spectrum. However, the algorithm used in their study is unavailable to the wider scientific community due to commercial proprietary reasons. Here, we present a new MATLAB algorithm for the quantification of NGR spectra that is transparent and accessible to future NGR users. We demonstrate the algorithm's performance by comparing its results to shore-based inductively coupled plasma-mass spectrometry (ICP-MS), inductively coupled plasma-emission spectrometry (ICP-ES), and quantitative wavelength-dispersive X-ray fluorescence (XRF) analyses. Samples for these comparisons come from eleven sites (U1341, U1343, U1366-U1369, U1414, U1428-U1430, U1463) cored in two oceans during five expeditions. In short, our algorithm rapidly produces detailed high-quality information on sediment properties during IODP expeditions at no extra cost

Impact of High Methane Flux on the Properties of Pore Fluid and Methane-Derived Authigenic Carbonate in the ARAON Mounds, Chukchi Sea

We investigated the pore fluid and methane-derived authigenic carbonate (MDAC) chemistry from the ARAON Mounds in the Chukchi Sea to reveal how methane (CH4) seepage impacts their compositional and isotopic properties. During the ARA07C and ARA09C Expeditions, many in situ gas hydrates (GHs) and MDACs were found near the seafloor. The fluid chemistry has been considerably modified in association with the high CH4 flux and its related byproducts (GHs and MDACs). Compared to Site ARA09C-St 08 (reference site), which displays a linear SO42- downcore profile, the other sites (e.g., ARA07C-St 13, ARA07C-St 14, ARA09C-St 04, ARA09C-St 07, and ARA09C-St 12) that are found byproducts exhibit concave-up and/or kink type SO42- profiles. The physical properties and fluid pathways in sediment columns have been altered by these byproducts, which prevents the steady state condition of the dissolved species through them. Consequently, chemical zones are separated between bearing and non-bearing byproducts intervals under non-steady state condition from the seafloor to the sulfate-methane transition (SMT). GH dissociation also significantly impacts pore fluid properties (e.g., low Cl-, enriched delta D and delta O-18). The upward CH4 with depleted delta C-13 from the thermogenic origin affects the chemical signatures of MDACs. The enriched delta O-18 fluid from GH dissociation also influences the properties of MDACs. Thus, in the ARAON Mounds, the chemistry of the fluid and MDAC has significantly changed, most likely responding to the CH4 flux and GH dissociation through geological time. Overall, our findings will improve the understanding and prediction of the pore fluid and MDAC chemistry in the Arctic Ocean related to CH4 seepage by global climate change

Bulk mineral assemblage of sediment cores from Svalbard fjords determined via full pattern QXRD

The XRD data has been gained from pulverized and homogenized samples of every 5 cm by KOPRI personal at KOPRI and University of Tromsoe sampling parties. XRD raw measurements were run at Crystallography, Geosciences, University of Bremen in 2018-2020. Measurement conditions: Philips X'Pert Diffractometer, Cu radiation, fixed divergence, secoundary Ni filter, 3-85 ° 2theta, 0.0016° step size, 100 sec calculated step time. XRD mineral assemblage determination were subsequently gained through the QUAX full pattern quantitative determination software (see Vogt et al. 2002 at Pangaea methods wiki). The software allows for differentiation of all minerals. Here, the Fe-oxides and hydroxides were in the focus of the research manuscript. A QXRD investigation allows for not only identification of mineral content but also for detailing authigenic vs. allochthonous minerals, transport of detrital input to the sediment core and the interpretation of the transport processes and the local environment as well as the paleoceanographic reconstruction of the region. Sediment ages are given through the below mentioned data sets. A series of fjord surface sediments were collected from various Svalbard fjord systems during expeditions of RV Helmer Hanssen from UiT The Arctic University of Norway between 2012 and 2019 (Fig. 1). Four gravity cores were retrieved along a 150 km long N‒S transect from the continental shelf off northern Svalbard to the innermost Wijdefjorden: core HH17-1085-GC (hereafter 1085; 80.27°N, 16.21°E, 322 m water depth; continental shelf), HH17-1094-GC (hereafter 1094; 79.74°N, 15.42°E, 148 m water depth; fjord mouth), HH17-1100-GC (hereafter 1100; 79.30°N, 15.78°E, 112 m water depth; central fjord), and HH17-1106-GC (hereafter 1106; 79.00°N, 16.21°E, 160 m water depth; inner fjord