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A series of NHC-supported 1,2-dithienyldiborenes was synthesized from the corresponding (dihalo)thienylborane NHC precursors. NMR and UV-vis spectroscopic data, as well as X-ray crystallographic analyses, were used to assess the electronic and steric influences on the B=B double bond of various NHCs and electron-donating substituents on the thienyl ligands. Crystallographic data showed that the degree of coplanarity of the diborene core and thienyl groups is highly dependent on the sterics of the substituents. Furthermore, any increase in the electron- donating ability of the substituents resulted in the destabilization of the HOMO and greater instability of the resulting diborenes.
A circum-Arctic monitoring framework for quantifying annual erosion rates of permafrost coasts
(2023)
This study demonstrates a circum-Arctic monitoring framework for quantifying annual change of permafrost-affected coasts at a spatial resolution of 10 m. Frequent cloud coverage and challenging lighting conditions, including polar night, limit the usability of optical data in Arctic regions. For this reason, Synthetic Aperture RADAR (SAR) data in the form of annual median and standard deviation (sd) Sentinel-1 (S1) backscatter images covering the months June–September for the years 2017–2021 were computed. Annual composites for the year 2020 were hereby utilized as input for the generation of a high-quality coastline product via a Deep Learning (DL) workflow, covering 161,600 km of the Arctic coastline. The previously computed annual S1 composites for the years 2017 and 2021 were employed as input data for the Change Vector Analysis (CVA)-based coastal change investigation. The generated DL coastline product served hereby as a reference. Maximum erosion rates of up to 67 m per year could be observed based on 400 m coastline segments. Overall highest average annual erosion can be reported for the United States (Alaska) with 0.75 m per year, followed by Russia with 0.62 m per year. Out of all seas covered in this study, the Beaufort Sea featured the overall strongest average annual coastal erosion of 1.12 m. Several quality layers are provided for both the DL coastline product and the CVA-based coastal change analysis to assess the applicability and accuracy of the output products. The predicted coastal change rates show good agreement with findings published in previous literature. The proposed methods and data may act as a valuable tool for future analysis of permafrost loss and carbon emissions in Arctic coastal environments.
Permafrost degradation is observed all over the world as a consequence of climate change and the associated Arctic amplification, which has severe implications for the environment. Landslides, increased rates of surface deformation, rising likelihood of infrastructure damage, amplified coastal erosion rates, and the potential turnover of permafrost from a carbon sink to a carbon source are thereby exemplary implications linked to the thawing of frozen ground material. In this context, satellite earth observation is a potent tool for the identification and continuous monitoring of relevant processes and features on a cheap, long-term, spatially explicit, and operational basis as well as up to a circumpolar scale.
A total of 325 articles published in 30 different international journals during the past two decades were investigated on the basis of studied environmental foci, remote sensing platforms, sensor combinations, applied spatio-temporal resolutions, and study locations in an extensive review on past achievements, current trends, as well as future potentials and challenges of satellite earth observation for permafrost related analyses. The development of analysed environmental subjects, utilized sensors and platforms, and the number of annually published articles over time are addressed in detail. Studies linked to atmospheric features and processes, such as the release of greenhouse gas emissions, appear to be strongly under-represented. Investigations on the spatial distribution of study locations revealed distinct study clusters across the Arctic. At the same time, large sections of the continuous permafrost domain are only poorly covered and remain to be investigated in detail. A general trend towards increasing attention in satellite earth observation of permafrost and related processes and features was observed. The overall amount of published articles hereby more than doubled since the year 2015. New sources of satellite data, such as the Sentinel satellites and the Methane Remote Sensing LiDAR Mission (Merlin), as well as novel methodological approaches, such as data fusion and deep learning, will thereby likely improve our understanding of the thermal state and distribution of permafrost, and the effects of its degradation. Furthermore, cloud-based big data processing platforms (e.g. Google Earth Engine (GEE)) will further enable sophisticated and long-term analyses on increasingly larger scales and at high spatial resolutions.
In this thesis, a specific focus was put on Arctic permafrost coasts, which feature increasing vulnerability to environmental parameters, such as the thawing of frozen ground, and are therefore associated with amplified erosion rates. In particular, a novel monitoring framework for quantifying Arctic coastal erosion rates within the permafrost domain at high spatial resolution and on a circum-Arctic scale is presented within this thesis. Challenging illumination conditions and frequent cloud cover restrict the applicability of optical satellite imagery in Arctic regions. In order to overcome these limitations, Synthetic Aperture RADAR (SAR) data derived from Sentinel-1 (S1), which is largely independent from sun illumination and weather conditions, was utilized. Annual SAR composites covering the months June–September were combined with a Deep Learning (DL) framework and a Change Vector Analysis (CVA) approach to generate both a high-quality and circum-Arctic coastline product as well as a coastal change product that highlights areas of erosion and build-up. Annual composites in the form of standard deviation (sd) and median backscatter were computed and used as inputs for both the DL framework and the CVA coastal change quantification. The final DL-based coastline product covered a total of 161,600 km of Arctic coastline and featured a median accuracy of ±6.3 m to the manually digitized reference data. Annual coastal change quantification between 2017–2021 indicated erosion rates of up to 67 m per year for some areas based on 400 m coastal segments. In total, 12.24% of the investigated coastline featured an average erosion rate of 3.8 m per year, which corresponds to 17.83 km2 of annually eroded land area. Multiple quality layers associated to both products, the generated DL-coastline and the coastal change rates, are provided on a pixel basis to further assess the accuracy and applicability of the proposed data, methods, and products.
Lastly, the extracted circum-Arctic erosion rates were utilized as a basis in an experimental framework for estimating the amount of permafrost and carbon loss as a result of eroding permafrost coastlines. Information on permafrost fraction, Active Layer Thickness (ALT), soil carbon content, and surface elevation were thereby combined with the aforementioned erosion rates. While the proposed experimental framework provides a valuable outline for quantifying the volume loss of frozen ground and carbon release, extensive validation of the utilized environmental products and resulting volume loss numbers based on 200 m segments are necessary. Furthermore, data of higher spatial resolution and information of carbon content for deeper soil depths are required for more accurate estimates.
Climate change and associated Arctic amplification cause a degradation of permafrost which in turn has major implications for the environment. The potential turnover of frozen ground from a carbon sink to a carbon source, eroding coastlines, landslides, amplified surface deformation and endangerment of human infrastructure are some of the consequences connected with thawing permafrost. Satellite remote sensing is hereby a powerful tool to identify and monitor these features and processes on a spatially explicit, cheap, operational, long-term basis and up to circum-Arctic scale. By filtering after a selection of relevant keywords, a total of 325 articles from 30 international journals published during the last two decades were analyzed based on study location, spatio-
temporal resolution of applied remote sensing data, platform, sensor combination and studied environmental focus for a comprehensive overview of past achievements, current efforts, together with future challenges and opportunities. The temporal development of publication frequency, utilized platforms/sensors and the addressed environmental topic is thereby highlighted. The total
number of publications more than doubled since 2015. Distinct geographical study hot spots were revealed, while at the same time large portions of the continuous permafrost zone are still only sparsely covered by satellite remote sensing investigations. Moreover, studies related to Arctic greenhouse gas emissions in the context of permafrost degradation appear heavily underrepresented.
New tools (e.g., Google Earth Engine (GEE)), methodologies (e.g., deep learning or data fusion etc.)and satellite data (e.g., the Methane Remote Sensing LiDAR Mission (Merlin) and the Sentinel-fleet)will thereby enable future studies to further investigate the distribution of permafrost, its thermal state and its implications on the environment such as thermokarst features and greenhouse gas emission rates on increasingly larger spatial and temporal scales.
Introduction
Cold storage of platelets is considered to contribute to lower risk of bacterial growth and to more efficient hemostatic capacity. For the optimization of storage strategies, it is required to further elucidate the influence of refrigeration on platelet integrity. This study focused on adenosine diphosphate (ADP)-related platelet responsiveness.
Materials and Methods
Platelets were prepared from apheresis-derived platelet concentrates or from peripheral whole blood, stored either at room temperature or at 4°C. ADP-induced aggregation was tested with light transmission. Activation markers, purinergic receptor expression, and P2Y12 receptor function were determined by flow cytometry. P2Y1 and P2X1 function was assessed by fluorescence assays, cyclic nucleotide concentrations by immunoassays, and vasodilator-stimulated phosphoprotein (VASP)-phosphorylation levels by Western blot analysis.
Results
In contrast to room temperature, ADP-induced aggregation was maintained under cold storage for 6 days, associated with elevated activation markers like fibrinogen binding or CD62P expression. Purinergic receptor expression was not essentially different, whereas P2Y1 function deteriorated rapidly at cold storage, but not P2Y12 activity. Inhibitory pathways of cold-stored platelets were characterized by reduced responses to nitric oxide and prostaglandin E1. Refrigeration of citrated whole blood also led to the attenuation of induced inhibition of platelet aggregation, detectable within 24 hours.
Conclusion
ADP responsiveness is preserved under cold storage for 6 days due to stable P2Y12 activity and concomitant disintegration of inhibitory pathways enabling a higher reactivity of stored platelets. The ideal storage time at cold temperature for the highest hemostatic effect of platelets should be evaluated in further studies.
Exploring the potential of C-Band SAR in contributing to burn severity mapping in tropical savanna
(2019)
The ability to map burn severity and to understand how it varies as a function of time of year and return frequency is an important tool for landscape management and carbon accounting in tropical savannas. Different indices based on optical satellite imagery are typically used for mapping fire scars and for estimating burn severity. However, cloud cover is a major limitation for analyses using optical data over tropical landscapes. To address this pitfall, we explored the suitability of C-band Synthetic Aperture Radar (SAR) data for detecting vegetation response to fire, using experimental fires in northern Australia. Pre- and post-fire results from Sentinel-1 C-band backscatter intensity data were compared to those of optical satellite imagery and were corroborated against structural changes on the ground that we documented through terrestrial laser scanning (TLS). Sentinel-1 C-band backscatter (VH) proved sensitive to the structural changes imparted by fire and was correlated with the Normalised Burn Ratio (NBR) derived from Sentinel-2 optical data. Our results suggest that C-band SAR holds potential to inform the mapping of burn severity in savannas, but further research is required over larger spatial scales and across a broader spectrum of fire regime conditions before automated products can be developed. Combining both Sentinel-1 SAR and Sentinel-2 multi-spectral data will likely yield the best results for mapping burn severity under a range of weather conditions.
Platelet Toll-Like-Receptor-2 and -4 Mediate Different Immune-Related Responses to Bacterial Ligands
(2022)
Background
Like immune cells, platelets express toll-like receptors (TLRs) on their surface membrane. TLR2 and TLR4 are able to recognize bacterial antigens and have the potential to influence hemostatic functions and classical intracellular signaling pathways. This study investigated the role of TLR2 and TLR4 for immune-related functions in human platelets.
Materials and Methods
Washed platelets and neutrophils were prepared from fresh human peripheral blood. Basal-, Pam3CSK4- (as TLR2 agonist) and Lipopolysaccharides (LPS; as TLR4 agonist) -induced CD62P expression, fibrinogen binding and TLR2 or TLR4 expression, intracellular reactive oxygen species (ROS) production in H2DCFDA-loaded platelets and uptake of fluorescence-labeled TLR ligands, and fluorophore-conjugated fibrinogen were evaluated by flow cytometry. Analysis of platelet–neutrophil complexes was performed after coincubation of washed platelets and neutrophils in the presence and absence of TLR2 or TLR4 agonists on poly-L-lysine coated surfaces, followed by immunostaining and immunofluorescence imaging.
Results
Pam3CSK4 rapidly and transiently increased TLR2 and TLR4 expression. Over the course of 30 minutes after activation with Pam3CSK4 and LPS, the expression of both receptors decreased. Pam3CSK4-stimulated intracellular ROS production and the uptake of TLR ligands or fibrinogen much stronger than LPS. Besides, TLR4 activation led to a significant increase of platelet–neutrophil contacts.
Conclusion
Stimulation leads to rapid mobilization of TLR2 or TLR4 to the platelet surface, presumably followed by receptor internalization along with bound TLR ligands. After activation, platelet TLR2 and TLR4 mediate different immune-related reactions. In particular, TLR2 induces intracellular responses in platelets, whereas TLR4 initiates interactions with other immune cells such as neutrophils.
The mitotic spindle assembly checkpoint (SAC) maintains genome stability and marks an important target for antineoplastic therapies. However, it has remained unclear how cells execute cell fate decisions under conditions of SAC‐induced mitotic arrest. Here, we identify USP9X as the mitotic deubiquitinase of the X‐linked inhibitor of apoptosis protein (XIAP) and demonstrate that deubiquitylation and stabilization of XIAP by USP9X lead to increased resistance toward mitotic spindle poisons. We find that primary human aggressive B‐cell lymphoma samples exhibit high USP9X expression that correlate with XIAP overexpression. We show that high USP9X/XIAP expression is associated with shorter event‐free survival in patients treated with spindle poison‐containing chemotherapy. Accordingly, aggressive B‐cell lymphoma lines with USP9X and associated XIAP overexpression exhibit increased chemoresistance, reversed by specific inhibition of either USP9X or XIAP. Moreover, knockdown of USP9X or XIAP significantly delays lymphoma development and increases sensitivity to spindle poisons in a murine Eμ‐Myc lymphoma model. Together, we specify the USP9X–XIAP axis as a regulator of the mitotic cell fate decision and propose that USP9X and XIAP are potential prognostic biomarkers and therapeutic targets in aggressive B‐cell lymphoma.
Thin films of transition metal oxides open up a gateway to nanoscale electronic devices beyond silicon characterized by novel electronic functionalities. While such films are commonly prepared in an oxygen atmosphere, they are typically considered to be ideally terminated with the stoichiometric composition. Using the prototypical correlated metal SrVO\(_{3}\) as an example, it is demonstrated that this idealized description overlooks an essential ingredient: oxygen adsorbing at the surface apical sites. The oxygen adatoms, which are present even if the films are kept in an ultrahigh vacuum environment and not explicitly exposed to air, are shown to severely affect the intrinsic electronic structure of a transition metal oxide film. Their presence leads to the formation of an electronically dead surface layer but also alters the band filling and the electron correlations in the thin films. These findings highlight that it is important to take into account surface apical oxygen or—mutatis mutandis—the specific oxygen configuration imposed by a capping layer to predict the behavior of ultrathin films of transition metal oxides near the single unit-cell limit.
The Essential Climate Variable (ECV) Permafrost is currently undergoing strong changes due to rising ground and air temperatures. Surface movement, forming characteristic landforms such as rock glaciers, is one key indicator for mountain permafrost. Monitoring this movement can indicate ongoing changes in permafrost; therefore, rock glacier velocity (RGV) has recently been added as an ECV product. Despite the increased understanding of rock glacier dynamics in recent years, most observations are either limited in terms of the spatial coverage or temporal resolution. According to recent studies, Sentinel-1 (C-band) Differential SAR Interferometry (DInSAR) has potential for monitoring RGVs at high spatial and temporal resolutions. However, the suitability of DInSAR for the detection of heterogeneous small-scale spatial patterns of rock glacier velocities was never at the center of these studies. We address this shortcoming by generating and analyzing Sentinel-1 DInSAR time series over five years to detect small-scale displacement patterns of five high alpine permafrost environments located in the Central European Alps on a weekly basis at a range of a few millimeters. Our approach is based on a semi-automated procedure using open-source programs (SNAP, pyrate) and provides East-West displacement and elevation change with a ground sampling distance of 5 m. Comparison with annual movement derived from orthophotos and unpiloted aerial vehicle (UAV) data shows that DInSAR covers about one third of the total movement, which represents the proportion of the year suited for DInSAR, and shows good spatial agreement (Pearson R: 0.42–0.74, RMSE: 4.7–11.6 cm/a) except for areas with phase unwrapping errors. Moreover, the DInSAR time series unveils spatio-temporal variations and distinct seasonal movement dynamics related to different drivers and processes as well as internal structures. Combining our approach with in situ observations could help to achieve a more holistic understanding of rock glacier dynamics and to assess the future evolution of permafrost under changing climatic conditions.
Arctic permafrost coasts become increasingly vulnerable due to environmental drivers such as the reduced sea-ice extent and duration as well as the thawing of permafrost itself. A continuous quantification of the erosion process on large to circum-Arctic scales is required to fully assess the extent and understand the consequences of eroding permafrost coastlines. This study presents a novel approach to quantify annual Arctic coastal erosion and build-up rates based on Sentinel-1 (S1) Synthetic Aperture RADAR (SAR) backscatter data, in combination with Deep Learning (DL) and Change Vector Analysis (CVA). The methodology includes the generation of a high-quality Arctic coastline product via DL, which acted as a reference for quantifying coastal erosion and build-up rates from annual median and standard deviation (sd) backscatter images via CVA. The analysis was applied on ten test sites distributed across the Arctic and covering about 1038 km of coastline. Results revealed maximum erosion rates of up to 160 m for some areas and an average erosion rate of 4.37 m across all test sites within a three-year temporal window from 2017 to 2020. The observed erosion rates within the framework of this study agree with findings published in the previous literature. The proposed methods and data can be applied on large scales and, prospectively, even for the entire Arctic. The generated products may be used for quantifying the loss of frozen ground, estimating the release of stored organic material, and can act as a basis for further related studies in Arctic coastal environments.
Forest systems provide crucial ecosystem functions to our environment, such as balancing carbon stocks and influencing the local, regional and global climate. A trend towards an increasing frequency of climate change induced extreme weather events, including drought, is hereby a major challenge for forest management. Within this context, the application of remote sensing data provides a powerful means for fast, operational and inexpensive investigations over large spatial scales and time. This study was dedicated to explore the potential of satellite data in combination with harmonic analyses for quantifying the vegetation response to drought events in German forests. The harmonic modelling method was compared with a z-score standardization approach and correlated against both, meteorological and topographical data. Optical satellite imagery from Landsat and the Moderate Resolution Imaging Spectroradiometer (MODIS) was used in combination with three commonly applied vegetation indices. Highest correlation scores based on the harmonic modelling technique were computed for the 6th harmonic degree. MODIS imagery in combination with the Normalized Difference Vegetation Index (NDVI) generated hereby best results for measuring spectral response to drought conditions. Strongest correlation between remote sensing data and meteorological measures were observed for soil moisture and the self-calibrated Palmer Drought Severity Index (scPDSI). Furthermore, forests regions over sandy soils with pine as the dominant tree type were identified to be particularly vulnerable to drought. In addition, topographical analyses suggested mitigated drought affects along hill slopes. While the proposed approaches provide valuable information about vegetation dynamics as a response to meteorological weather conditions, standardized in-situ measurements over larger spatial scales and related to drought quantification are required for further in-depth quality assessment of the used methods and data.
Background and Objectives
Immunoadsorptions (IA) are used to remove autoantibodies from the plasma in autoimmune disorders. In this study, we evaluated the effects of a single-use, recombinant staphylococcal protein A-based immunoadsorber on blood composition of the patient.
Materials and Methods
In a cohort of patients with myasthenia gravis or stiff-person syndrome, essential parameters of blood cell count, coagulation, clinical chemistry or plasma proteins and immunoglobulins (Ig) were measured before and after IA (n = 11).
Results
In average, IA reduced the levels of total IgG, IgG1, IgG2 and IgG4 by approximately 60%, the acetylcholine receptor autoantibody levels by more than 70%. IgG3, IgA or IgM were diminished to a lower extent. In contrast to fibrinogen or other coagulation factors, the column markedly removed vitamin K-dependent coagulation factors II, VII, IX and X by approximately 40%–70%. Accordingly, international normalized ratio and activated partial thromboplastin time were increased after IA by 59.1% and 32.7%, respectively. Coagulation tests almost returned to baseline values within 24 h. Blood cell count, electrolytes, total protein or albumin were not essentially affected. No clinical events occurred.
Conclusion
The single-use, multiple-pass protein A adsorber column is highly efficient to remove IgG1, IgG2 and IgG4 or specific acetylcholine receptor autoantibodies from the plasma. Coagulation parameters should be monitored, since the column has the capacity to largely reduce vitamin K-dependent factors.
Storage of platelet concentrates (PC) at cold temperature (CT) is discussed as an alternative to the current standard of storage at room temperature (RT). Recently, we could show that cold-induced attenuation of inhibitory signaling is an important mechanism promoting platelet reactivity. For developing strategies in blood banking, it is required to elucidate the time-dependent onset of facilitated platelet activation. Thus, freshly prepared platelet-rich-plasma (PRP) was stored for 1 and 2 h at CT (2–6 °C) or at RT (20–24 °C), followed by subsequent comparative analysis. Compared to RT, basal and induced vasodilator-stimulated phosphoprotein (VASP) phosphorylation levels were decreased under CT within 1 h by approximately 20%, determined by Western blot analysis and flow cytometry. Concomitantly, ADP- and collagen-induced threshold aggregation values were enhanced by up to 30–40%. Furthermore, platelet-covered areas on collagen-coated slides and aggregate formation under flow conditions were increased after storage at CT, in addition to induced activation markers. In conclusion, a time period of 1–2 h for refrigeration is sufficient to induce an attenuation of inhibitory signaling, accompanied with an enhancement of platelet responsiveness. Short-term refrigeration may be considered as a rational approach to obtain PC with higher functional reactivity for the treatment of hemorrhage.