TY - JOUR A1 - Yu, Hongtao A1 - Quan, Ting A1 - Mei, Shilin A1 - Kochovski, Zdravko A1 - Huang, Wei A1 - Meng, Hong A1 - Lu, Yan T1 - Prompt Electrodeposition of Ni Nanodots on Ni Foam to Construct a High-Performance Water-Splitting Electrode BT - Efficient, Scalable, and Recyclable JF - Nano-Micro Letters N2 - HighlightsFacile electrodeposition for fabricating active Ni nanodots (NiNDs) on Ni foam (NF) is shown.Binder- and heteroatom-free recyclable NiO/NiNDs@NF electrodes are efficiently made.NiO/NiNDs@NF bifunctional catalytic electrodes are used for water splitting. AbstractIn past decades, Ni-based catalytic materials and electrodes have been intensively explored as low-cost hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) catalysts for water splitting. With increasing demands for Ni worldwide, simplifying the fabrication process, increasing Ni recycling, and reducing waste are tangible sustainability goals. Here, binder-free, heteroatom-free, and recyclable Ni-based bifunctional catalytic electrodes were fabricated via a one-step quick electrodeposition method. Typically, active Ni nanodot (NiND) clusters are electrodeposited on Ni foam (NF) in Ni(NO3)(2) acetonitrile solution. After drying in air, NiO/NiND composites are obtained, leading to a binder-free and heteroatom-free NiO/NiNDs@NF catalytic electrode. The electrode shows high efficiency and long-term stability for catalyzing hydrogen and oxygen evolution reactions at low overpotentials ((10)(HER)=119mV and (50)(OER)=360mV) and can promote water catalysis at 1.70V@10mAcm(-2). More importantly, the recovery of raw materials (NF and Ni(NO3)(2)) is quite easy because of the solubility of NiO/NiNDs composites in acid solution for recycling the electrodes. Additionally, a large-sized (S similar to 70cm(2)) NiO/NiNDs@NF catalytic electrode with high durability has also been constructed. This method provides a simple and fast technology to construct high-performance, low-cost, and environmentally friendly Ni-based bifunctional electrocatalytic electrodes for water splitting. KW - Electrodeposition KW - Ni nanodots KW - Bifunctional catalysts KW - Water splitting KW - Large-size Y1 - 2019 U6 - https://doi.org/10.1007/s40820-019-0269-x SN - 2311-6706 SN - 2150-5551 VL - 11 IS - 41 PB - Shanghai JIAO TONG univ press CY - Shanghai ER - TY - JOUR A1 - Schwarze, Martin A1 - Schellhammer, Karl Sebastian A1 - Ortstein, Katrin A1 - Benduhn, Johannes A1 - Gaul, Christopher A1 - Hinderhofer, Alexander A1 - Perdigón-Toro, Lorena A1 - Scholz, Reinhard A1 - Kublitski, Jonas A1 - Roland, Steffen A1 - Lau, Matthias A1 - Poelking, Carl A1 - Andrienko, Denis A1 - Cuniberti, Gianaurelio A1 - Schreiber, Frank A1 - Neher, Dieter A1 - Vandewal, Koen A1 - Ortmann, Frank A1 - Leo, Karl T1 - Impact of molecular quadrupole moments on the energy levels at organic heterojunctions JF - Nature Communications N2 - The functionality of organic semiconductor devices crucially depends on molecular energies, namely the ionisation energy and the electron affinity. Ionisation energy and electron affinity values of thin films are, however, sensitive to film morphology and composition, making their prediction challenging. In a combined experimental and simulation study on zinc-phthalocyanine and its fluorinated derivatives, we show that changes in ionisation energy as a function of molecular orientation in neat films or mixing ratio in blends are proportional to the molecular quadrupole component along the p-p-stacking direction. We apply these findings to organic solar cells and demonstrate how the electrostatic interactions can be tuned to optimise the energy of the charge-transfer state at the donor-acceptor interface and the dissociation barrier for free charge carrier generation. The confirmation of the correlation between interfacial energies and quadrupole moments for other materials indicates its relevance for small molecules and polymers. Y1 - 2019 U6 - https://doi.org/10.1038/s41467-019-10435-2 SN - 2041-1723 VL - 10 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Pisoni, Stefano A1 - Stolterfoht, Martin A1 - Lockinger, Johannes A1 - Moser, Thierry A1 - Jiang, Yan A1 - Caprioglio, Pietro A1 - Neher, Dieter A1 - Buecheler, Stephan A1 - Tiwari, Ayodhya N. T1 - On the origin of open-circuit voltage losses in flexible n-i-p perovskite solar cells JF - Science and technology of advanced materials : STAM N2 - The possibility to manufacture perovskite solar cells (PSCs) at low temperatures paves the way to flexible and lightweight photovoltaic (PV) devices manufactured via high-throughput roll-to-roll processes. In order to achieve higher power conversion efficiencies, it is necessary to approach the radiative limit via suppression of non-radiative recombination losses. Herein, we performed a systematic voltage loss analysis for a typical low-temperature processed, flexible PSC in n-i-p configuration using vacuum deposited C-60 as electron transport layer (ETL) and two-step hybrid vacuum-solution deposition for CH3NH3PbI3 perovskite absorber. We identified the ETL/absorber interface as a bottleneck in relation to non-radiative recombination losses, the quasi-Fermi level splitting (QFLS) decreases from similar to 1.23 eV for the bare absorber, just similar to 90 meV below the radiative limit, to similar to 1.10 eV when C-60 is used as ETL. To effectively mitigate these voltage losses, we investigated different interfacial modifications via vacuum deposited interlayers (BCP, B4PyMPM, 3TPYMB, and LiF). An improvement in QFLS of similar to 30-40 meV is observed after interlayer deposition and confirmed by comparable improvements in the open-circuit voltage after implementation of these interfacial modifications in flexible PSCs. Further investigations on absorber/hole transport layer (HTL) interface point out the detrimental role of dopants in Spiro-OMeTAD film (widely employed HTL in the community) as recombination centers upon oxidation and light exposure. [GRAPHICS] . KW - Perovskite solar cell KW - flexible KW - interface engineering KW - non-radiative recombination KW - quasi-Fermi level splitting Y1 - 2019 U6 - https://doi.org/10.1080/14686996.2019.1633952 SN - 1468-6996 SN - 1878-5514 VL - 20 SP - 786 EP - 795 PB - Taylor & Francis CY - Abingdon ER - TY - JOUR A1 - Seroussi, Helene A1 - Nowicki, Sophie A1 - Simon, Erika A1 - Abe-Ouchi, Ayako A1 - Albrecht, Torsten A1 - Brondex, Julien A1 - Cornford, Stephen A1 - Dumas, Christophe A1 - Gillet-Chaulet, Fabien A1 - Goelzer, Heiko A1 - Golledge, Nicholas R. A1 - Gregory, Jonathan M. A1 - Greve, Ralf A1 - Hoffman, Matthew J. A1 - Humbert, Angelika A1 - Huybrechts, Philippe A1 - Kleiner, Thomas A1 - Larourl, Eric A1 - Leguy, Gunter A1 - Lipscomb, William H. A1 - Lowry, Daniel A1 - Mengel, Matthias A1 - Morlighem, Mathieu A1 - Pattyn, Frank A1 - Payne, Anthony J. A1 - Pollard, David A1 - Price, Stephen F. A1 - Quiquet, Aurelien A1 - Reerink, Thomas J. A1 - Reese, Ronja A1 - Rodehacke, Christian B. A1 - Schlegel, Nicole-Jeanne A1 - Shepherd, Andrew A1 - Sun, Sainan A1 - Sutter, Johannes A1 - Van Breedam, Jonas A1 - van de Wal, Roderik S. W. A1 - Winkelmann, Ricarda A1 - Zhang, Tong T1 - initMIP-Antarctica BT - an ice sheet model initialization experiment of ISMIP6 JF - The Cryosphere : TC ; an interactive open access journal of the European Geosciences Union N2 - Ice sheet numerical modeling is an important tool to estimate the dynamic contribution of the Antarctic ice sheet to sea level rise over the coming centuries. The influence of initial conditions on ice sheet model simulations, however, is still unclear. To better understand this influence, an initial state intercomparison exercise (initMIP) has been developed to compare, evaluate, and improve initialization procedures and estimate their impact on century-scale simulations. initMlP is the first set of experiments of the Ice Sheet Model Intercomparison Project for CMIP6 (ISMIP6), which is the primary Coupled Model Intercomparison Project Phase 6 (CMIP6) activity focusing on the Greenland and Antarctic ice sheets. Following initMlP-Greenland, initMlP-Antarctica has been designed to explore uncertainties associated with model initialization and spin-up and to evaluate the impact of changes in external forcings. Starting from the state of the Antarctic ice sheet at the end of the initialization procedure, three forward experiments are each run for 100 years: a control run, a run with a surface mass balance anomaly, and a run with a basal melting anomaly beneath floating ice. This study presents the results of initMlP-Antarctica from 25 simulations performed by 16 international modeling groups. The submitted results use different initial conditions and initialization methods, as well as ice flow model parameters and reference external forcings. We find a good agreement among model responses to the surface mass balance anomaly but large variations in responses to the basal melting anomaly. These variations can be attributed to differences in the extent of ice shelves and their upstream tributaries, the numerical treatment of grounding line, and the initial ocean conditions applied, suggesting that ongoing efforts to better represent ice shelves in continental-scale models should continue. Y1 - 2019 U6 - https://doi.org/10.5194/tc-13-1441-2019 SN - 1994-0416 SN - 1994-0424 VL - 13 IS - 5 SP - 1441 EP - 1471 PB - Copernicus CY - Göttingen ER - TY - JOUR A1 - Pick, Leonie A1 - Effenberger, Frederic A1 - Zhelavskaya, Irina A1 - Korte, Monika T1 - A Statistical Classifier for Historical Geomagnetic Storm Drivers Derived Solely From Ground-Based Magnetic Field Measurements JF - Earth and Space Science N2 - Solar wind observations show that geomagnetic storms are mainly driven by interplanetary coronal mass ejections (ICMEs) and corotating or stream interaction regions (C/SIRs). We present a binary classifier that assigns one of these drivers to 7,546 storms between 1930 and 2015 using ground‐based geomagnetic field observations only. The input data consists of the long‐term stable Hourly Magnetospheric Currents index alongside the corresponding midlatitude geomagnetic observatory time series. This data set provides comprehensive information on the global storm time magnetic disturbance field, particularly its spatial variability, over eight solar cycles. For the first time, we use this information statistically with regard to an automated storm driver identification. Our supervised classification model significantly outperforms unskilled baseline models (78% accuracy with 26[19]% misidentified interplanetary coronal mass ejections [corotating or stream interaction regions]) and delivers plausible driver occurrences with regard to storm intensity and solar cycle phase. Our results can readily be used to advance related studies fundamental to space weather research, for example, studies connecting galactic cosmic ray modulation and geomagnetic disturbances. They are fully reproducible by means of the underlying open‐source software (Pick, 2019, http://doi.org/10.5880/GFZ.2.3.2019.003) KW - geomagnetic observatory data KW - geomagnetic storm drivers KW - historical geomagnetic storms KW - supervised machine learning Y1 - 2019 U6 - https://doi.org/10.1029/2019EA000726 SN - 2333-5084 VL - 6 SP - 2000 EP - 2015 PB - American Geophysical Union CY - Malden, Mass. ER - TY - JOUR A1 - Herzschuh, Ulrike A1 - Cao, Xianyong A1 - Laepple, Thomas A1 - Dallmeyer, Anne A1 - Telford, Richard J. A1 - Ni, Jian A1 - Chen, Fahu A1 - Kong, Zhaochen A1 - Liu, Guangxiu A1 - Liu, Kam-Biu A1 - Liu, Xingqi A1 - Stebich, Martina A1 - Tang, Lingyu A1 - Tian, Fang A1 - Wang, Yongbo A1 - Wischnewski, Juliane A1 - Xu, Qinghai A1 - Yan, Shun A1 - Yang, Zhenjing A1 - Yu, Ge A1 - Zhang, Yun A1 - Zhao, Yan A1 - Zheng, Zhuo T1 - Position and orientation of the westerly jet determined Holocene rainfall patterns in China JF - Nature Communications N2 - Proxy-based reconstructions and modeling of Holocene spatiotemporal precipitation patterns for China and Mongolia have hitherto yielded contradictory results indicating that the basic mechanisms behind the East Asian Summer Monsoon and its interaction with the westerly jet stream remain poorly understood. We present quantitative reconstructions of Holocene precipitation derived from 101 fossil pollen records and analyse them with the help of a minimal empirical model. We show that the westerly jet-stream axis shifted gradually southward and became less tilted since the middle Holocene. This was tracked by the summer monsoon rain band resulting in an early-Holocene precipitation maximum over most of western China, a mid-Holocene maximum in north-central and northeastern China, and a late-Holocene maximum in southeastern China. Our results suggest that a correct simulation of the orientation and position of the westerly jet stream is crucial to the reliable prediction of precipitation patterns in China and Mongolia. Y1 - 2019 U6 - https://doi.org/10.1038/s41467-019-09866-8 SN - 2041-1723 VL - 10 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Zimmermann, Heike Hildegard A1 - Harms, Lars A1 - Epp, Laura Saskia A1 - Mewes, Nick A1 - Bernhardt, Nadine A1 - Kruse, Stefan A1 - Stoof-Leichsenring, Kathleen Rosemarie A1 - Pestryakova, Luidmila Agafyevna A1 - Wieczorek, Mareike A1 - Trense, Daronja A1 - Herzschuh, Ulrike T1 - Chloroplast and mitochondrial genetic variation of larches at the Siberian tundrataiga ecotone revealed by de novo assembly JF - PLoS one N2 - Larix populations at the tundra-taiga ecotone in northern Siberia are highly under-represented in population genetic studies, possibly due to the remoteness of these regions that can only be accessed at extraordinary expense. The genetic signatures of populations in these boundary regions are therefore largely unknown. We aim to generate organelle reference genomes for the detection of single nucleotide polymorphisms (SNPs) that can be used for paleogenetic studies. We present 19 complete chloroplast genomes and mitochondrial genomic sequences of larches from the southern lowlands of the Taymyr Peninsula (northernmost range of Larix gmelinii (Rupr.) Kuzen.), the lower Omoloy River, and the lower Kolyma River (both in the range of Larix cajanderi Mayr). The genomic data reveal 84 chloroplast SNPs and 213 putatively mitochondrial SNPs. Parsimony-based chloroplast haplotype networks show no spatial structure of individuals from different geographic origins, while the mitochondrial haplotype network shows at least a slight spatial structure with haplotypes from the Omoloy and Kolyma populations being more closely related to each other than to most of the haplotypes from the Taymyr populations. Whole genome alignments with publicly available complete chloroplast genomes of different Larix species show that among official plant barcodes only the rcbL gene contains sufficient polymorphisms, but has to be sequenced completely to distinguish the different provenances. We provide 8 novel mitochondrial SNPs that are putatively diagnostic for the separation of L. gmelinii and L. cajanderi, while 4 chloroplast SNPs have the potential to distinguish the L. gmelinii/ L. cajanderi group from other Larix species. Our organelle references can be used for a targeted primer and probe design allowing the generation of short amplicons. This is particularly important with regard to future investigations of, for example, the biogeographic history of Larix by screening ancient sedimentary DNA of Larix. Y1 - 2019 U6 - https://doi.org/10.1371/journal.pone.0216966 SN - 1932-6203 VL - 14 IS - 7 PB - PLoS CY - San Fransisco ER - TY - JOUR A1 - Cao, Xianyong A1 - Tian, Fang A1 - Li, Furong A1 - Gaillard, Marie-Jose A1 - Rudaya, Natalia A1 - Xu, Qinghai A1 - Herzschuh, Ulrike T1 - Pollen-based quantitative land-cover reconstruction for northern Asia covering the last 40 ka cal BP JF - Climate of the past : an interactive open access journal of the European Geosciences Union N2 - We collected the available relative pollen productivity estimates (PPEs) for 27 major pollen taxa from Eurasia and applied them to estimate plant abundances during the last 40 ka cal BP (calibrated thousand years before present) using pollen counts from 203 fossil pollen records in northern Asia (north of 40 degrees N). These pollen records were organized into 42 site groups and regional mean plant abundances calculated using the REVEALS (Regional Estimates of Vegetation Abundance from Large Sites) model. Time-series clustering, constrained hierarchical clustering, and detrended canonical correspondence analysis were performed to investigate the regional pattern, time, and strength of vegetation changes, respectively. Reconstructed regional plant functional type (PFT) components for each site group are generally consistent with modern vegetation in that vegetation changes within the regions are characterized by minor changes in the abundance of PFTs rather than by an increase in new PFTs, particularly during the Holocene. We argue that pollen-based REVEALS estimates of plant abundances should be a more reliable reflection of the vegetation as pollen may overestimate the turnover, particularly when a high pollen producer invades areas dominated by low pollen producers. Comparisons with vegetation-independent climate records show that climate change is the primary factor driving land-cover changes at broad spatial and temporal scales. Vegetation changes in certain regions or periods, however, could not be explained by direct climate change, e.g. inland Siberia, where a sharp increase in evergreen conifer tree abundance occurred at ca. 7-8 ka cal BP despite an unchanging climate, potentially reflecting their response to complex climate-permafrost-fire-vegetation interactions and thus a possible long-term lagged climate response. Y1 - 2019 U6 - https://doi.org/10.5194/cp-15-1503-2019 SN - 1814-9324 SN - 1814-9332 VL - 15 IS - 4 SP - 1503 EP - 1536 PB - Copernicus CY - Göttingen ER - TY - JOUR A1 - Kruse, Stefan A1 - Gerdes, Alexander A1 - Kath, Nadja J. A1 - Epp, Laura Saskia A1 - Stoof-Leichsenring, Kathleen Rosemarie A1 - Pestryakova, Luidmila Agafyevna A1 - Herzschuh, Ulrike T1 - Dispersal distances and migration rates at the arctic treeline in Siberia - a genetic and simulation-based study JF - Biogeosciences N2 - A strong temperature increase in the Arctic is expected to lead to latitudinal treeline shift. This tundra-taiga turnover would cause a positive vegetation-climate feedback due to albedo decrease. However, reliable estimates of tree migration rates are currently lacking due to the complex processes involved in forest establishment, which depend strongly on seed dispersal. We aim to fill this gap using LAVESI, an individual-based and spatially explicit Larix vegetation simulator. LAVESI was designed to simulate plots within homogeneous forests. Here, we improve the implementation of the seed dispersal function via field-based investigations. We inferred the effective seed dispersal distances of a typical open-forest stand on the southern Taymyr Peninsula (northern central Siberia) from genetic parentage analysis using eight nuclear microsatellite markers. The parentage analysis gives effective seed dispersal distances (median similar to 10 m) close to the seed parents. A comparison between simulated and observed effective seed dispersal distances reveals an overestimation of recruits close to the releasing tree and a shorter dispersal distance generally. We thus adapted our model and used the newly parameterised version to simulate south-to-north transects; a slow-moving treeline front was revealed. The colonisation of the tundra areas was assisted by occasional long-distance seed dispersal events beyond the treeline area. The treeline (similar to 1 tree ha(-1)) advanced by similar to 1.6 m yr(-1), whereas the forest line (similar to 100 trees ha(-1)) advanced by only similar to 0.6 m yr(-1). We conclude that the treeline in northern central Siberia currently lags behind the current strong warming and will continue to lag in the near future. Y1 - 2019 U6 - https://doi.org/10.5194/bg-16-1211-2019 SN - 1726-4170 SN - 1726-4189 VL - 16 IS - 6 SP - 1211 EP - 1224 PB - Copernicus CY - Göttingen ER - TY - JOUR A1 - Brieger, Frederic A1 - Herzschuh, Ulrike A1 - Pestryakova, Luidmila Agafyevna A1 - Bookhagen, Bodo A1 - Zakharov, Evgenii S. A1 - Kruse, Stefan T1 - Advances in the Derivation of Northeast Siberian Forest Metrics Using High-Resolution UAV-Based Photogrammetric Point Clouds JF - Remote sensing N2 - Forest structure is a crucial component in the assessment of whether a forest is likely to act as a carbon sink under changing climate. Detailed 3D structural information about the tundra–taiga ecotone of Siberia is mostly missing and still underrepresented in current research due to the remoteness and restricted accessibility. Field based, high-resolution remote sensing can provide important knowledge for the understanding of vegetation properties and dynamics. In this study, we test the applicability of consumer-grade Unmanned Aerial Vehicles (UAVs) for rapid calculation of stand metrics in treeline forests. We reconstructed high-resolution photogrammetric point clouds and derived canopy height models for 10 study sites from NE Chukotka and SW Yakutia. Subsequently, we detected individual tree tops using a variable-window size local maximum filter and applied a marker-controlled watershed segmentation for the delineation of tree crowns. With this, we successfully detected 67.1% of the validation individuals. Simple linear regressions of observed and detected metrics show a better correlation (R2) and lower relative root mean square percentage error (RMSE%) for tree heights (mean R2 = 0.77, mean RMSE% = 18.46%) than for crown diameters (mean R2 = 0.46, mean RMSE% = 24.9%). The comparison between detected and observed tree height distributions revealed that our tree detection method was unable to representatively identify trees <2 m. Our results show that plot sizes for vegetation surveys in the tundra–taiga ecotone should be adapted to the forest structure and have a radius of >15–20 m to capture homogeneous and representative forest stands. Additionally, we identify sources of omission and commission errors and give recommendations for their mitigation. In summary, the efficiency of the used method depends on the complexity of the forest’s stand structure. KW - UAV KW - photogrammetry KW - remote sensing KW - structure from motion KW - tundra-taiga ecotone KW - point cloud KW - forest structure Y1 - 2019 U6 - https://doi.org/10.3390/rs11121447 SN - 2072-4292 VL - 11 IS - 12 PB - MDPI CY - Basel ER -