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- ItemSingle molecule magnet with an unpaired electron trapped between two lanthanide ions inside a fullerene(London : Nature Publishing Group, 2017) Liu, F.; Krylov, D.S.; Spree, L.; Avdoshenko, S.M.; Samoylova, N.A.; Rosenkranz, M.; Kostanyan, A.; Greber, T.; Wolter, A.U.B.; Büchner, B.; Popov, A.A.Increasing the temperature at which molecules behave as single-molecule magnets is a serious challenge in molecular magnetism. One of the ways to address this problem is to create the molecules with strongly coupled lanthanide ions. In this work, endohedral metallofullerenes Y 2 @C 80 and Dy 2 @C 80 are obtained in the form of air-stable benzyl monoadducts. Both feature an unpaired electron trapped between metal ions, thus forming a single-electron metal-metal bond. Giant exchange interactions between lanthanide ions and the unpaired electron result in single-molecule magnetism of Dy 2 @C 80 (CH 2 Ph) with a record-high 100 s blocking temperature of 18 K. All magnetic moments in Dy 2 @C 80 (CH 2 Ph) are parallel and couple ferromagnetically to form a single spin unit of 21 μ B with a dysprosium-electron exchange constant of 32 cm -1. The barrier of the magnetization reversal of 613 K is assigned to the state in which the spin of one Dy centre is flipped.
- ItemSelf-amplified Amazon forest loss due to vegetation-atmosphere feedbacks(London : Nature Publishing Group, 2017) Zemp, D.C.; Schleussner, C.-F.; Barbosa, H.M.J.; Hirota, M.; Montade, V.; Sampaio, G.; Staal, A.; Wang-Erlandsson, L.; Rammig, A.Reduced rainfall increases the risk of forest dieback, while in return forest loss might intensify regional droughts. The consequences of this vegetation-atmosphere feedback for the stability of the Amazon forest are still unclear. Here we show that the risk of self-amplified Amazon forest loss increases nonlinearly with dry-season intensification. We apply a novel complex-network approach, in which Amazon forest patches are linked by observation-based atmospheric water fluxes. Our results suggest that the risk of self-amplified forest loss is reduced with increasing heterogeneity in the response of forest patches to reduced rainfall. Under dry-season Amazonian rainfall reductions, comparable to Last Glacial Maximum conditions, additional forest loss due to self-amplified effects occurs in 10-13% of the Amazon basin. Although our findings do not indicate that the projected rainfall changes for the end of the twenty-first century will lead to complete Amazon dieback, they suggest that frequent extreme drought events have the potential to destabilize large parts of the Amazon forest.
- ItemUnderstanding the origin of Paris Agreement emission uncertainties(London : Nature Publishing Group, 2017) Rogelj, J.; Fricko, O.; Meinshausen, M.; Krey, V.; Zilliacus, J.J.J.; Riahi, K.The UN Paris Agreement puts in place a legally binding mechanism to increase mitigation action over time. Countries put forward pledges called nationally determined contributions (NDC) whose impact is assessed in global stocktaking exercises. Subsequently, actions can then be strengthened in light of the Paris climate objective: Limiting global mean temperature increase to well below 2 °C and pursuing efforts to limit it further to 1.5 °C. However, pledged actions are currently described ambiguously and this complicates the global stocktaking exercise. Here, we systematically explore possible interpretations of NDC assumptions, and show that this results in estimated emissions for 2030 ranging from 47 to 63 GtCO2e yr-1. We show that this uncertainty has critical implications for the feasibility and cost to limit warming well below 2 °C and further to 1.5 °C. Countries are currently working towards clarifying the modalities of future NDCs. We identify salient avenues to reduce the overall uncertainty by about 10 percentage points through simple, technical clarifications regarding energy accounting rules. Remaining uncertainties depend to a large extent on politically valid choices about how NDCs are expressed, and therefore raise the importance of a thorough and robust process that keeps track of where emissions are heading over time.
- ItemWater scarcity hotspots travel downstream due to human interventions in the 20th and 21st century(London : Nature Publishing Group, 2017) Veldkamp, T.I.E.; Wada, Y.; Aerts, J.C.J.H.; Döll, P.; Gosling, S.N.; Liu, J.; Masaki, Y.; Oki, T.; Ostberg, S.; Pokhrel, Y.; Satoh, Y.; Kim, H.; Ward, P.J.Water scarcity is rapidly increasing in many regions. In a novel, multi-model assessment, we examine how human interventions (HI: land use and land cover change, man-made reservoirs and human water use) affected monthly river water availability and water scarcity over the period 1971-2010. Here we show that HI drastically change the critical dimensions of water scarcity, aggravating water scarcity for 8.8% (7.4-16.5%) of the global population but alleviating it for another 8.3% (6.4-15.8%). Positive impacts of HI mostly occur upstream, whereas HI aggravate water scarcity downstream; HI cause water scarcity to travel downstream. Attribution of water scarcity changes to HI components is complex and varies among the hydrological models. Seasonal variation in impacts and dominant HI components is also substantial. A thorough consideration of the spatially and temporally varying interactions among HI components and of uncertainties is therefore crucial for the success of water scarcity adaptation by HI.
- ItemSolid-state ensemble of highly entangled photon sources at rubidium atomic transitions(London : Nature Publishing Group, 2017) Keil, R.; Zopf, M.; Chen, Y.; Höfer, B.; Zhang, J.; Ding, F.; Schmidt, O.G.Semiconductor InAs/GaAs quantum dots grown by the Stranski-Krastanov method are among the leading candidates for the deterministic generation of polarization-entangled photon pairs. Despite remarkable progress in the past 20 years, many challenges still remain for this material, such as the extremely low yield, the low degree of entanglement and the large wavelength distribution. Here, we show that with an emerging family of GaAs/AlGaAs quantum dots grown by droplet etching and nanohole infilling, it is possible to obtain a large ensemble of polarization-entangled photon emitters on a wafer without any post-growth tuning. Under pulsed resonant two-photon excitation, all measured quantum dots emit single pairs of entangled photons with ultra-high purity, high degree of entanglement and ultra-narrow wavelength distribution at rubidium transitions. Therefore, this material system is an attractive candidate for the realization of a solid-state quantum repeater - among many other key enabling quantum photonic elements.
- ItemHybrid soliton dynamics in liquid-core fibres(Berlin : Nature Pulishing, 2017) Chemnitz, Mario; Gebhardt, Martin; Gaida, Christian; Stutzki, Fabian; Kobelke, Jens; Limpert, Jens; Tünnermann, Andreas; Schmidt, Markus A.The discovery of optical solitons being understood as temporally and spectrally stationary optical states has enabled numerous innovations among which, most notably, supercontinuum light sources have become widely used in both fundamental and applied sciences. Here, we report on experimental evidence for dynamics of hybrid solitons—a new type of solitary wave, which emerges as a result of a strong non-instantaneous nonlinear response in CS2-filled liquid-core optical fibres. Octave-spanning supercontinua in the mid-infrared region are observed when pumping the hybrid waveguide with a 460 fs laser (1.95 μm) in the anomalous dispersion regime at nanojoule-level pulse energies. A detailed numerical analysis well correlated with the experiment uncovers clear indicators of emerging hybrid solitons, revealing their impact on the bandwidth, onset energy and noise characteristics of the supercontinua. Our study highlights liquid-core fibres as a promising platform for fundamental optics and applications towards novel coherent and reconfigurable light sources.
- ItemUniversal emulsion stabilization from the arrested adsorption of rough particles at liquid-liquid interfaces([London] : Nature Publishing Group UK, 2017) Zanini, Michele; Marschelke, Claudia; Anachkov, Svetoslav E.; Marini, Emanuele; Synytska, Alla; Isa, LucioSurface heterogeneities, including roughness, significantly affect the adsorption, motion and interactions of particles at fluid interfaces. However, a systematic experimental study, linking surface roughness to particle wettability at a microscopic level, is currently missing. Here we synthesize a library of all-silica microparticles with uniform surface chemistry, but tuneable surface roughness and study their spontaneous adsorption at oil-water interfaces. We demonstrate that surface roughness strongly pins the particles' contact lines and arrests their adsorption in long-lived metastable positions, and we directly measure the roughness-induced interface deformations around isolated particles. Pinning imparts tremendous contact angle hysteresis, which can practically invert the particle wettability for sufficient roughness, irrespective of their chemical nature. As a unique consequence, the same rough particles stabilize both water-in-oil and oil-in-water emulsions depending on the phase they are initially dispersed in. These results both shed light on fundamental phenomena concerning particle adsorption at fluid interfaces and indicate future design rules for particle-based emulsifiers.
- ItemBio-degradable highly fluorescent conjugated polymer nanoparticles for bio-medical imaging applications([London] : Nature Publishing Group UK, 2017) Repenko, Tatjana; Rix, Anne; Ludwanowski, Simon; Go, Dennis; Kiessling, Fabian; Lederle, Wiltrud; Kuehne, Alexander J. C.Conjugated polymer nanoparticles exhibit strong fluorescence and have been applied for biological fluorescence imaging in cell culture and in small animals. However, conjugated polymer particles are hydrophobic and often chemically inert materials with diameters ranging from below 50 nm to several microns. As such, conjugated polymer nanoparticles cannot be excreted through the renal system. This drawback has prevented their application for clinical bio-medical imaging. Here, we present fully conjugated polymer nanoparticles based on imidazole units. These nanoparticles can be bio-degraded by activated macrophages. Reactive oxygen species induce scission of the conjugated polymer backbone at the imidazole unit, leading to complete decomposition of the particles into soluble low molecular weight fragments. Furthermore, the nanoparticles can be surface functionalized for directed targeting. The approach opens a wide range of opportunities for conjugated polymer particles in the fields of medical imaging, drug-delivery, and theranostics.
- ItemHighly indistinguishable and strongly entangled photons from symmetric GaAs quantum dots(London : Nature Publishing Group, 2017) Huber, D.; Reindl, M.; Huo, Y.; Huang, H.; Wildmann, J.S.; Schmidt, O.G.; Rastelli, A.; Trotta, R.The development of scalable sources of non-classical light is fundamental to unlocking the technological potential of quantum photonics. Semiconductor quantum dots are emerging as near-optimal sources of indistinguishable single photons. However, their performance as sources of entangled-photon pairs are still modest compared to parametric down converters. Photons emitted from conventional Stranski-Krastanov InGaAs quantum dots have shown non-optimal levels of entanglement and indistinguishability. For quantum networks, both criteria must be met simultaneously. Here, we show that this is possible with a system that has received limited attention so far: GaAs quantum dots. They can emit triggered polarization-entangled photons with high purity (g (2) (0) = 0.002±0.002), high indistinguishability (0.93±0.07 for 2 ns pulse separation) and high entanglement fidelity (0.94±0.01). Our results show that GaAs might be the material of choice for quantum-dot entanglement sources in future quantum technologies.
- ItemCubosomes from hierarchical self-assembly of poly(ionic liquid) block copolymers([London] : Nature Publishing Group UK, 2017) He, Hongkun; Rahimi, Khosrow; Zhong, Mingjiang; Mourran, Ahmed; Luebke, David R.; Nulwala, Hunaid B.; Möller, Martin; Matyjaszewski, KrzysztofCubosomes are micro- and nanoparticles with a bicontinuous cubic two-phase structure, reported for the self-assembly of low molecular weight surfactants, for example, lipids, but rarely formed by polymers. These objects are characterized by a maximum continuous interface and high interface to volume ratio, which makes them promising candidates for efficient adsorbents and host-guest applications. Here we demonstrate self-assembly to nanoscale cuboidal particles with a bicontinuous cubic structure by amphiphilic poly(ionic liquid) diblock copolymers, poly(acrylic acid)-block-poly(4-vinylbenzyl)-3-butyl imidazolium bis(trifluoromethylsulfonyl)imide, in a mixture of tetrahydrofuran and water under optimized conditions. Structure determining parameters include polymer composition and concentration, temperature, and the variation of the solvent mixture. The formation of the cubosomes can be explained by the hierarchical interactions of the constituent components. The lattice structure of the block copolymers can be transferred to the shape of the particle as it is common for atomic and molecular faceted crystals.