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Type: article × search.filters.applied.f.series: Nature Communications 11 (2020) ×

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    Integrated molecular diode as 10 MHz half-wave rectifier based on an organic nanostructure heterojunction
    ([London] : Nature Publishing Group UK, 2020) Li, Tianming; Bandari, Vineeth Kumar; Hantusch, Martin; Xin, Jianhui; Kuhrt, Robert; Ravishankar, Rachappa; Xu, Longqian; Zhang, Jidong; Knupfer, Martin; Zhu, Feng; Yan, Donghang; Schmidt, Oliver G.
    Considerable efforts have been made to realize nanoscale diodes based on single molecules or molecular ensembles for implementing the concept of molecular electronics. However, so far, functional molecular diodes have only been demonstrated in the very low alternating current frequency regime, which is partially due to their extremely low conductance and the poor degree of device integration. Here, we report about fully integrated rectifiers with microtubular soft-contacts, which are based on a molecularly thin organic heterojunction and are able to convert alternating current with a frequency of up to 10 MHz. The unidirectional current behavior of our devices originates mainly from the intrinsically different surfaces of the bottom planar and top microtubular Au electrodes while the excellent high frequency response benefits from the charge accumulation in the phthalocyanine molecular heterojunction, which not only improves the charge injection but also increases the carrier density.
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    Probing multiphoton light-induced molecular potentials
    ([London] : Nature Publishing Group UK, 2020) Kübel, M.; Spanner, M.; Dube, Z.; Naumov, A.Yu.; Chelkowski, S.; Bandrauk, A.D.; Vrakking, M.J.J.; Corkum, P.B.; Villeneuve, D.M.; Staudte, A.
    The strong coupling between intense laser fields and valence electrons in molecules causes distortions of the potential energy hypersurfaces which determine the motion of the nuclei and influence possible reaction pathways. The coupling strength varies with the angle between the light electric field and valence orbital, and thereby adds another dimension to the effective molecular potential energy surface, leading to the emergence of light-induced conical intersections. Here, we demonstrate that multiphoton couplings can give rise to complex light-induced potential energy surfaces that govern molecular behavior. In the laser-induced dissociation of H2+, the simplest of molecules, we measure a strongly modulated angular distribution of protons which has escaped prior observation. Using two-color Floquet theory, we show that the modulations result from ultrafast dynamics on light-induced molecular potentials. These potentials are shaped by the amplitude, duration and phase of the dressing fields, allowing for manipulating the dissociation dynamics of small molecules.
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    Collapse of layer dimerization in the photo-induced hidden state of 1T-TaS2
    ([London] : Nature Publishing Group UK, 2020) Stahl, Quirin; Kusch, Maximilian; Heinsch, Florian; Garbarino, Gaston; Kretzschmar, Norman; Hanff, Kerstin; Rossnagel, Kai; Geck, Jochen; Ritschel, Tobias
    Photo-induced switching between collective quantum states of matter is a fascinating rising field with exciting opportunities for novel technologies. Presently, very intensively studied examples in this regard are nanometer-thick single crystals of the layered material 1T-TaS2, where picosecond laser pulses can trigger a fully reversible insulator-to-metal transition (IMT). This IMT is believed to be connected to the switching between metastable collective quantum states, but the microscopic nature of this so-called hidden quantum state remained largely elusive up to now. Here, we characterize the hidden quantum state of 1T-TaS2 by means of state-of-the-art x-ray diffraction and show that the laser-driven IMT involves a marked rearrangement of the charge and orbital order in the direction perpendicular to the TaS2-layers. More specifically, we identify the collapse of interlayer molecular orbital dimers as a key mechanism for this non-thermal collective transition between two truly long-range ordered electronic crystals.
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    Hysteresis of tropical forests in the 21st century
    ([London] : Nature Publishing Group UK, 2020) Staal, Arie; Fetzer, Ingo; Wang-Erlandsson, Lan; Bosmans, Joyce H. C.; Dekker, Stefan C.; van Nes, Egbert H.; Rockström, Johan; Tuinenburg, Obbe A.
    Tropical forests modify the conditions they depend on through feedbacks at different spatial scales. These feedbacks shape the hysteresis (history-dependence) of tropical forests, thus controlling their resilience to deforestation and response to climate change. Here, we determine the emergent hysteresis from local-scale tipping points and regional-scale forest-rainfall feedbacks across the tropics under the recent climate and a severe climate-change scenario. By integrating remote sensing, a global hydrological model, and detailed atmospheric moisture tracking simulations, we find that forest-rainfall feedback expands the geographic range of possible forest distributions, especially in the Amazon. The Amazon forest could partially recover from complete deforestation, but may lose that resilience later this century. The Congo forest currently lacks resilience, but is predicted to gain it under climate change, whereas forests in Australasia are resilient under both current and future climates. Our results show how tropical forests shape their own distributions and create the climatic conditions that enable them.
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    Gate controlled valley polarizer in bilayer graphene
    ([London] : Nature Publishing Group UK, 2020) Chen, Hao; Zhou, Pinjia; Liu, Jiawei; Qiao, Jiabin; Oezyilmaz, Barbaros; Martin, Jens
    Sign reversal of Berry curvature across two oppositely gated regions in bilayer graphene can give rise to counter-propagating 1D channels with opposite valley indices. Considering spin and sub-lattice degeneracy, there are four quantized conduction channels in each direction. Previous experimental work on gate-controlled valley polarizer achieved good contrast only in the presence of an external magnetic field. Yet, with increasing magnetic field the ungated regions of bilayer graphene will transit into the quantum Hall regime, limiting the applications of valley-polarized electrons. Here we present improved performance of a gate-controlled valley polarizer through optimized device geometry and stacking method. Electrical measurements show up to two orders of magnitude difference in conductance between the valley-polarized state and gapped states. The valley-polarized state displays conductance of nearly 4e2/h and produces contrast in a subsequent valley analyzer configuration. These results pave the way to further experiments on valley-polarized electrons in zero magnetic field.
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    Engineering grain boundaries at the 2D limit for the hydrogen evolution reaction
    ([London] : Nature Publishing Group UK, 2020) He, Yongmin; Tang, Pengyi; Hu, Zhili; He, Qiyuan; Zhu, Chao; Wang, Luqing; Zeng, Qingsheng; Golani, Prafful; Gao, Guanhui; Fu, Wei; Huang, Zhiqi; Gao, Caitian; Xia, Juan; Wang, Xingli; Wang, Xuewen; Zhu, Chao; Ramasse, Quentin M.; Zhang, Ao; An, Boxing; Zhang, Yongzhe; Martí-Sánchez, Sara; Morante, Joan Ramon; Wang, Liang; Tay, Beng Kang; Yakobson, Boris I.; Trampert, Achim; Zhang, Hua; Wu, Minghong; Wang, Qi Jie; Arbiol, Jordi; Liu, Zheng
    Atom-thin transition metal dichalcogenides (TMDs) have emerged as fascinating materials and key structures for electrocatalysis. So far, their edges, dopant heteroatoms and defects have been intensively explored as active sites for the hydrogen evolution reaction (HER) to split water. However, grain boundaries (GBs), a key type of defects in TMDs, have been overlooked due to their low density and large structural variations. Here, we demonstrate the synthesis of wafer-size atom-thin TMD films with an ultra-high-density of GBs, up to ~1012 cm−2. We propose a climb and drive 0D/2D interaction to explain the underlying growth mechanism. The electrocatalytic activity of the nanograin film is comprehensively examined by micro-electrochemical measurements, showing an excellent hydrogen-evolution performance (onset potential: −25 mV and Tafel slope: 54 mV dec−1), thus indicating an intrinsically high activation of the TMD GBs.
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    On the influence of density and morphology on the Urban Heat Island intensity
    ([London] : Nature Publishing Group UK, 2020) Li, Yunfei; Schubert, Sebastian; Kropp, Jürgen P.; Rybski, Diego
    The canopy layer urban heat island (UHI) effect, as manifested by elevated near-surface air temperatures in urban areas, exposes urban dwellers to additional heat stress in many cities, specially during heat waves. We simulate the urban climate of various generated cities under the same weather conditions. For mono-centric cities, we propose a linear combination of logarithmic city area and logarithmic gross building volume, which also captures the influence of building density. By studying various city shapes, we generalise and propose a reduced form to estimate UHI intensities based only on the structure of urban sites, as well as their relative distances. We conclude that in addition to the size, the UHI intensity of a city is directly related to the density and an amplifying effect that urban sites have on each other. Our approach can serve as a UHI rule of thumb for the comparison of urban development scenarios.
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    The role of allyl ammonium salts in palladium-catalyzed cascade reactions towards the synthesis of spiro-fused heterocycles
    ([London] : Nature Publishing Group UK, 2020) Ye, Fei; Ge, Yao; Spannenberg, Anke; Neumann, Helfried; Beller, Matthias
    There is a continuous need for designing new and improved synthetic methods aiming at minimizing reaction steps while increasing molecular complexity. In this respect, catalytic, one-pot cascade methodologies constitute an ideal tool for the construction of complex molecules with high chemo-, regio-, and stereoselectivity. Herein, we describe two general and efficient cascade procedures for the synthesis of spiro-fused heterocylces. This transformation combines selective nucleophilic substitution (SN2′), palladium-catalyzed Heck and C–H activation reactions in a cascade manner. The use of allylic ammonium salts and specific Pd catalysts are key to the success of the transformations. The synthetic utility of these methodologies is showcased by the preparation of 48 spiro-fused dihydrobenzofuranes and indolines including a variety of fluorinated derivatives.
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    Taking stock of national climate policies to evaluate implementation of the Paris Agreement
    ([London] : Nature Publishing Group UK, 2020) Roelfsema, Mark; van Soest, Heleen L.; Harmsen, Mathijs; van Vuuren, Detlef P.; Bertram, Christoph; den Elzen, Michel; Höhne, Niklas; Iacobuta, Gabriela; Krey, Volker; Kriegler, Elmar; Luderer, Gunnar; Riahi, Keywan; Ueckerdt, Falko; Després, Jacques; Drouet, Laurent; Emmerling, Johannes; Frank, Stefan; Fricko, Oliver; Gidden, Matthew; Humpenöder, Florian; Huppmann, Daniel; Fujimori, Shinichiro; Fragkiadakis, Kostas; Gi, Keii; Keramidas, Kimon; Köberle, Alexandre C.; Aleluia Reis, Lara; Rochedo, Pedro; Schaeffer, Roberto; Oshiro, Ken; Vrontisi, Zoi; Chen, Wenying; Iyer, Gokul C.; Edmonds, Jae; Kannavou, Maria; Jiang, Kejun; Mathur, Ritu; Safonov, George; Vishwanathan, Saritha Sudharmma
    Many countries have implemented national climate policies to accomplish pledged Nationally Determined Contributions and to contribute to the temperature objectives of the Paris Agreement on climate change. In 2023, the global stocktake will assess the combined effort of countries. Here, based on a public policy database and a multi-model scenario analysis, we show that implementation of current policies leaves a median emission gap of 22.4 to 28.2 GtCO2eq by 2030 with the optimal pathways to implement the well below 2 °C and 1.5 °C Paris goals. If Nationally Determined Contributions would be fully implemented, this gap would be reduced by a third. Interestingly, the countries evaluated were found to not achieve their pledged contributions with implemented policies (implementation gap), or to have an ambition gap with optimal pathways towards well below 2 °C. This shows that all countries would need to accelerate the implementation of policies for renewable technologies, while efficiency improvements are especially important in emerging countries and fossil-fuel-dependent countries.
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    How to speed up ion transport in nanopores
    ([London] : Nature Publishing Group UK, 2020) Breitsprecher, Konrad; Janssen, Mathijs; Srimuk, Pattarachai; Mehdi, B. Layla; Presser, Volker; Holm, Christian; Kondrat, Svyatoslav
    Electrolyte-filled subnanometre pores exhibit exciting physics and play an increasingly important role in science and technology. In supercapacitors, for instance, ultranarrow pores provide excellent capacitive characteristics. However, ions experience difficulties in entering and leaving such pores, which slows down charging and discharging processes. In an earlier work we showed for a simple model that a slow voltage sweep charges ultranarrow pores quicker than an abrupt voltage step. A slowly applied voltage avoids ionic clogging and co-ion trapping—a problem known to occur when the applied potential is varied too quickly—causing sluggish dynamics. Herein, we verify this finding experimentally. Guided by theoretical considerations, we also develop a non-linear voltage sweep and demonstrate, with molecular dynamics simulations, that it can charge a nanopore even faster than the corresponding optimized linear sweep. For discharging we find, with simulations and in experiments, that if we reverse the applied potential and then sweep it to zero, the pores lose their charge much quicker than they do for a short-circuited discharge over their internal resistance. Our findings open up opportunities to greatly accelerate charging and discharging of subnanometre pores without compromising the capacitive characteristics, improving their importance for energy storage, capacitive deionization, and electrochemical heat harvesting.