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Now showing 1 - 10 of 28
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    High-Quality Graphene Using Boudouard Reaction
    (Weinheim : Wiley-VCH, 2022) Grebenko, Artem K.; Krasnikov, Dmitry V.; Bubis, Anton V.; Stolyarov, Vasily S.; Vyalikh, Denis V.; Makarova, Anna A.; Fedorov, Alexander; Aitkulova, Aisuluu; Alekseeva, Alena A.; Gilshtein, Evgeniia; Bedran, Zakhar; Shmakov, Alexander N.; Alyabyeva, Liudmila; Mozhchil, Rais N.; Ionov, Andrey M.; Gorshunov, Boris P.; Laasonen, Kari; Podzorov, Vitaly; Nasibulin, Albert G.
    Following the game-changing high-pressure CO (HiPco) process that established the first facile route toward large-scale production of single-walled carbon nanotubes, CO synthesis of cm-sized graphene crystals of ultra-high purity grown during tens of minutes is proposed. The Boudouard reaction serves for the first time to produce individual monolayer structures on the surface of a metal catalyst, thereby providing a chemical vapor deposition technique free from molecular and atomic hydrogen as well as vacuum conditions. This approach facilitates inhibition of the graphene nucleation from the CO/CO2 mixture and maintains a high growth rate of graphene seeds reaching large-scale monocrystals. Unique features of the Boudouard reaction coupled with CO-driven catalyst engineering ensure not only suppression of the second layer growth but also provide a simple and reliable technique for surface cleaning. Aside from being a novel carbon source, carbon monoxide ensures peculiar modification of catalyst and in general opens avenues for breakthrough graphene-catalyst composite production.
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    Charge‐Compensated N‐Doped π ‐Conjugated Polymers: Toward both Thermodynamic Stability of N‐Doped States in Water and High Electron Conductivity
    (Weinheim : Wiley-VCH, 2022) Borrmann, Fabian; Tsuda, Takuya; Guskova, Olga; Kiriy, Nataliya; Hoffmann, Cedric; Neusser, David; Ludwigs, Sabine; Lappan, Uwe; Simon, Frank; Geisler, Martin; Debnath, Bipasha; Krupskaya, Yulia; Al‐Hussein, Mahmoud; Kiriy, Anton
    The understanding and applications of electron-conducting π-conjugated polymers with naphtalene diimide (NDI) blocks show remarkable progress in recent years. Such polymers demonstrate a facilitated n-doping due to the strong electron deficiency of the main polymer chain and the presence of the positively charged side groups stabilizing a negative charge of the n-doped backbone. Here, the n-type conducting NDI polymer with enhanced stability of its n-doped states for prospective “in-water” applications is developed. A combined experimental–theoretical approach is used to identify critical features and parameters that control the doping and electron transport process. The facilitated polymer reduction ability and the thermodynamic stability in water are confirmed by electrochemical measurements and doping studies. This material also demonstrates a high conductivity of 10−2 S cm−1 under ambient conditions and 10−1 S cm−1 in vacuum. The modeling explains the stabilizing effects for various dopants. The simulations show a significant doping-induced “collapse” of the positively charged side chains on the core bearing a partial negative charge. This explains a decrease in the lamellar spacing observed in experiments. This study fundamentally enables a novel pathway for achieving both thermodynamic stability of the n-doped states in water and the high electron conductivity of polymers.
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    Intermixing-Driven Surface and Bulk Ferromagnetism in the Quantum Anomalous Hall Candidate MnBi6Te10
    (Weinheim : Wiley-VCH, 2023) Tcakaev, Abdul‐Vakhab; Rubrecht, Bastian; Facio, Jorge I.; Zabolotnyy, Volodymyr B.; Corredor, Laura T.; Folkers, Laura C.; Kochetkova, Ekaterina; Peixoto, Thiago R. F.; Kagerer, Philipp; Heinze, Simon; Bentmann, Hendrik; Green, Robert J.; Gargiani, Pierluigi; Valvidares, Manuel; Weschke, Eugen; Haverkort, Maurits W.; Reinert, Friedrich; van den Brink, Jeroen; Büchner, Bernd; Wolter, Anja U. B.; Isaeva, Anna; Hinkov, Vladimir
    The recent realizations of the quantum anomalous Hall effect (QAHE) in MnBi2Te4 and MnBi4Te7 benchmark the (MnBi2Te4)(Bi2Te3)n family as a promising hotbed for further QAHE improvements. The family owes its potential to its ferromagnetically (FM) ordered MnBi2Te4 septuple layers (SLs). However, the QAHE realization is complicated in MnBi2Te4 and MnBi4Te7 due to the substantial antiferromagnetic (AFM) coupling between the SLs. An FM state, advantageous for the QAHE, can be stabilized by interlacing the SLs with an increasing number n of Bi2Te3 quintuple layers (QLs). However, the mechanisms driving the FM state and the number of necessary QLs are not understood, and the surface magnetism remains obscure. Here, robust FM properties in MnBi6Te10 (n = 2) with Tc ≈ 12 K are demonstrated and their origin is established in the Mn/Bi intermixing phenomenon by a combined experimental and theoretical study. The measurements reveal a magnetically intact surface with a large magnetic moment, and with FM properties similar to the bulk. This investigation thus consolidates the MnBi6Te10 system as perspective for the QAHE at elevated temperatures.
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    Tailoring Intermolecular Interactions Towards High‐Performance Thermoelectric Ionogels at Low Humidity
    (Weinheim : Wiley-VCH, 2022) Zhao, Wei; Sun, Tingting; Zheng, Yiwei; Zhang, Qihao; Huang, Aibin; Wang, Lianjun; Jiang, Wan
    Development of ionic thermoelectric (iTE) materials is of immense interest for efficient heat-to-electricity conversion due to their giant ionic Seebeck coefficient (Si), but challenges remain in terms of relatively small Si at low humidity, poor stretchability, and ambiguous interaction mechanism in ionogels. Herein, a novel ionogel is reported consisting of polyethylene oxide (PEO), polyethylene oxide-polypropylene oxide-polyethylene oxide (P123), and 1-ethyl-3-methylimidazolium acetate (Emim:OAC). By delicately designing the interactions between ions and polymers, the migration of anions is restricted due to their strong binding with the hydroxyl groups of polymers, while the transport of cations is facilitated through segmental motions due to the increased amorphous regions, thereby leading to enlarged diffusion difference between the cations and anions. Moreover, the plasticizing effect of P123 and Emim:OAC can increase the elongation at break. As a consequence, the ionogel exhibits excellent properties including high Si (18 mV K−1 at relative humidity of 60%), good ionic conductivity (1.1 mS cm−1), superior stretchability (787%), and high stability (over 80% retention after 600 h). These findings show a promising strategy to obtain multifunctional iTE materials by engineering the intermolecular interactions and demonstrate the great potential of ionogels for harvesting low-grade heat in human-comfortable humidity environments.
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    Beyond Janus Geometry: Characterization of Flow Fields around Nonspherical Photocatalytic Microswimmers
    (Weinheim : Wiley-VCH, 2022) Heckel, Sandra; Bilsing, Clemens; Wittmann, Martin; Gemming, Thomas; Büttner, Lars; Czarske, Jürgen; Simmchen, Juliane
    Catalytic microswimmers that move by a phoretic mechanism in response to a self-induced chemical gradient are often obtained by the design of spherical janus microparticles, which suffer from multi-step fabrication and low yields. Approaches that circumvent laborious multi-step fabrication include the exploitation of the possibility of nonuniform catalytic activity along the surface of irregular particle shapes, local excitation or intrinsic asymmetry. Unfortunately, the effects on the generation of motion remain poorly understood. In this work, single crystalline BiVO4 microswimmers are presented that rely on a strict inherent asymmetry of charge-carrier distribution under illumination. The origin of the asymmetrical flow pattern is elucidated because of the high spatial resolution of measured flow fields around pinned BiVO4 colloids. As a result the flow from oxidative to reductive particle sides is confirmed. Distribution of oxidation and reduction reactions suggests a dominant self-electrophoretic motion mechanism with a source quadrupole as the origin of the induced flows. It is shown that the symmetry of the flow fields is broken by self-shadowing of the particles and synthetic surface defects that impact the photocatalytic activity of the microswimmers. The results demonstrate the complexity of symmetry breaking in nonspherical microswimmers and emphasize the role of self-shadowing for photocatalytic microswimmers. The findings are leading the way toward understanding of propulsion mechanisms of phoretic colloids of various shapes.
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    Flexomagnetism and vertically graded Néel temperature of antiferromagnetic Cr2O3 thin films
    ([London] : Nature Publishing Group UK, 2022) Makushko, Pavlo; Kosub, Tobias; Pylypovskyi, Oleksandr V.; Hedrich, Natascha; Li, Jiang; Pashkin, Alexej; Avdoshenko, Stanislav; Hübner, René; Ganss, Fabian; Wolf, Daniel; Lubk, Axel; Liedke, Maciej Oskar; Butterling, Maik; Wagner, Andreas; Wagner, Kai; Shields, Brendan J.; Lehmann, Paul; Veremchuk, Igor; Fassbender, Jürgen; Maletinsky, Patrick; Makarov, Denys
    Antiferromagnetic insulators are a prospective materials platform for magnonics, spin superfluidity, THz spintronics, and non-volatile data storage. A magnetomechanical coupling in antiferromagnets offers vast advantages in the control and manipulation of the primary order parameter yet remains largely unexplored. Here, we discover a new member in the family of flexoeffects in thin films of Cr2O3. We demonstrate that a gradient of mechanical strain can impact the magnetic phase transition resulting in the distribution of the Néel temperature along the thickness of a 50-nm-thick film. The inhomogeneous reduction of the antiferromagnetic order parameter induces a flexomagnetic coefficient of about 15 μB nm−2. The antiferromagnetic ordering in the inhomogeneously strained films can persist up to 100 °C, rendering Cr2O3 relevant for industrial electronics applications. Strain gradient in Cr2O3 thin films enables fundamental research on magnetomechanics and thermodynamics of antiferromagnetic solitons, spin waves and artificial spin ice systems in magnetic materials with continuously graded parameters.
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    Tailoring electron beams with high-frequency self-assembled magnetic charged particle micro optics
    ([London] : Nature Publishing Group UK, 2022) Huber, R.; Kern, F.; Karnaushenko, D.D.; Eisner, E.; Lepucki, P.; Thampi, A.; Mirhajivarzaneh, A.; Becker, C.; Kang, T.; Baunack, S.; Büchner, B.; Karnaushenko, D.; Schmidt, O.G.; Lubk, A.
    Tunable electromagnets and corresponding devices, such as magnetic lenses or stigmators, are the backbone of high-energy charged particle optical instruments, such as electron microscopes, because they provide higher optical power, stability, and lower aberrations compared to their electric counterparts. However, electromagnets are typically macroscopic (super-)conducting coils, which cannot generate swiftly changing magnetic fields, require active cooling, and are structurally bulky, making them unsuitable for fast beam manipulation, multibeam instruments, and miniaturized applications. Here, we present an on-chip microsized magnetic charged particle optics realized via a self-assembling micro-origami process. These micro-electromagnets can generate alternating magnetic fields of about ±100 mT up to a hundred MHz, supplying sufficiently large optical power for a large number of charged particle optics applications. That particular includes fast spatiotemporal electron beam modulation such as electron beam deflection, focusing, and wave front shaping as required for stroboscopic imaging.
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    A new dimension for magnetosensitive e-skins: active matrix integrated micro-origami sensor arrays
    ([London] : Nature Publishing Group UK, 2022) Becker, Christian; Bao, Bin; Karnaushenko, Dmitriy D.; Bandari, Vineeth Kumar; Rivkin, Boris; Li, Zhe; Faghih, Maryam; Karnaushenko, Daniil; Schmidt, Oliver G.
    Magnetic sensors are widely used in our daily life for assessing the position and orientation of objects. Recently, the magnetic sensing modality has been introduced to electronic skins (e-skins), enabling remote perception of moving objects. However, the integration density of magnetic sensors is limited and the vector properties of the magnetic field cannot be fully explored since the sensors can only perceive field components in one or two dimensions. Here, we report an approach to fabricate high-density integrated active matrix magnetic sensor with three-dimensional (3D) magnetic vector field sensing capability. The 3D magnetic sensor is composed of an array of self-assembled micro-origami cubic architectures with biased anisotropic magnetoresistance (AMR) sensors manufactured in a wafer-scale process. Integrating the 3D magnetic sensors into an e-skin with embedded magnetic hairs enables real-time multidirectional tactile perception. We demonstrate a versatile approach for the fabrication of active matrix integrated 3D sensor arrays using micro-origami and pave the way for new electronic devices relying on the autonomous rearrangement of functional elements in space.
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    Dimensional reduction and incommensurate dynamic correlations in the S=1/2 triangular-lattice antiferromagnet Ca3ReO5Cl2
    ([London] : Nature Publishing Group UK, 2022) Zvyagin, S.A.; Ponomaryov, A.N.; Wosnitza, J.; Hirai, D.; Hiroi, Z.; Gen, M.; Kohama, Y.; Matsuo, A.; Matsuda, Y.H.; Kindo, K.
    The observation of spinon excitations in the S=1/2 triangular antiferromagnet Ca3ReO5Cl2 reveals a quasi-one-dimensional (1D) nature of magnetic correlations, in spite of the nominally 2D magnetic structure. This phenomenon is known as frustration-induced dimensional reduction. Here, we present high-field electron spin resonance spectroscopy and magnetization studies of Ca3ReO5Cl2, allowing us not only to refine spin-Hamiltonian parameters, but also to investigate peculiarities of its low-energy spin dynamics. We argue that the presence of the uniform Dzyaloshinskii-Moriya interaction (DMI) shifts the spinon continuum in momentum space and, as a result, opens a zero-field gap at the Γ point. We observed this gap directly. The shift is found to be consistent with the structural modulation in the ordered state, suggesting this material as a perfect model triangular-lattice system, where a pure DMI-spiral ground state can be realized.
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    Giant stress response of terahertz magnons in a spin-orbit Mott insulator
    ([London] : Nature Publishing Group UK, 2022) Kim, Hun-Ho; Ueda, Kentaro; Nakata, Suguru; Wochner, Peter; Mackenzie, Andrew; Hicks, Clifford; Khaliullin, Giniyat; Liu, Huimei; Keimer, Bernhard; Minola, Matteo
    Magnonic devices operating at terahertz frequencies offer intriguing prospects for high-speed electronics with minimal energy dissipation However, guiding and manipulating terahertz magnons via external parameters present formidable challenges. Here we report the results of magnetic Raman scattering experiments on the antiferromagnetic spin-orbit Mott insulator Sr2IrO4 under uniaxial stress. We find that the energies of zone-center magnons are extremely stress sensitive: lattice strain of 0.1% increases the magnon energy by 40%. The magnon response is symmetric with respect to the sign of the applied stress (tensile or compressive), but depends strongly on its direction in the IrO2 planes. A theory based on coupling of the spin-orbit-entangled iridium magnetic moments to lattice distortions provides a quantitative explanation of the Raman data and a comprehensive framework for the description of magnon-lattice interactions in magnets with strong spin-orbit coupling. The possibility to efficiently manipulate the propagation of terahertz magnons via external stress opens up multifold design options for reconfigurable magnonic devices.