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    Nitrogen and boron doped carbon layer coated multiwall carbon nanotubes as high performance anode materials for lithium ion batteries
    ([London] : Nature Publishing Group, 2021) Liu, Bo; Sun, Xiaolei; Liao, Zhongquan; Lu, Xueyi; Zhang, Lin; Hao, Guang-Ping
    Lithium ion batteries (LIBs) are at present widely used as energy storage and conversion device in our daily life. However, due to the limited power density, the application of LIBs is still restricted in some areas such as commercial vehicles or heavy-duty trucks. An effective strategy to solve this problem is to increase energy density through the development of battery materials. At the same time, a stable long cycling battery is a great demand of environmental protection and industry. Herein we present our new materials, nitrogen and boron doped carbon layer coated multiwall carbon nanotubes (NBC@MWCNTs), which can be used as anodes for LIBs. The electrochemical results demonstrate that the designed NBC@MWCNTs electrode possesses high stable capacity over an ultra-long cycling lifespan (5000 cycles) and superior rate capability even at very high current density (67.5 A g−1). Such impressive lithium storage properties could be ascribed to the synergistic coupling effect of the distinctive structural features, the reduced diffusion length of lithium ions, more active sites generated by doped atoms for lithium storage, as well as the enhancement of the electrode structural integrity. Taken together, these results indicate that the N, B-doped carbon@MWCNTs materials may have great potential for applications in next-generation high performance rechargeable batteries.
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    In situ correlation between metastable phase-transformation mechanism and kinetics in a metallic glass
    ([London] : Nature Publishing Group, 2021) Orava, Jiri; Balachandran, Shanoob; Han, Xiaoliang; Shuleshova, Olga; Nurouzi, Ebrahim; Soldatov, Ivan; Oswald, Steffen; Gutowski, Olof; Ivashko, Oleh; Dippel, Ann-Christin; v. Zimmermann, Martin; Ivanov, Yurii P.; Greer, A. Lindsay; Raabe, Dierk; Herbig, Michael; Kaban, Ivan
    A combination of complementary high-energy X-ray diffraction, containerless solidification during electromagnetic levitation and transmission electron microscopy is used to map in situ the phase evolution in a prototype Cu-Zr-Al glass during flash-annealing imposed at a rate ranging from 102 to 103 K s−1 and during cooling from the liquid state. Such a combination of experimental techniques provides hitherto inaccessible insight into the phase-transformation mechanism and its kinetics with high temporal resolution over the entire temperature range of the existence of the supercooled liquid. On flash-annealing, most of the formed phases represent transient (metastable) states – they crystallographically conform to their equilibrium phases but the compositions, revealed by atom probe tomography, are different. It is only the B2 CuZr phase which is represented by its equilibrium composition, and its growth is facilitated by a kinetic mechanism of Al partitioning; Al-rich precipitates of less than 10 nm in a diameter are revealed. In this work, the kinetic and chemical conditions of the high propensity of the glass for the B2 phase formation are formulated, and the multi-technique approach can be applied to map phase transformations in other metallic-glass-forming systems.
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    Publisher Correction: Evolution of electronic and magnetic properties of Sr2IrO4 under strain
    ([London] : Nature Publishing Group, 2022) Pärschke, Ekaterina M.; Chen, Wei-Chih; Ray, Rajyavardhan; Chen, Cheng-Chien
    In the original version of this Article, all the figures (together with the captions) are inadvertently misplaced. Figures 1, 2, 3, 4, 5, 6 and 7 were wrongly placed in the positions of Figures 7, 1, 2, 3, 4, 5 and 6, respectively. This has been corrected in both the PDF and HTML versions of the Article.
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    Complete field-induced spectral response of the spin-1/2 triangular-lattice antiferromagnet CsYbSe2
    ([London] : Nature Publishing Group, 2023) Xie, Tao; Eberharter, A. A.; Xing, Jie; Nishimoto, S.; Brando, M.; Khanenko, P.; Sichelschmidt, J.; Turrini, A. A.; Mazzone, D. G.; Naumov, P. G.; Sanjeewa, L. D.; Harrison, N.; Sefat, Athena S.; Normand, B.; Läuchli, A. M.; Podlesnyak, A.; Nikitin, S. E.
    Fifty years after Anderson’s resonating valence-bond proposal, the spin-1/2 triangular-lattice Heisenberg antiferromagnet (TLHAF) remains the ultimate platform to explore highly entangled quantum spin states in proximity to magnetic order. Yb-based delafossites are ideal candidate TLHAF materials, which allow experimental access to the full range of applied in-plane magnetic fields. We perform a systematic neutron scattering study of CsYbSe2, first proving the Heisenberg character of the interactions and quantifying the second-neighbor coupling. We then measure the complex evolution of the excitation spectrum, finding extensive continuum features near the 120°-ordered state, throughout the 1/3-magnetization plateau and beyond this up to saturation. We perform cylinder matrix-product-state (MPS) calculations to obtain an unbiased numerical benchmark for the TLHAF and spectacular agreement with the experimental spectra. The measured and calculated longitudinal spectral functions reflect the role of multi-magnon bound and scattering states. These results provide valuable insight into unconventional field-induced spin excitations in frustrated quantum materials.
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    Unraveling the nature of spin excitations disentangled from charge contributions in a doped cuprate superconductor
    ([London] : Nature Publishing Group, 2022) Zhang, Wenliang; Agrapidis, Cliò Efthimia; Tseng, Yi; Asmara, Teguh Citra; Paris, Eugenio; Strocov, Vladimir N.; Giannini, Enrico; Nishimoto, Satoshi; Wohlfeld, Krzysztof; Schmitt, Thorsten
    The nature of the spin excitations in superconducting cuprates is a key question toward a unified understanding of the cuprate physics from long-range antiferromagnetism to superconductivity. The intense spin excitations up to the over-doped regime revealed by resonant inelastic X-ray scattering bring new insights as well as questions like how to understand their persistence or their relation to the collective excitations in ordered magnets (magnons). Here, we study the evolution of the spin excitations upon hole-doping the superconducting cuprate Bi2Sr2CaCu2O8+δ by disentangling the spin from the charge excitations in the experimental cross section. We compare our experimental results against density matrix renormalization group calculations for a t-J-like model on a square lattice. Our results unambiguously confirm the persistence of the spin excitations, which are closely connected to the persistence of short-range magnetic correlations up to high doping. This suggests that the spin excitations in hole-doped cuprates are related to magnons—albeit short-ranged.
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    Anomalous and anisotropic nonlinear susceptibility in the proximate Kitaev magnet α-RuCl3
    ([London] : Nature Publishing Group, 2021) Holleis, Ludwig; Prestigiacomo, Joseph C.; Fan, Zhijie; Nishimoto, Satoshi; Osofsky, Michael; Chern, Gia-Wei; van den Brink, Jeroen; Shivaram, B.S.
    The leading order nonlinear (NL) susceptibility, χ3, in a paramagnet is negative and diverges as T → 0. This divergence is destroyed when spins correlate and the NL response provides unique insights into magnetic order. Dimensionality, exchange interaction, and preponderance of quantum effects all imprint their signatures in the NL magnetic response. Here, we study the NL susceptibilities in the proximate Kitaev magnet α-RuCl3, which differs from the expected antiferromagnetic behavior. For T < Tc = 7.5 K and field B in the ab-plane, we obtain contrasting NL responses in low (<2 T) and high field regions. For low fields, the NL behavior is dominated by a quadratic response (positive χ2), which shows a rapid rise below Tc. This large χ2 > 0 implies a broken sublattice symmetry of magnetic order at low temperatures. Classical Monte Carlo (CMC) simulations in the standard K − H − Γ model secure such a quadratic B dependence of M, only for T ≈ Tc with χ2 being zero as T → 0. It is also zero for all temperatures in exact diagonalization calculations. On the other hand, we find an exclusive cubic term (χ3) that describes the high field NL behavior well. χ3 is large and positive both below and above Tc crossing zero only for T > 50 K. In contrast, for B ∥ c-axis, no separate low/high field behaviors are measured and only a much smaller χ3 is apparent.
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    Tunable chirality of noncentrosymmetric magnetic Weyl semimetals in rare-earth carbides
    ([London] : Nature Publishing Group, 2022) Ray, Rajyavardhan; Sadhukhan, Banasree; Richter, Manuel; Facio, Jorge I.; van den Brink, Jeroen
    Even if Weyl semimetals are characterized by quasiparticles with well-defined chirality, exploiting this experimentally is severely hampered by Weyl lattice fermions coming in pairs with opposite chirality, typically causing the net chirality picked up by experimental probes to vanish. Here, we show this issue can be circumvented in a controlled manner when both time-reversal- and inversion symmetry are broken. To this end, we investigate chirality disbalance in the carbide family RMC2 (R a rare-earth and M a transition metal), showing several members to be Weyl semimetals. Using the noncentrosymmetric ferromagnet NdRhC2 as an illustrating example, we show that an odd number of Weyl nodes can be stabilized at its Fermi surface by properly tilting its magnetization. The chiral configuration endows a topological phase transition as the Weyl node transitions across the Fermi sheets, which triggers interesting chiral electromagnetic responses. Further, the tilt direction determines the sign of the resulting net chirality, opening up a simple route to control its sign and strength.
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    Plethora of tunable Weyl fermions in kagome magnet Fe3Sn2 thin films
    ([London] : Nature Publishing Group, 2022) Ren, Zheng; Li, Hong; Sharma, Shrinkhala; Bhattarai, Dipak; Zhao, He; Rachmilowitz, Bryan; Bahrami, Faranak; Tafti, Fazel; Fang, Shiang; Ghimire, Madhav Prasad; Wang, Ziqiang; Zeljkovic, Ilija
    Interplay of magnetism and electronic band topology in unconventional magnets enables the creation and fine control of novel electronic phenomena. In this work, we use scanning tunneling microscopy and spectroscopy to study thin films of a prototypical kagome magnet Fe3Sn2. Our experiments reveal an unusually large number of densely-spaced spectroscopic features straddling the Fermi level. These are consistent with signatures of low-energy Weyl fermions and associated topological Fermi arc surface states predicted by theory. By measuring their response as a function of magnetic field, we discover a pronounced evolution in energy tied to the magnetization direction. Electron scattering and interference imaging further demonstrates the tunable nature of a subset of related electronic states. Our experiments provide a direct visualization of how in-situ spin reorientation drives changes in the electronic density of states of the Weyl fermion band structure. Combined with previous reports of massive Dirac fermions, flat bands, and electronic nematicity, our work establishes Fe3Sn2 as an interesting platform that harbors an extraordinarily wide array of topological and correlated electron phenomena.
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    Intertwined electronic and magnetic structure of the van-der-Waals antiferromagnet Fe2P2S6
    ([London] : Nature Publishing Group, 2023) Koitzsch, A.; Klaproth, T.; Selter, S.; Shemerliuk, Y.; Aswartham, S.; Janson, O.; Büchner, B.; Knupfer, M.
    Many unusual and promising properties have been reported recently for the transition metal trichalcogenides of the type MPS3 (M = V, Mn, Fe, Ni..), such as maintaining magnetic order to the atomically thin limit, ultra-sharp many-body excitons, metal-insulator transitions and, especially for Fe2P2S6, giant linear dichroism among others. Here we conduct a detailed investigation of the electronic structure of Fe2P2S6 using angle-resolved photoemission spectroscopy, q-dependent electron energy loss spectroscopy, optical spectroscopies and density functional theory. Fe2P2S6 is a Mott insulator with a gap of E gap ≈ 1.4 eV and zigzag antiferromagnetism below T N = 119 K. The low energy excitations are dominated by Fe 3d states. Large and sign-changing linear dichroism is observed. We provide a microscopic mechanism explaining key properties of the linear dichroism based on the correlated character of the electronic structure, thereby elucidating the nature of the spin-charge coupling in Fe2P2S6 and related materials.
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    High-energy magnetic excitations from heavy quasiparticles in CeCu2Si2
    ([London] : Nature Publishing Group, 2021) Song, Yu; Wang, Weiyi; Cao, Chongde; Yamani, Zahra; Xu, Yuanji; Sheng, Yutao; Löser, Wolfgang; Qiu, Yiming; Yang, Yi-feng; Birgeneau, Robert J.; Dai, Pengcheng
    Magnetic fluctuations is the leading candidate for pairing in cuprate, iron-based, and heavy fermion superconductors. This view is challenged by the recent discovery of nodeless superconductivity in CeCu2Si2, and calls for a detailed understanding of the corresponding magnetic fluctuations. Here, we mapped out the magnetic excitations in superconducting (S-type) CeCu2Si2 using inelastic neutron scattering, finding a strongly asymmetric dispersion for E ≲ 1.5 meV, which at higher energies evolves into broad columnar magnetic excitations that extend to E ≳ 5 meV. While low-energy magnetic excitations exhibit marked three-dimensional characteristics, the high-energy magnetic excitations in CeCu2Si2 are almost two-dimensional, reminiscent of paramagnons found in cuprate and iron-based superconductors. By comparing our experimental findings with calculations in the random-phase approximation,we find that the magnetic excitations in CeCu2Si2 arise from quasiparticles associated with its heavy electron band, which are also responsible for superconductivity. Our results provide a basis for understanding magnetism and superconductivity in CeCu2Si2, and demonstrate the utility of neutron scattering in probing band renormalization in heavy fermion metals.