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  1. Abstract

    This study presents a new material, “HxCrS2” (denotes approximate composition) formed by proton‐exchange of NaCrS2which has a measured capacity of 728 mAh g−1with significant improvements to capacity retention, sustaining over 700 mAh g−1during cycling experiments. This is the highest reported capacity for a transition metal sulfide electrode and outperforms the most promising proposed sodium anodes to date. HxCrS2exhibits a biphasic structure featuring alternating crystalline and amorphous lamella on the scale of a few nanometers. This unique structural motif enables reversible access to Cr redox in the material resulting in higher capacities than seen in the parent structure which features only S redox. Pretreatment by proton‐exchange offers a route to materials such as HxCrS2which provide fast diffusion and high capacities for sodium‐ion batteries.

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  2. Abstract

    Three-dimensional dynamics of flexible fibers in shear flow are studied numerically, with a qualitative comparison to experiments. Initially, the fibers are straight, with different orientations with respect to the flow. By changing the rotation speed of a shear rheometer, we change the ratioAof bending to shear forces. We observe fibers in the flow-vorticity plane, which gives insight into the motion out of the shear plane. The numerical simulations of moderately flexible fibers show that they rotate along effective Jeffery orbits, and therefore the fiber orientation rapidly becomes very close to the flow-vorticity plane, on average close to the flow direction, and the fiber remains in an almost straight configuration for a long time. This ‘ordering’ of fibers is temporary since they alternately bend and straighten while tumbling. We observe numerically and experimentally that if the fibers are initially in the compressional region of the shear flow, they can undergo compressional buckling, with a pronounced deformation of shape along their whole length during a short time, which is in contrast to the typical local bending that originates over a long time from the fiber ends. We identify differences between local and compressional bending and discuss their competition, which depends on the initial orientation of the fiber and the bending stiffness ratioA. There are two main finding. First, the compressional buckling is limited to a certain small range of the initial orientations, excluding those from the flow-vorticity plane. Second, since fibers straighten in the flow-vorticity plane while tumbling, the compressional buckling is transient—it does not appear for times longer than 1/4 of the Jeffery period. For larger times, bending of fibers is always driven by their ends.

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  3. Abstract

    Van der Waals (vdW) materials are an indispensable part of functional device technology due to their versatile physical properties and ease of exfoliating to the low‐dimensional limit. Among all the compounds investigated so far, the search for magnetic vdW materials has intensified in recent years, fueled by the realization of magnetism in 2D. However, metallic magnetic vdW systems are still uncommon. In addition, they rarely host high‐mobility charge carriers, which is an essential requirement for high‐speed electronic applications. Another shortcoming of 2D magnets is that they are highly air sensitive. Using chemical reasoning, TaCo2Te2is introduced as an air‐stable, high‐mobility, magnetic vdW material. It has a layered structure, which consists of Peierls distorted Co chains and a large vdW gap between the layers. It is found that the bulk crystals can be easily exfoliated and the obtained thin flakes are robust to ambient conditions after 4 months of monitoring using an optical microscope. Signatures of canted antiferromagntic behavior are also observed at low‐temperature. TaCo2Te2shows a metallic character and a large, nonsaturating, anisotropic magnetoresistance. Furthermore, the Hall data and quantum oscillation measurements reveal the presence of both electron‐ and hole‐type carriers and their high mobility.

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  4. Abstract

    While several magnetic topological semimetals have been discovered in recent years, their band structures are far from ideal, often obscured by trivial bands at the Fermi energy. Square‐net materials with clean, linearly dispersing bands show potential to circumvent this issue. CeSbTe, a square‐net material, features multiple magnetic‐field‐controllable topological phases. Here, it is shown that in this material, even higher degrees of tunability can be achieved by changing the electron count at the square‐net motif. Increased electron filling results in structural distortion and formation of charge density waves (CDWs). The modulation wave‐vector evolves continuously leading to a region of multiple discrete CDWs and a corresponding complex “Devil's staircase” magnetic ground state. A series of fractionally quantized magnetization plateaus is observed, which implies direct coupling between CDW and a collective spin‐excitation. It is further shown that the CDW creates a robust idealized nonsymmorphic Dirac semimetal, thus providing access to topological systems with rich magnetism.

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  5. Abstract

    Moiré superlattices created by the twisted stacking of two-dimensional crystals can host electronic bands with flat energy dispersion in which enhanced interactions promote correlated electron states. The twisted double bilayer graphene (TDBG), where two Bernal bilayer graphene are stacked with a twist angle, is such a moiré system with tunable flat bands. Here, we use gate-tuned scanning tunneling spectroscopy to directly demonstrate the tunability of the band structure of TDBG with an electric field and to show spectroscopic signatures of electronic correlations and topology for its flat band. Our spectroscopic experiments are in agreement with a continuum model of TDBG band structure and reveal signatures of a correlated insulator gap at partial filling of its isolated flat band. The topological properties of this flat band are probed with the application of a magnetic field, which leads to valley polarization and the splitting of Chern bands with a large effective g-factor.

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  6. Abstract

    While metal‐halide perovskite light‐emitting diodes (PeLEDs) hold the potential for a new generation of display and lighting technology, their slow operation speed and response time limit their application scope. Here, high‐speed PeLEDs driven by nanosecond electrical pulses with a rise time of 1.2 ns are reported with a maximum radiance of approximately 480 kW sr−1 m−2at 8.3 kA cm−2, and an external quantum efficiency (EQE) of 1% at approximately 10 kA cm−2, through improved device configuration designs and material considerations. Enabled by the fast operation of PeLEDs, the temporal response provides access to transient charge carrier dynamics under electrical excitation, revealing several new electroluminescence quenching pathways. Finally, integrated distributed feedback (DFB) gratings are explored, which facilitate more directional light emission with a maximum radiance of approximately 1200 kW sr−1 m−2at 8.5 kA cm−2, a more than two‐fold enhancement to forward radiation output.

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  7. Abstract

    New developments in the field of topological matter are often driven by materials discovery, including novel topological insulators, Dirac semimetals, and Weyl semimetals. In the last few years, large efforts have been made to classify all known inorganic materials with respect to their topology. Unfortunately, a large number of topological materials suffer from non‐ideal band structures. For example, topological bands are frequently convoluted with trivial ones, and band structure features of interest can appear far below the Fermi level. This leaves just a handful of materials that are intensively studied. Finding strategies to design new topological materials is a solution. Here, a new mechanism is introduced, which is based on charge density waves and non‐symmorphic symmetry, to design an idealized Dirac semimetal. It is then shown experimentally that the antiferromagnetic compound GdSb0.46Te1.48is a nearly ideal Dirac semimetal based on the proposed mechanism, meaning that most interfering bands at the Fermi level are suppressed. Its highly unusual transport behavior points to a thus far unknown regime, in which Dirac carriers with Fermi energy very close to the node seem to gradually localize in the presence of lattice and magnetic disorder.

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  8. Abstract When a suspension of spherical or near-spherical particles passes through a constriction the particle volume fraction either remains the same or decreases. In contrast to these particulate suspensions, here we observe that an entangled fiber suspension increases its volume fraction up to 14-fold after passing through a constriction. We attribute this response to the entanglements among the fibers that allows the network to move faster than the liquid. By changing the fiber geometry, we find that the entanglements originate from interlocking shapes or high fiber flexibility. A quantitative poroelastic model is used to explain the increase in velocity and extrudate volume fraction. These results provide a new strategy to use fiber volume fraction, flexibility, and shape to tune soft material properties, e.g., suspension concentration and porosity, during delivery, as occurs in healthcare, three-dimensional printing, and material repair. 
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    Free, publicly-accessible full text available December 1, 2024
  9. In addition to the repulsive and attractive interaction forces described by Derjaguin–Landau–Verwey–Overbeek (DLVO) theory, many charged colloid systems are stabilized by non-DLVO contributions stemming from specific material attributes. Here, we investigate non-DLVO contributions to the stability of polymer colloids stemming from the intra-particle glass transition temperature ( T g ). Flash nanoprecipitation is used to fabricate nanoparticles (NPs) from a library of polymers and dispersion stability is studied in the presence of both hydrophilic and hydrophobic salts. When adding KCl, stability undergoes a discontinuous decrease as T g increases above room temperature, indicating greater stability of rubbery NPs over glassy NPs. Glassy NPs are also found to interact strongly with hydrophobic phosphonium cations (PR 4 + ), yielding charge inversion and intermediate aggregation while rubbery NPs resist ion adsorption. Differences in the lifetime of ionic structuration within mobile surface layers is presented as a potential mechanism underlying the observed phenomenon. 
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