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Creators/Authors contains: "Huang, Chen"

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  1. We apply ultrafast nanoscale microscopic imaging and analytical modeling to investigate the coherent field and spin textures of dual plasmonic vortices as a means to design the momentum flow, and spin topology by interaction of their gyrating fields. The ultrafast laser normal incidence illumination by circularly polarized light of two vortex generator structures with variable separations in silver films launches structured surface plasmon polariton fields. Two distinct primary vortices and a third emergent vortex, generated by interaction of the primary vortices and tunable by design of their separation, form through the spin–orbit interaction of light. The gyration of plasmon fields and the consequent vectorial Poynting momentum flow is imaged with sub-optical cycle phase and spatial resolution by interferometric time-resolved two-photon photoemission electron microscopy (ITR-2P-PEEM). The ultrafast imaging and analytical modeling of the interaction of the dual plasmonic vortices examines the nanoscale control of plasmon spin topology and momentum driven transport. 
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  2. The Cl–S mixed-anion sublattice of Li1.6AlCl3.4S0.6creates face- and edge-shared octahedra that connect to form 3D ion conduction pathways with low activation energy barriers. 
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  3. Abstract Localized atomistic disorder in halide‐based solid electrolytes (SEs) can be leveraged to boost Li+mobility. In this study, Li+transport in structurally modified Li3HoCl6, via Brintroduction and Li+deficiency, is explored. The optimized Li3‐3yHo1+yCl6‐xBrxachieves an ionic conductivity of 3.8 mS cm−1at 25 °C, the highest reported for holmium halide materials.6,7Li nuclear magnetic resonance and relaxometry investigations unveil enhanced ion dynamics with bromination, attaining a Li+motional rate neighboring 116 MHz. X‐ray diffraction analyses reveal mixed‐anion‐induced phase transitions with disproportionate octahedral expansions and distortions, creating Ho‐free planes with favorable energetics for Li+migration. Bond valence site energy analysis highlights preferred Li+transport pathways, particularly in structural planes devoid of Ho3+blocking effects. Molecular dynamics simulations corroborate enhanced Li+diffusion with Brintroduction into Li3HoCl6. Li‐Ho electrostatic repulsions in the (001) plane presumably drive Li+diffusion into the Ho‐free (002) layer, enabling rapid intraplanar Li+motion and exchange between the 2d and 4h sites. Li3‐3yHo1+yCl6‐xBrxalso demonstrates good battery cycling stability. These findings offer valuable insights into the intricate correlations between structure and ion transport and will help guide the design of high‐performance fast ion conductors for all‐solid‐state batteries. 
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  4. Li3.6In7S11.8Cl has a face-centered cubic arrangement of S2−/Clstabilized by Li+/In3+that form 3D ion conduction paths. The moisture stability and fast ion conduction make Li3.6In7S11.8Cl a promising electrolyte for solid-state batteries. 
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  5. Abstract All‐solid‐state potassium batteries emerge as promising alternatives to lithium batteries, leveraging their high natural abundance and cost‐effectiveness. Developing potassium solid electrolytes (SEs) with high room‐temperature ionic conductivity is critical for realizing efficient potassium batteries. In this study, we present the synthesis of K2.98Sb0.91S3.53Cl0.47, showcasing a room‐temperature ionic conductivity of 0.32 mS/cm and a low activation energy of 0.26 eV. This represents an increase of over two orders of magnitude compared to the parent compound K3SbS4, marking the highest reported ionic conductivity for non‐oxide potassium SEs. Solid‐state39K magic‐angle‐spinning nuclear magnetic resonance on K2.98Sb0.91S3.53Cl0.47reveals an increased population of mobile K+ions with fast dynamics. Ab initio molecular dynamics (AIMD) simulations further confirm a delocalized K+density and significantly enhanced K+diffusion. This work demonstrates diversification of the anion sublattice as an effective approach to enhance ion transport and highlights K2.98Sb0.91S3.53Cl0.47as a promising SE for all‐solid‐state potassium batteries. 
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  6. Abstract We report a theoretical investigation of effects of Mn and Co substitution in the transition metal sites of the kagomé-lattice ferromagnet, Fe 3 Sn 2 . Herein, hole- and electron-doping effects of Fe 3 Sn 2 have been studied by density-functional theory calculations on the parent phase and on the substituted structural models of Fe 3− x M x Sn 2 (M = Mn, Co; x = 0.5, 1.0). All optimized structures favor the ferromagnetic ground state. Analysis of the electronic density of states (DOS) and band structure plots reveals that the hole (electron) doping leads to a progressive decrease (increase) in the magnetic moment per Fe atom and per unit cell overall. The high DOS is retained nearby the Fermi level in the case of both Mn and Co substitutions. The electron doping with Co results in the loss of nodal band degeneracies, while in the case of hole doping with Mn emergent nodal band degeneracies and flatbands initially are suppressed in Fe 2.5 Mn 0.5 Sn 2 but re-emerge in Fe 2 MnSn 2 . These results provide key insights into potential modifications of intriguing coupling between electronic and spin degrees of freedom observed in Fe 3 Sn 2 . 
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