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The rediscovery of one-dimensional (1D) and quasi-1D (q-1D) van der Waals (vdW) crystals ushered the realization of nascent physical properties in 1D that are suitable for applications in photonics, electronics, and sensing. However, despite renewed interest in the creation and understanding of the physical properties of 1D and q-1D vdW crystals, the lack of accessible synthetic pathways for growing well-defined nanostructures that extend across several length scales remains. Using the highly anisotropic 1D vdW NbS3–I crystal as a model phase, we present a catalyst-free and bottom-up synthetic approach to access ultralong nanowires, with lengths reaching up to 7.9 mm and with uniform thicknesses ranging from 13 to 160 nm between individual nanowires. Control over the synthetic parameters enabled the modulation of intra- and interchain growth modalities to selectively yield only 1D nanowires or quasi-2D nanoribbons. Comparative synthetic and density functional theory (DFT) studies with a closely related nondimerized phase, ZrS3, show that the unusual preferential growth along 1D can be correlated to the strongly anisotropic bonding and dimeric nature of NbS3–I.more » « less
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Single photon emitters (SPEs) in hexagonal boron nitride (hBN) are elementary building blocks for room-temperature on-chip quantum photonic technologies. However, fundamental challenges, such as slow radiative decay and nondeterministic placement of the emitters, limit their full potential. Here, we demonstrate large-area arrays of plasmonic nanoresonators (PNRs) for Purcell-induced room-temperature SPEs by engineering emitter-cavity coupling and enhancing radiative emission. Gold-coated silicon pillars with an alumina spacer enable a 10-fold local-field enhancement in the emission band of native hBN defects. We observe bright SPEs with an average saturated emission rate surpassing 5 million counts per second, an average lifetime of <0.5 ns, and 29% yield. Density functional theory reveals the beneficial role of an alumina spacer between hBN and gold, mitigating the electronic broadening of emission from defects proximal to the metal. Our results offer arrays of bright, heterogeneously integrated single-photon sources, paving the way for robust and scalable quantum information systems.more » « less
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Abstract Oxide solid electrolytes (OSEs) have the potential to achieve improved safety and energy density for lithium-ion batteries, but their high grain-boundary (GB) resistance generally is a bottleneck. In the well-studied perovskite oxide solid electrolyte, Li 3 x La 2/3- x TiO 3 (LLTO), the ionic conductivity of grain boundaries is about three orders of magnitude lower than that of the bulk. In contrast, the related Li 0.375 Sr 0.4375 Ta 0.75 Zr 0.25 O 3 (LSTZ0.75) perovskite exhibits low grain boundary resistance for reasons yet unknown. Here, we use aberration-corrected scanning transmission electron microscopy and spectroscopy, along with an active learning moment tensor potential, to reveal the atomic scale structure and composition of LSTZ0.75 grain boundaries. Vibrational electron energy loss spectroscopy is applied for the first time to reveal atomically resolved vibrations at grain boundaries of LSTZ0.75 and to characterize the otherwise unmeasurable Li distribution therein. We find that Li depletion, which is a major reason for the low grain boundary ionic conductivity of LLTO, is absent for the grain boundaries of LSTZ0.75. Instead, the low grain boundary resistivity of LSTZ0.75 is attributed to the formation of a nanoscale defective cubic perovskite interfacial structure that contained abundant vacancies. Our study provides new insights into the atomic scale mechanisms of low grain boundary resistivity.more » « less
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