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Covalent organic frameworks linked by carbon‐carbon double bonds (C=C COFs) are an emerging class of crystalline, porous, and conjugated polymeric materials with potential applications in organic electronics, photocatalysis, and energy storage. Despite the rapidly growing interest in sp2 carbon‐conjugated COFs, only a small number of closely related condensation reactions have been successfully employed for their synthesis to date. Herein, we report the first example of a C=C COF, CORN‐COF‐1 (CORN = Cornell University), prepared by N‐heterocyclic carbene (NHC) dimerization. In‐depth characterization reveals that CORN‐COF‐1 possesses a two‐dimensional layered structure and hexagonal guest‐accessible pores decorated with a high density of strongly reducing tetraazafulvalene linkages. Exposure of CORN‐COF‐1 to tetracyanoethylene (TCNE, E1/2 = 0.13 V and −0.87 V vs. SCE) oxidizes the COF and encapsulates the radical anion TCNE•− and the dianion TCNE2− as guest molecules, as confirmed by spectroscopic and magnetic analysis. Notably, the reactive TCNE•− radical anion, which generally dimerizes in the solid state, is uniquely stabilized within the pores of CORN‐COF‐1. Overall, our findings broaden the toolbox of reactions available for the synthesis of redox‐active C=C COFs, paving the way for the design of novel materials.

Skyrmions and antiskyrmions are nanoscale swirling textures of magnetic moments formed by chiral interactions between atomic spins in magnetic noncentrosymmetric materials and multilayer films with broken inversion symmetry. These quasiparticles are of interest for use as information carriers in next-generation, low-energy spintronic applications. To develop skyrmion-based memory and logic, we must understand skyrmion-defect interactions with two main goals—determining how skyrmions navigate intrinsic material defects and determining how to engineer disorder for optimal device operation. Here, we introduce a tunable means of creating a skyrmion-antiskyrmion system by engineering the disorder landscape in FeGe using ion irradiation. Specifically, we irradiate epitaxial B20-phase FeGe films with 2.8 MeV Au⁴⁺ions at varying fluences, inducing amorphous regions within the crystalline matrix. Using low-temperature electrical transport and magnetization measurements, we observe a strong topological Hall effect with a double-peak feature that serves as a signature of skyrmions and antiskyrmions. These results are a step towards the development of information storage devices that use skyrmions and antiskyrmions as storage bits, and our system may serve as a testbed for theoretically predicted phenomena in skyrmion-antiskyrmion crystals.

We present measurements of thermally generated transverse spin currents in the topological insulator Bi₂Se₃, thereby completing measurements of interconversions among the full triad of thermal gradients, charge currents, and spin currents. We accomplish this by comparing the spin Nernst magneto-thermopower to the spin Hall magnetoresistance for bilayers of Bi₂Se₃/CoFeB. We find that Bi₂Se₃does generate substantial thermally driven spin currents. A lower bound for the ratio of spin current density to thermal gradient is$\frac{J_s}{{\mathbf{\nabla }}_{\mathit{x}}\mathit{T}}$= (4.9 ± 0.9) × 10⁶$\left(\frac{\hslash }{2e}\right)\frac{\mathbf{A}{\mathbf{m}}^{\mathbf{-}\mathbf{2}}}{\mathbf{K}\text{μ}{\mathbf{m}}^{\mathbf{-}\mathbf{1}}}$, and a lower bound for the magnitude of the spin Nernst ratio is −0.61 ± 0.11. The spin Nernst ratio for Bi₂Se₃is the largest among all materials measured to date, two to three times larger compared to previous measurements for the heavy metals Pt and W. Strong thermally generated spin currents in Bi₂Se₃can be understood via Mott relations to be due to an overall large spin Hall conductivity and its dependence on electron energy.