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تسجيل مستخدم جديدTunable electrochemistry with moire flat bands and topological defects at twisted bilayer graphene
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Tailoring electron transfer dynamics across solid-liquid interfaces is fundamental to the interconversion of electrical and chemical energy. Stacking atomically thin layers with a very small azimuthal misorientation to produce moire superlattices enables the controlled engineering of electronic band structures and the formation of extremely flat electronic bands. Here, we report a strong twist angle dependence of heterogeneous charge transfer kinetics at twisted bilayer graphene electrodes with the greatest enhancement observed near the magic angle (~1.1 degrees). This effect is driven by the angle-dependent tuning of moire-derived flat bands that modulate electron transfer processes with the solution-phase redox couple. Combined experimental and computational analysis reveals that the variation in electrochemical activity with moire angle is controlled by atomic reconstruction of the moire superlattice at twist angles <2 degrees, and topological defect AA stacking regions produce a large anomalous local electrochemical enhancement that cannot be accounted for by the elevated local density of states alone. Our results introduce moire flat band materials as a distinctively tunable paradigm for mediating electrochemical transformations.
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Twisted graphene bilayers provide a versatile platform to engineer metamaterials with novel emergent properties by exploiting the resulting geometric moir{e} superlattice. Such superlattices are known to host bulk valley currents at tiny angles ($alp
haapprox 0.3 ^circ$) and flat bands at magic angles ($alpha approx 1^circ$). We show that tuning the twist angle to $alpha^*approx 0.8^circ$ generates flat bands away from charge neutrality with a triangular superlattice periodicity. When doped with $pm 6$ electrons per moire cell, these bands are half-filled and electronic interactions produce a symmetry-broken ground state (Stoner instability) with spin-polarized regions that order ferromagnetically. Application of an interlayer electric field breaks inversion symmetry and introduces valley-dependent dispersion that quenches the magnetic order. With these results, we propose a solid-state platform that realizes electrically tunable strong correlations.
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We present electronic structure calculations of twisted double bilayer graphene (TDBG): A tetralayer graphene structure composed of two AB-stacked graphene bilayers with a relative rotation angle between them. Using first-principles calculations, we
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