arXiv · 2606.18477
Hydration-controlled twist forms a moir\'e glass in charge-frustrated layered silicates
Abstract
Twisting layered materials produces moir\'e superlattices, but prescribed twist angles are usually obtained by demanding assembly procedures. Here we show that montmorillonite, an abundant swelling clay, forms tunable moir\'e superlattices naturally. Focal-series high-resolution transmission electron microscopy, geometric phase analysis, and molecular dynamics simulation reveal that its apparent rotational disorder is biased toward low-angle misorientations inherited from discrete hydration states. Multilayer stacks preferentially adopt twists near 1-2{\deg}, 4{\deg}, and 10{\deg}, producing long-wavelength moir\'es without long-range rotational order. We define this kinetically trapped state as a moir\'e glass, distinct from featureless turbostratic stacking. Simulations indicate that lattice-charge disorder stabilizes the angular preferences, whereas charge ordering promotes random stacking. Hydration screens interlayer interactions and lubricates twist, while dehydration arrests the resulting configurations in discrete steps. These results establish dynamic hydration as a macroscopic handle for programming twist in layered matter.
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Juhyeok Lee, Piotr Zarzycki, Colin Ophus, Jim Ciston, Benjamin Gilbert, Jillian F. Banfield, Mary C. Scott, Michael L. Whittaker. 2026-06-16. Hydration-controlled twist forms a moir\'e glass in charge-frustrated layered silicates. https://arxiv.org/abs/2606.18477
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