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Harnessing Ferroelectricity for Agile Control of Twisted Oxide Structures

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Two-dimensional multilayers – made of van der Waals (vdW) compounds like graphene – are a playground for novel physics due to the interference-like structural patterns (moirés) resulting from interlayer lattice mismatch and twist angle. Yet, the remarkable phenomena they host – from anomalous transport to topological polar states – are typically fixed, lacking a key feature to create next-generation ultralow-power devices: the ability to switch electrically between states, potentially non-volatile.
Critically, the field is being revitalized by the advent of freestanding membranes of perovskite oxides. Particularly promising are ferroelectrics with electrically switchable polarization and structure. Moiré engineering offers unique prospects for controlling the polar order and functionality of such materials, as demonstrated by the ultradense electric-vortex patterns reported by my group and collaborators in BaTiO3 bilayers (Nature, 2024).
We can now get ambitious: in ferroelectric oxide moirés, properties result from the interplay between interfacial couplings (unknown, controlled by mismatch and twist) and intrinsic polar order (tunable by bias). I want to control this interplay – and even the twist angle itself – by acting electrically on the ferroelectric layer, exploiting our ability to drive transitions between distinct structures. To accomplish this we need to quantify and understand interlayer interactions, potentially tunable via vdW spacers like graphene.
Given the complex physics and limited experimental data, a simulation approach is essential. We will: (1) develop predictive machine-learning models for key perovskite oxide moirés, including hybrids with graphene; (2) determine how moiré features depend on intrinsic-intralayer vs. interfacial-interlayer couplings; (3) test optimum systems for dynamic electric control. In parallel we will lay the foundation for richer materials/property combinations (magnetic, electronic), unlocking decades of discovery.

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LUXEMBOURG INSTITUTE OF SCIENCE AND TECHNOLOGY
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