Twist-Angle Engineering of Moiré Potentials for High-Performance Ionics in Bilayer Graphene

Fuente: arXiv
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Autores principales: Fukuzawa, Gen, Lee, Yebin, Mizoguchi, Teruyasu
Formato: Preprint
Publicado: 2026
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author Fukuzawa, Gen
Lee, Yebin
Mizoguchi, Teruyasu
author_facet Fukuzawa, Gen
Lee, Yebin
Mizoguchi, Teruyasu
contents Controlling ion transport is a fundamental challenge for advanced energy storage. Bilayer graphene offers a unique platform for modulating ion diffusion via twist-angle-dependent moire superlattices, yet conventional stacking configurations face an inherent trade-off: AA stacking provides stable Li intercalation but high diffusion barriers, while AB stacking enables fast diffusion but poor intercalation stability. Twisted bilayer graphene (tBLG) offers potential to overcome this limitation, yet systematic understanding across different twist angles remains limited. Here, we investigate Li intercalation in tBLG using first-principles density functional theory, evaluating intercalation energies and diffusion barriers across multiple twist angles through potential energy surface (PES) mapping. The Sigma 37 structure (9.43 degrees) simultaneously achieves the most favorable intercalation energy (-2.39 eV) and the lowest diffusion barrier (0.14 eV) among all structures examined, resolving the conventional stacking trade-off. Furthermore, using the Smooth Overlap of Atomic Positions (SOAP) descriptor, we demonstrate that the PES is governed by local atomic environments and that a model trained on limited structures predicts the PES of untested configurations with high accuracy. This transferability enables efficient screening without exhaustive first-principles calculations, establishing a systematic framework for twist-angle engineering of ion transport in two-dimensional layered materials.
format Preprint
id arxiv_https___arxiv_org_abs_2603_27453
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Twist-Angle Engineering of Moiré Potentials for High-Performance Ionics in Bilayer Graphene
Fukuzawa, Gen
Lee, Yebin
Mizoguchi, Teruyasu
Materials Science
Controlling ion transport is a fundamental challenge for advanced energy storage. Bilayer graphene offers a unique platform for modulating ion diffusion via twist-angle-dependent moire superlattices, yet conventional stacking configurations face an inherent trade-off: AA stacking provides stable Li intercalation but high diffusion barriers, while AB stacking enables fast diffusion but poor intercalation stability. Twisted bilayer graphene (tBLG) offers potential to overcome this limitation, yet systematic understanding across different twist angles remains limited. Here, we investigate Li intercalation in tBLG using first-principles density functional theory, evaluating intercalation energies and diffusion barriers across multiple twist angles through potential energy surface (PES) mapping. The Sigma 37 structure (9.43 degrees) simultaneously achieves the most favorable intercalation energy (-2.39 eV) and the lowest diffusion barrier (0.14 eV) among all structures examined, resolving the conventional stacking trade-off. Furthermore, using the Smooth Overlap of Atomic Positions (SOAP) descriptor, we demonstrate that the PES is governed by local atomic environments and that a model trained on limited structures predicts the PES of untested configurations with high accuracy. This transferability enables efficient screening without exhaustive first-principles calculations, establishing a systematic framework for twist-angle engineering of ion transport in two-dimensional layered materials.
title Twist-Angle Engineering of Moiré Potentials for High-Performance Ionics in Bilayer Graphene
topic Materials Science
url https://arxiv.org/abs/2603.27453