Two-dimensional (2D) room-temperature ferromagnetism is highly sought after for its great application potential but is challenged by chemical or magnetic structural instability. If room-temperature ferromagnetism can be realized in structurally stable 2D graphene, it will have a broad application prospect and market in flexible spintronics and wearable artificial intelligence. Although symmetry breaking such as vacancies, edges can introduce localized magnetic moments in intrinsically antimagnetic graphene, their weak coupling can only hold long-range ordering at low temperatures. Here, a robust ferromagnetic order has been observed in large-area graphene (centimeter scale) through mechanical folding and successive preprocesses of rapid cooling and heating method, where the Curie temperature of ∼6-layer graphene is close to 100 K and that of ∼10-layer graphene is above room temperature. We propose that the observed ferromagnetism is possibly attributed to the surface sp3-type bonds emergent in the structure phase transition caused by strain effects.
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