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For broad nanoscale applications, it is crucial to implement more functional properties, especially those ferroic orders, into two-dimensional materials. Here GdI is theoretically identified as a honeycomb antiferromagnet with large magnetic moment. The intercalation of metal atoms can dope electrons into Gd’s -orbitals, which alters its magnetic state and lead to Peierls transition. Due to the strong electron-phonon coupling, the Peierls transition induces prominent ferroelasticity, making it a multiferroic system. The strain from undirectional stretching can be self-relaxed via resizing of triple ferroelastic domains, which can protect the magnet aganist mechnical breaking in flexible applications.

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