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A large bulk band gap is critical for the applications of quantum spin hall(QSH) insulators in spintronics at room temperature. Based on first-principlescalculations, we predict that the methyl-functionalized III-Bi monolayers,namely III-Bi-(CH3)2 (III=Ga, In, Tl) thin films, own QSH states with band gapas large as 0.260, 0.304 and 0.843 eV, respectively, making them suitable forroom-temperature applications. The topological characteristics are confirmed bys-px,y band inversion, topological invariant Z2, and the topologicallyprotected edge states. Noticeably, for GaBi/InBi-(CH3)2 films, the s-px,y bandinversion occurred in the progress of spin-orbital coupling (SOC), while forTlBi(CH3)2 film, the s-px,y band inversion happened in the progress of chemicalbonding. Significantly, the QSH states in III-Bi-(CH3)2 films are robustagainst the mechanical strains and various methyl coverages, making these filmsparticularly flexible to substrate choice for device applications. Besides, theh-BN substrate is an ideal substrate for III-Bi-(CH3)2 films to realize largegap nontrivial topological states.. These findings demonstrate that themethyl-functionalized III-Bi films may be good QSH effect platforms fortopological electronic devices design and fabrication in spintronics.

Robust Large Gap Quantum Spin Hall Insulators in Methyl-functionalized III-Bi Buckled Honeycombs