The pursuit of high-temperature quantum anomalous Hall (QAH) insulators faces fundamental challenges, including narrow topological gaps and low Curie temperatures (TC) in existing materials. Here, we propose a transformative strategy using bilateral hydrogenation to engineer a robust QAH state in the topologically trivial ferromagnetic semiconductor Cr2Ge2Te6. First-principles calculations reveal that hydrogenation induces a topological phase transition in Cr2Ge2Te6 by shifting its Dirac points-originally embedded in the conduction bands-to the vicinity of the Fermi level in Cr2Ge2Te6H6. This electronic restructuring, coupled with spin-orbit coupling, opens a global topological gap of 118.1 meV, establishing a robust QAH state with Chern number C= 3. Concurrently, hydrogenation enhances ferromagnetic superexchange via the dz2-pz-dxz channel, significantly strengthening the nearest-neighbor coupling J1 by 3.06 times and switching J2 from antiferromagnetic to ferromagnetic. Monte Carlo simulations predict a high TC = 198 K, sustained well above liquid nitrogen temperature and far exceeding pristine Cr2Ge2Te6 (28 K). This work establishes surface hydrogenation as a powerful route to simultaneously control topology and magnetism in 2D materials, unlocking high-temperature QAH platforms for dissipationless spintronic applications.
@article{arxiv.2509.09164,
title = {Bilateral Hydrogenation Realizes High-Temperature Quantum Anomalous Hall Insulator in 2D Cr$_{\text{2}}$Ge$_{\text{2}}$Te$_{\text{6}}$},
author = {Xiang Li and Xin-Wei Yi and Jing-Yang You and Jia-Wen Li and Qing-Han Yang and Gang Su and Bo Gu},
journal= {arXiv preprint arXiv:2509.09164},
year = {2025}
}