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Realization of Coexisting Charge Density Wave and Quantum Spin/Anomalous Hall State in Monolayer NbTe2

The combination of nontrivial topology and charge density wave (CDW) has been proposed as a powerful resource for realizing novel quantum phenomena such as axion electrodynamics and the anomalous Hall effect. Hence, topological materials with CDW states attract great interest, yet they are still very rare, particularly in the 2D limit. Here, it is predicted that monolayer NbTe2 in its high‐symmetry 1T phase stabilized by anharmonicity at room temperature exhibits nontrivial topology sensitive to electronic interactions: it changes from a quantum spin Hall (QSH) state to a quantum anomalous Hall (QAH) state when the Hubbard potential U exceeds a critical value. At low temperature, a 4 × 4 CDW order emerges and coexists with the nontrivial topology. Meanwhile, the critical U increases because CDW reduces density of states at Fermi level. More interestingly, in contrast to the high‐symmetry structure that actually is a topologically nontrivial metal, the CDW structure shows an insulating nontrivial gap either in the QSH or the QAH phase, indicating CDW is an effective means to modulate the topological state for developing new functions and devices. These discoveries establish NbTe2 as a promising candidate to explore exotic quantum states at the confluence of nontrivial topology, electronic correlation, and CDW.