A Gapped Phase in Semimetallic T_d‐WTe₂ Induced by Lithium Intercalation

Abstract The Weyl semimetal WTe₂ has shown several correlated electronic behaviors, such as the quantum spin Hall effect, superconductivity, ferroelectricity, and a possible exciton insulator state, all of which can be tuned by various physical and chemical approaches. Here, a new electronic phase in WTe₂ induced by lithium intercalation is discovered. The new phase exhibits an increasing resistivity with decreasing temperature and its carrier density is almost two orders of magnitude lower than the carrier density of the semimetallic T_d phase, probed by in situ Hall measurements as a function of lithium intercalation. The theoretical calculations predict the new lithiated phase to be a potential charge density wave (CDW) phase with a bandgap of ≈0.14 eV, in good agreement with the in situ transport data. The new phase is structurally distinct from the initial T_d phase, characterized by polarization‐angle‐dependent Raman spectroscopy, and large lattice distortions close to 6% are predicted in the new phase. This finding of a new gapped phase in a 2D semimetal demonstrates electrochemical intercalation as a powerful tuning knob for modulating electron density and phase stability in 2D materials.