Layered transition-metal dichalcogenides down to the monolayer (ML) limit provide a fertile platform for exploring charge-density waves (CDWs). Here, we experimentally unveil the richness of the CDW phases in ML-NbTe for the first time. Not only the theoretically predicted 4 × 4 and 4 × 1 phases but also two unexpected and phases are realized. For such a complex CDW system, we establish an exhaustive growth phase diagram via systematic efforts in the material synthesis and scanning tunneling microscope characterization. Moreover, the energetically stable phase is the larger-scale order (), which is surprisingly in contradiction to the prior prediction (4 × 4). These findings are confirmed using two different kinetic pathways: i.e., direct growth at proper growth temperatures () and low- growth followed by high- annealing. Our results provide a comprehensive diagram of the "zoo" of CDW orders in ML-NbTe.

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http://dx.doi.org/10.1021/acs.nanolett.2c04306DOI Listing

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