Dimensional crossover of charge order in IrTe2 with strong interlayer coupling

Tuning dimensionality in van der Waals materials with finite interlayer coupling has introduced various electronic phase transitions by conventional mechanical exfoliation. Particularly when the electronic order is tied to the modulation of the interlayer coupling, such dimensional tunability has a strong impact on its stability and properties, which has rarely been investigated experimentally. Here, we demonstrate a dimensional crossover of charge order in IrTe2 from genuine two- to quasi-three-dimensions using low-temperature scanning tunneling microscopy and spectroscopy. Employing atomically thin IrTe2 flakes ranging from monolayer to multilayer, we observe a gradual phase transition of charge order and exponential decay of Coulomb gap with increasing thickness. Moreover, we find a suppression of the density of states emerging at an abrupt lateral interface between two and three dimensions. These findings are attributed to the interplay between the strongly coupled layers and substrate-driven perturbation, which can provide a new insight into the dimensional crossover of strongly coupled layered materials with hidden electronic phases.