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Abstract TiSe2is an exciting material because it can be tuned between superconducting and charge density wave (CDW) transitions. In the monolayer limit, TiSe2exhibits a sizable energy gap in the CDW phase that makes it a promising quantum material. It is shown that interfacing a single layer of TiSe2with dissimilar van der Waals materials enables control of its properties. Using angle‐resolved photoemission spectroscopy, the energy gap opening is analyzed as a function of temperature for TiSe2monolayers supported on different van der Waals substrates. A substantial increase in the CDW transition temperature of ≈45 K is observed on MoS2compared to graphite (highly oriented pyrolytic graphite) substrates. This control of the CDW in monolayer TiSe2is suggested to arise from varying charge screening of the unconventional CDW of TiSe2by the substrate. In addition, the suppression of CDW order and a complete closing of the energy gap by electron doping of monolayer TiSe2is demonstrated. Regulating the many‐body physics phenomena in monolayer TiSe2lays the foundation of modifying TiSe2in, for example, artificial van der Waals heterostructures and thus creates a new approach for utilizing the quantum states of TiSe2in device applications.more » « less
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