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Dynamic control of conductivity and optical properties via atomic structurechanges is of tremendous technological importance in information storage.Energy consumption considerations provide a driving force toward employing thinmaterials in devices. Monolayer transition metal dichalcogenides are nearlyatomically-thin materials that can exist in multiple crystal structures, eachwith distinct electrical properties. Using density functional approaches, wediscover that electrostatic gating device configurations have the potential todrive structural semiconductor-to-semimetal phase transitions in some monolayertransition metal dichalcogenides. For the first time, we show that thedynamical control of this phase transition can be achieved in carefullydesigned electronic devices. We discover that the semiconductor-to-semimetalphase transition in monolayer MoTe2 can be driven by a gate voltage of severalVolts with appropriate choice of dielectric. Structural transitions inmonolayer TaSe2 are predicted to occur under similar conditions. While therequired field magnitudes are large for these two materials, we find that thegate voltage for the transition can be reduced arbitrarily by alloying, e.g.for MoxW1-xTe2 monolayers. We have developed a method for computing phasediagrams of monolayer materials with respect to charge and voltage, validatedby comparing to direct calculations and experimental measurements. Our findingsidentify a new physical mechanism, not existing in bulk materials, todynamically control structural phase transitions in two-dimensional materials,enabling potential applications in phase-change electronic devices.

Structural Semiconductor-to-Semimetal Phase Transition in Two-Dimensional Materials Induced by Electrostatic Gating