Electric-Field-Induced Reversible Phase Transitions in a Spontaneously Ion-Intercalated 2D Metal Oxide

Electric field driven reversible phase transitions in two-dimensional (2D) materials are appealing for their potential in switching applications. Here, we introduce potassium intercalated MnO₂ as an exemplary case. We demonstrate the synthesis of large-area single-crystal layered MnO₂ via chemical vapor deposition as thin as 5 nm. These crystals are spontaneously intercalated by potassium ions during the synthesis. We showed that the charge transport in 2D K-MnO₂ is dominated by motion of hydrated potassium ions in the interlayer space. Under a few volts bias, separation of potassium and the structural water leads to formation of different phases at the opposite terminals, and at larger biases K-MnO₂ crystals exhibit reversible layered-to-spinel phase transition. These phase transitions are accompanied by electrical and optical changes in the material. We used the electric field driven ionic motion in K-MnO₂ based devices to demonstrate the memristive capabilities of two terminal devices.