Giant Tunneling Electro‐Resistance in Ultrathin Ferroelectric Tunnel Junctions: The Interface Barrier Gain Mechanism

Abstract Ultrathin ferroelectric tunnel junctions (FTJs) hold considerable promise for next‐generation, high‐speed, low‐power, and high‐density nonvolatile memory applications. Achieving a substantial tunneling electro‐resistance (TER) remains a challenge as the ferroelectric layer is thinned to nanoscale dimensions, often resulting in a diminished or lost polarization. An innovative interface barrier gain mechanism is introduced, employing interface electronic state modulation to precisely control the size of an additional interface barrier. This strategy lessens the dependency of the tunneling barrier on ferroelectric polarization strength, facilitating a remarkable TER even at ferroelectric thicknesses as minimal as ≈1 nm. The focus is on composite FTJs using In 2 Se 3 /MTe 2 (M = Mo, W), where the inclusion of an MTe 2 monolayer disrupts the asymmetric electrode configuration. The weak ferroelectric polarization reversal of the In 2 Se 3 monolayer effectively modulates the electronic state coupling at the In 2 Se 3 /MTe 2 interface. This modulation leads to variations in the width and height of the Schottky barrier at the heterojunction‐electrode interface corresponding with the ferroelectric polarization reversal, establishing a beneficial Ohmic contact in the “on” state and resulting in an exponential TER increase up to 5.4 × 10 6 %. This work introduces a universal mechanism to overcome the thickness limitations traditionally associated with enhancing TER, marking a significant advancement in the development of ultrathin ferroelectric nonvolatile devices.