First-principles design of ferromagnetic monolayer MnO2 at the complex interface

Abstract

Abstract Rapidly increasing interest in low-dimensional materials is driven by the emerging requirement to develop nanoscale solid-state devices with novel functional properties that are not available in three-dimensional bulk phases. Among the well-known low-dimensional systems, complex transition metal oxide interface holds promise for broad applications in electronic and spintronics devices. Herein, intriguing metal-insulator and ferromagnetic-antiferromagnetic transitions are achieved in monolayer MnO2 that is sandwiched into SrTiO3-based heterointerface systems through interface engineering. By using first-principles calculations, we modeled three types of SrTiO3-based heterointerface systems with different interface terminations and performed a comparative study on the spin-dependent magnetic and electronic properties that are established in the confined MnO2 monolayer. First-principles study predicts that metal-insulator transition and magnetic transition in the monolayer MnO2 are independent on the thickness of capping layers. Moreover, 100% spin-polarized two-dimensional electron gases accompanied by robust room temperature magnetism are uncovered in the monolayer MnO2. Not only is the buried MnO2 monolayer a new interface phase of fundamental physical interest, but it is also a promising candidate material for nanoscale spintronics applications. Our study suggests interface engineering at complex oxide interfaces is an alternative approach to designing high-performance two-dimensional materials.