High-Throughput Computational Design of High-Performance High-K Dielectrics for 2D Electronics

Two-dimensional (2D) semiconductors such as molybdenum disulfide (MoS2) could potentially replace silicon in future electronic devices. However, the high-performance integration of high-k dielectrics on 2D semiconductors remains a grand challenge. In this talk, we show that for the interface between conventional high-k dielectrics and 2D MoS₂, hydrogenation is a desired approach to passivate the dangling bonds and improve the interface properties, in which the hydrogenation can selectively occur at high-k dielectrics such as Si₃N₄ and HfO₂, and do not affect the 2D semiconductor MoS₂. We further demonstrate the improved performance for hydrogenated interface of HfO₂/MoS₂, as evidenced by the increased carrier mobility, narrow hysteresis window, and much reduced interfere state density. We find that this selective hydrogenation strategy can be generalized to any interface of high-k dielectrics and 2D semiconductors, where there exists free energy difference for hydrogen adsorption between them. Finally, we report a data-driven approach to accelerate the development of various promising inorganic molecular crystals as the high-performance high-k dielectrics for 2D MoS₂ based electronic devices. These results deepen the understanding the interface of 2D semiconductors and high-k dielectrics, and could be useful for developing a broad range of high-performance 2D electronic and optoelectronic devices.