High-Throughput Computational Design of Inorganic Molecular Crystal-Based High-κ Dielectrics for Two-Dimensional Electronics

Inorganic molecular crystals (IMCs) hold great promise as high-κ dielectrics for two-dimensional (2D) electronics due to their dangling-bond-free surfaces and the capability of direct integration on 2D semiconductors. However, only a limited number of IMCs have been identified so far, and interface properties between IMC-based high-κ dielectrics and 2D semiconductors remain largely unexplored. Here, we present an efficient high-throughput screening of IMC-based high-κ dielectrics from a large materials database, of which 6 IMCs (Sb2S2O9, two Bi2O3 phases, As2S2O9, Sb2O3, and Te2H2O3F4) have been predicted to be the most promising gate dielectrics for 2D semiconductors due to their optimal trade-off between dielectric constant and band gap, as well as facile growth possibility. For predominant 2D semiconducting channel materials such as molybdenum disulfide (MoS2) and black phosphorene (BP), the respective promising IMC-based high-κ dielectrics have been pinpointed. We further showcase two high-performance 2D semiconductor/IMC interfaces (BP/Sb2S2O9 and MoS2/Bi2O3), as evidenced by large band offsets, high defect tolerance, and low leakage current. The downscaling capability of the IMCs to the sub-1 nm equivalent oxide thickness (EOT) regime is also unraveled for both dynamic random access memory (DRAM) and central processing unit (CPU) applications. Our results accelerate the exploration of IMC-based high-κ dielectrics and promote the development of high-performance 2D electronics.