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

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

ACS Nano

10.1021/acsnano.5c12416

https://doi.org/10.1021/acsnano.5c12416

Tong Yang, Jingyu He, Keda Ding, Ke Yang, Wei Han, Minggang Zeng, Yulin Yang, Jiong Zhao, Yang Chai, Shu Ping Lau, Kian Ping Loh, Jun Zhou, Ming Yang

01 October 2025

Yang, T., He, J., Ding, K., Yang, K., Han, W., Zeng, M., Yang, Y., Zhao, J., Chai, Y., Lau, S. P., Loh, K. P., Zhou, J., & Yang, M. (2025). High-Throughput Computational Design of Inorganic Molecular Crystal-Based High-κ Dielectrics for Two-Dimensional Electronics. ACS Nano. https://doi.org/10.1021/acsnano.5c12416

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.

Publisher Copyright

There was no specific funding for the research done

This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Nano, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see 10.1021/acsnano.5c12416

https://oar.a-star.edu.sg/communities-collections/articles/22366

1936-0851
1936-086X

Institute of High Performance Computing