Abstract

Molecular functional devices have been investigated through the study of molecular structure and its corresponding discrete orbital states since it determines the transport behaviors. [1,2] In contrast to the conventional strategy, we have demonstrated a novel strategy and design rule for realizing molecular-scale functions based on the energy band engineering in molecular heterojunction with two-dimensional (2D) semiconductors [3,4]. Recently, we have designed molecular heterojunction selector and the nonlinearity design rule with the role of the molecular dipole moment orientation which controls the band bending of the 2D semiconductor [4]. Likewise, various role of the molecular self-assembled monolayer (SAM) in hybrid heterostructure device with 2D semiconductor can give a novel and diverse functionality to the device that it can be a powerful platform for the next-generation functional devices. We implemented ferrocene substituted alkanethiol SAMs, which is a redox active molecule [5], in 2D MoS2 field-effect transistor (FET) structure. The redox state (oxidation or reduction) of the SAM is controlled through the gate bias and the oxidized molecular states (Fc -> Fc+) can act as a localized gate at the interface between molecule/2D semiconductor (MoS2) which the conductance of the n-type MoS2 channel can be modulated. This MoS2 FET with non-volatile multistate MoS2 channel can be suggested as electrochemically programmed molecular heterojunction artificial synapse.[1] L. A. Bumm, J. J. Arnold, M. T. Cygan, T. D. Dunbar, T. P. Burgin, L. Jones, D. L. Allara, J. M. Tour, P. S. Weiss, Science 271, 1705 ( 1996),.[2] H. Song, Y. Kim, Y. H. Jang, H. Jeong, M. A. Reed, T. Lee, Nature 462, 1039 ( 2009).[3] J. Shin, S. Yang, Y. Jang, J. S. Eo, T.-W. Kim, T. Lee, C.-H. Lee, G. Wang, Nat. Commun. 11, 1 (2020).[4] J. S. Eo, J. Shin, S. Yang, T. Jeon, J. Lee, S. Choi, C.-H. Lee, G. Wang, Adv. Sci. 2101390 (2021).[5] Y. Zhao, S. Bertolazzi, M. S. Maglione, C. Rovira, M. Mas-Torrent, P. Samori, Adv. Mater. 32, 2000740 (2020).

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