Hybrid molecular graphene transistor as an operando and optoelectronic platform

Lack of reproducibility hampers molecular devices integration into large-scale circuits. Thus, incorporating operando characterization can facilitate the understanding of multiple features producing disparities in different devices. In this work, we report the realization of hybrid molecular graphene field effect transistors (m-GFETs) based on 11-(Ferrocenyl)undecanethiol (FcC11SH) micro self-assembled monolayers (μSAMs) and high-quality graphene (Gr) in a back-gated configuration. On the one hand, Gr enables redox electron transfer, avoids molecular degradation and permits operando spectroscopy. On the other hand, molecular electrode decoration shifts the Gr Dirac point (VDP) to neutrality and generates a photocurrent in the Gr electron conduction regime. Benefitting from this heterogeneous response, the m-GFETs can implement optoelectronic AND/OR logic functions. Our approach represents a step forward in the field of molecular scale electronics with implications in sensing and computing based on sustainable chemicals ; We acknowledge the Comunidad de Madrid projects NMAT-2D-P2018/NMT-451 and TEC2SPACE-CM P2018/NMT-4291. IMDEA Nanociencia thanks support from the “Severo Ochoa” Programme for Centers of Excellence in R&D (MINECO, Grant CEX2020-001039-S). This work was also supported by Ministry of Science, Innovation and Universities under Grants PID2019-105552RB-C4-1 and ESP2017-92706-EXP, MADE MICINN: PID2019-105552RB-C44. We also acknowledge financial support from ONR-Global under Grant DEFROST N62909-19-1-2053 and EMPIR-20FUN06-MEMQuD-EURAMET. MAN, MF and MWK acknowledge funding by MICINN through PID 2021-122980OB C54. MWK acknowledges funding from Horizon 2020 Marie Skłodowska-Curie COFUND DOC-FAM, with Grant agreement No. 754397. PEEM experiments were performed at CIRCE beamline at ALBA Synchrotron Light Facility with experiment ID AV-2020024142