Abstract

Atomically thin two-dimensional (2D) materials have aroused an explosive growth of scientific interest for their outstanding physicochemical properties. In addition, decorations of 2D materials with organic semiconductors have also begun to receive scientific attention owing to the tunable optoelectronic properties and the excellent solution-based processability of the organic molecules. In this study, composite films that consisted of C60 with well-exfoliated nanosheets of transition metal dichalcogenides (TMDs) [1], antimony [2], or bismuth [3] were successfully fabricated onto a semiconducting SnO2 electrode via a two-step methodology: self-assembly into their composite aggregates by injection of a poor solvent into a good solvent with the dispersion, and subsequent electrophoretic deposition. In addition, photophysical and photoelectrochemical properties of the composite films were investigated in detail. For example, in a flash-photolysis time-resolved microwave conductivity (FP-TRMC) measurement of a composite material consisting of C60 and few-layered antimonene (FLSb) nanosheets (denoted as (FLSb+C60) m ), a rapid rise in transient conductivity was observed, whereas no conductivity signal was observed in the single components, FLSb and C60. This demonstrated the occurrence of photoinduced charge separation between FLSb and C60 in (FLSb+C60) m . Furthermore, a photoelectrochemical device with an electrophoretically deposited (FLSb+C60) m film exhibited an enhanced efficiency of photocurrent generation, compared to those of the single-components, FLSb and C60, due to the photoinduced charge separation between FLSb and C60. This work provides a promising approach for fabrication of 2D material–organic molecule composites and paves the way for their application in optoelectronics.[1] J. Baek, T. Umeyama, W. Choi, Y. Tsutsui, H. Yamada, S. Seki, and H. Imahori, Chem. Eur. J., 24, 1561-1572 (2018).[2] T. Umeyama, T. Ohara, Y. Tsutsui, S. Nakano, S. Seki, and H. Imahori, Chem. Eur. J., 26, 6726-6735 (2020).[3] T. Umeyama, H. Xu, T. Ohara, Y. Tsutsui, S. Seki, and H. Imahori, J. Phys. Chem. C, 125, 13954-13962 (2021).

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