A Cu3BHT-Graphene van der Waals Heterostructure with Strong Interlayer Coupling for Highly Efficient Photoinduced Charge Separation

Zhiyong Wang, Shuai Fu, Wenjie Zhang, Baokun Liang, Tsai Jung Liu, Mike Hambsch, Jonas F. Pöhls, Yufeng Wu, Jianjun Zhang, Tianshu Lan, Xiaodong Li, Haoyuan Qi, Miroslav Polozij, Stefan C.B. Mannsfeld, Ute Kaiser, Mischa Bonn, R. Thomas Weitz, Thomas Heine, Stuart S.P. Parkin*, Hai I. Wang*Renhao Dong*, Xinliang Feng*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

Two-dimensional van der Waals heterostructures (2D vdWhs) are of significant interest due to their intriguing physical properties critically defined by the constituent monolayers and their interlayer coupling. Synthetic access to 2D vdWhs based on chemically tunable monolayer organic 2D materials remains challenging. Herein, the fabrication of a novel organic–inorganic bilayer vdWh by combining π-conjugated 2D coordination polymer (2DCP, i.e., Cu3BHT, BHT = benzenehexathiol) with graphene is reported. Monolayer Cu3BHT with detectable µm2-scale uniformity and atomic flatness is synthesized using on-water surface chemistry. A combination of diffraction and imaging techniques enables the determination of the crystal structure of monolayer Cu3BHT with atomic precision. Leveraging the strong interlayer coupling, Cu3BHT-graphene vdWh exhibits highly efficient photoinduced interlayer charge separation with a net electron transfer efficiency of up to 34% from Cu3BHT to graphene, superior to those of reported bilayer 2D vdWhs and molecular-graphene vdWhs. This study unveils the potential for developing novel 2DCP-based vdWhs with intriguing physical properties.

Original languageEnglish
Article number2311454
JournalAdvanced Materials
Volume36
Issue number21
Early online date21 Feb 2024
DOIs
Publication statusPublished - 23 May 2024

Keywords

  • 2D van der Waals heterostructures
  • charge separation
  • conductive 2D coordination polymers
  • interlayer coupling

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