4.8 Article

Photophysics and Electronic Structure of Lateral Graphene/MoS2 and Metal/MoS2 Junctions

Journal

ACS NANO
Volume 14, Issue 12, Pages 16663-16671

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c02527

Keywords

photocurrent; graphene contacts; heterostructure; ARPES; Schottky barrier; molybdenum disulfide; first-principles calculations

Funding

  1. NSF CAREER [1453924]
  2. Swiss National Science Foundation [P300P2-171221]
  3. DOE Office of Science User Facility [DE-AC02-05CH11231]
  4. Alexander von Humboldt foundation
  5. German federal ministry of education and research
  6. National Science Foundation [DMREF-1729338, EFMA 1433378, EFMA 1433307]
  7. EXPEC Advanced Research Center, Petroleum Engineering and Development Department at Saudi Aramco
  8. Center for Low Energy Systems Technology (LEAST) - MARCO
  9. DARPA
  10. Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy [EXC 2089/1-390776260]
  11. U.S. DOE's National Nuclear Security Administration [DE-NA-0003525]

Ask authors/readers for more resources

Integration of semiconducting transition metal dichalcogenides (TMDs) into functional optoelectronic circuitries requires an understanding of the charge transfer across the interface between the TMD and the contacting material. Here, we use spatially resolved photocurrent microscopy to demonstrate electronic uniformity at the epitaxial graphene/molybdenum disulfide (EG/MoS2) interface. A 10x larger photocurrent is extracted at the EG/MoS2 interface when compared to the metal (Ti/Au)/MoS2 interface. This is supported by semi-local density functional theory (DFT), which predicts the Schottky barrier at the EG/MoS2 interface to be similar to 2x lower than that at Ti/MoS2. We provide a direct visualization of a 2D material Schottky barrier through combination of angle-resolved photoemission spectroscopy with spatial resolution selected to be similar to 300 nm (nano-ARPES) and DFT calculations. A bending of similar to 500 meV over a length scale of similar to 2-3 mu m in the valence band maximum of MoS2 is observed via nanoARPES. We explicate a correlation between experimental demonstration and theoretical predictions of barriers at graphene/TMD interfaces. Spatially resolved photocurrent mapping allows for directly visualizing the uniformity of built-in electric fields at heterostructure interfaces, providing a guide for microscopic engineering of charge transport across heterointerfaces. This simple probe-based technique also speaks directly to the 2D synthesis community to elucidate electronic uniformity at domain boundaries alongside morphological uniformity over large areas.

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