Super-resolved Optical Mapping of Reactive Sulfur-Vacancies in Two-Dimensional Transition Metal Dichalcogenides

Miao Zhang, Martina Lihter, Tzu Heng Chen, Michal Macha, Archith Rayabharam, Karla Banjac, Yanfei Zhao, Zhenyu Wang, Jing Zhang, Jean Comtet, Narayana R. Aluru, Magalí Lingenfelder, Andras Kis, Aleksandra Radenovic

Research output: Contribution to journalArticlepeer-review


Transition metal dichalcogenides (TMDs) represent a class of semiconducting two-dimensional (2D) materials with exciting properties. In particular, defects in 2D-TMDs and their molecular interactions with the environment can crucially affect their physical and chemical properties. However, mapping the spatial distribution and chemical reactivity of defects in liquid remains a challenge. Here, we demonstrate large area mapping of reactive sulfur-deficient defects in 2D-TMDs in aqueous solutions by coupling single-molecule localization microscopy with fluorescence labeling using thiol chemistry. Our method, reminiscent of PAINT strategies, relies on the specific binding of fluorescent probes hosting a thiol group to sulfur vacancies, allowing localization of the defects with an uncertainty down to 15 nm. Tuning the distance between the fluorophore and the docking thiol site allows us to control Föster resonance energy transfer (FRET) process and reveal grain boundaries and line defects due to the local irregular lattice structure. We further characterize the binding kinetics over a large range of pH conditions, evidencing the reversible adsorption of the thiol probes to the defects with a subsequent transitioning to irreversible binding in basic conditions. Our methodology provides a simple and fast alternative for large-scale mapping of nonradiative defects in 2D materials and can be used for in situ and spatially resolved monitoring of the interaction between chemical agents and defects in 2D materials that has general implications for defect engineering in aqueous condition.

Original languageEnglish (US)
Pages (from-to)7168-7178
Number of pages11
JournalACS Nano
Issue number4
StatePublished - Apr 27 2021


  • 2D materials
  • defects
  • interface
  • sulfur vacancy
  • super-resolution
  • thiol chemistry

ASJC Scopus subject areas

  • General Materials Science
  • General Engineering
  • General Physics and Astronomy


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