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Atomic structure and dynamics of self-limiting sub-nanometer pores in monolayer WS 2

DOI: 10.1021/acsnano.8b07051 DOI Help

Authors: Gyeong Hee Ryu (University of Oxford) , Arthur France-lanord (Massachusetts Institute of Technology) , Yi Wen (University of Oxford) , Si Zhou (University of Oxford) , Jeffrey C. Grossman (Massachusetts Institute of Technology) , Jamie H. Warner (University of Oxford)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Nano

State: Published (Approved)
Published: October 2018
Diamond Proposal Number(s): 16854

Abstract: We reveal a self-limiting mechanism during the formation of a specific type of circular nanopore in monolayer WS2 that limits its diameter to sub-nm. A single W atom vacancy (triangular nanopore) is transformed into the self-limiting nanopore (SLNP) through the atomic restructuring of S atoms around the area, reducing the number of dangling bonds at the nanopore edge by shifting them further in-plane with W–W bonding instead. Bond rotations in WS2 help accommodate the electron beam induced atomic loss and ensure the stability of the SLNP. The SLNP shows significant improvement in diameter stability during electron beam irradiation compared to other triangular nanopores in WS2 that typically continue to expand in diameter during atom loss. The atomic structure of these SLNPs is studied using aberration-corrected scanning transmission electron microscopy with an in situ heating holder, revealing that the SLNPs are mostly formed at a temperature of ∼500 °C, which is a balance between thermally activated S vacancy diffusion and sufficient S vacancy density to initiate local atomic reconstruction. At higher temperatures (i.e., 1000 °C), S vacancies quickly migrate away into long line vacancies, resulting in low S vacancy density and rapidly expanding holes generated at the edges of the line vacancies. At room temperature, S vacancy migration is low and vacancy density is very high, which limits atomic reconstruction, and instead many small holes open up. These results provide insights into the factors that lead to uniform sized nanopores in the sub-nm range in transition-metal dichalcogenides.

Journal Keywords: 2D materials; bond rotation; nanopore; scanning transmission electron microscopy; WS2

Subject Areas: Materials

Diamond Offline Facilities: Electron Physical Sciences Imaging Center (ePSIC)
Instruments: E02-JEM ARM 300CF