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Local Structure of Sulfur Vacancies on the Basal Plane of Monolayer MoS2

Journal Article · · ACS Nano
 [1];  [2];  [3];  [1];  [4];  [1];  [2];  [1];  [5];  [6];  [2];  [5]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  2. Stanford University, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States); Georgia Institute of Technology, Atlanta, GA (United States); University of Arizona, Tucson, AZ (United States)
  4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
+ Show Author Affiliations
We report the nature of the S-vacancy is central to controlling the electronic properties of monolayer MoS2. Understanding the geometric and electronic structures of the S-vacancy on the basal plane of monolayer MoS2 remains elusive. Here, operando S K-edge X-ray absorption spectroscopy shows the formation of clustered S-vacancies on the basal plane of monolayer MoS2 under reaction conditions (H2 atmosphere, 100–600 °C). First-principles calculations predict spectral fingerprints consistent with the experimental results. The Mo K-edge extended X-ray absorption fine structure shows the local structure as coordinatively unsaturated Mo with 4.1 ± 0.4 S atoms as nearest neighbors (above 400 °C in an H2 atmosphere). Conversely, the 6-fold Mo–Mo coordination in the crystal remains unchanged. Electrochemistry confirms similar active sites for hydrogen evolution. The identity of the S-vacancy defect on the basal plane of monolayer MoS2 is herein elucidated for applications in optoelectronics and catalysis.
Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
National Science Foundation (NSF); Seoul National University; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-05CH11231; AC02-76SF00515
OSTI ID:
1876003
Journal Information:
ACS Nano, Journal Name: ACS Nano Journal Issue: 4 Vol. 16; ISSN 1936-0851
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Figures / Tables (4)

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
DFT
X-ray absorption spectroscopy
hydrogen evolution reaction
monolayer molybdenum disulfide
operando
sulfur vacancy