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Title: Visualizing nanoscale excitonic relaxation properties of disordered edges and grain boundaries in monolayer molybdenum disulfide

The ideal building blocks for atomically thin, flexible optoelectronic and catalytic devices are two-dimensional monolayer transition metal dichalcogenide semiconductors. Although challenging for two-dimensional systems, sub-diffraction optical microscopy provides a nanoscale material understanding that is vital for optimizing their optoelectronic properties. We use the ‘Campanile’ nano-optical probe to spectroscopically image exciton recombination within monolayer MoS2 with sub-wavelength resolution (60 nm), at the length scale relevant to many critical optoelectronic processes. Moreover, synthetic monolayer MoS2 is found to be composed of two distinct optoelectronic regions: an interior, locally ordered but mesoscopically heterogeneous two-dimensional quantum well and an unexpected ~300-nm wide, energetically disordered edge region. Further, grain boundaries are imaged with sufficient resolution to quantify local exciton-quenching phenomena, and complimentary nano-Auger microscopy reveals that the optically defective grain boundary and edge regions are sulfur deficient. In conclusion, the nanoscale structure–property relationships established here are critical for the interpretation of edge- and boundary-related phenomena and the development of next-generation two-dimensional optoelectronic devices.
Authors:
 [1] ;  [2] ;  [3] ;  [3] ;  [3] ;  [2] ;  [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [1] ;  [4] ;  [2] ;  [2] ;  [1] ;  [1] ;  [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Univ. of California, Berkeley, CA (United States)
  4. Univ. of California, Berkeley, CA (United States); Arizona State Univ., Tempe, AZ (United States)
Publication Date:
Grant/Contract Number:
AC02-05CH11231; DMR-1055938
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1256037
Alternate Identifier(s):
OSTI ID: 1407380

Bao, Wei, Borys, Nicholas J., Ko, Changhyun, Suh, Joonki, Fan, Wen, Thron, Andrew, Zhang, Yingjie, Buyanin, Alexander, Zhang, Jie, Cabrini, Stefano, Ashby, Paul D., Weber-Bargioni, Alexander, Tongay, Sefaattin, Aloni, Shaul, Ogletree, D. Frank, Wu, Junqiao, Salmeron, Miquel B., and Schuck, P. James. Visualizing nanoscale excitonic relaxation properties of disordered edges and grain boundaries in monolayer molybdenum disulfide. United States: N. p., Web. doi:10.1038/ncomms8993.
Bao, Wei, Borys, Nicholas J., Ko, Changhyun, Suh, Joonki, Fan, Wen, Thron, Andrew, Zhang, Yingjie, Buyanin, Alexander, Zhang, Jie, Cabrini, Stefano, Ashby, Paul D., Weber-Bargioni, Alexander, Tongay, Sefaattin, Aloni, Shaul, Ogletree, D. Frank, Wu, Junqiao, Salmeron, Miquel B., & Schuck, P. James. Visualizing nanoscale excitonic relaxation properties of disordered edges and grain boundaries in monolayer molybdenum disulfide. United States. doi:10.1038/ncomms8993.
Bao, Wei, Borys, Nicholas J., Ko, Changhyun, Suh, Joonki, Fan, Wen, Thron, Andrew, Zhang, Yingjie, Buyanin, Alexander, Zhang, Jie, Cabrini, Stefano, Ashby, Paul D., Weber-Bargioni, Alexander, Tongay, Sefaattin, Aloni, Shaul, Ogletree, D. Frank, Wu, Junqiao, Salmeron, Miquel B., and Schuck, P. James. 2015. "Visualizing nanoscale excitonic relaxation properties of disordered edges and grain boundaries in monolayer molybdenum disulfide". United States. doi:10.1038/ncomms8993. https://www.osti.gov/servlets/purl/1256037.
@article{osti_1256037,
title = {Visualizing nanoscale excitonic relaxation properties of disordered edges and grain boundaries in monolayer molybdenum disulfide},
author = {Bao, Wei and Borys, Nicholas J. and Ko, Changhyun and Suh, Joonki and Fan, Wen and Thron, Andrew and Zhang, Yingjie and Buyanin, Alexander and Zhang, Jie and Cabrini, Stefano and Ashby, Paul D. and Weber-Bargioni, Alexander and Tongay, Sefaattin and Aloni, Shaul and Ogletree, D. Frank and Wu, Junqiao and Salmeron, Miquel B. and Schuck, P. James},
abstractNote = {The ideal building blocks for atomically thin, flexible optoelectronic and catalytic devices are two-dimensional monolayer transition metal dichalcogenide semiconductors. Although challenging for two-dimensional systems, sub-diffraction optical microscopy provides a nanoscale material understanding that is vital for optimizing their optoelectronic properties. We use the ‘Campanile’ nano-optical probe to spectroscopically image exciton recombination within monolayer MoS2 with sub-wavelength resolution (60 nm), at the length scale relevant to many critical optoelectronic processes. Moreover, synthetic monolayer MoS2 is found to be composed of two distinct optoelectronic regions: an interior, locally ordered but mesoscopically heterogeneous two-dimensional quantum well and an unexpected ~300-nm wide, energetically disordered edge region. Further, grain boundaries are imaged with sufficient resolution to quantify local exciton-quenching phenomena, and complimentary nano-Auger microscopy reveals that the optically defective grain boundary and edge regions are sulfur deficient. In conclusion, the nanoscale structure–property relationships established here are critical for the interpretation of edge- and boundary-related phenomena and the development of next-generation two-dimensional optoelectronic devices.},
doi = {10.1038/ncomms8993},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {2015},
month = {8}
}

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