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Title: Correlating the three-dimensional atomic defects and electronic properties of two-dimensional transition metal dichalcogenides

Abstract

The electronic, optical and chemical properties of two-dimensional transition metal dichalcogenides strongly depend on their three-dimensional atomic structure and crystal defects. Using Re-doped MoS2 as a model system, here we present scanning atomic electron tomography as a method to determine three-dimensional atomic positions as well as positions of crystal defects such as dopants, vacancies and ripples with a precision down to 4 pm. We further measure the three-dimensional bond distortion and local strain tensor induced by single dopants. By directly offering these experimental three-dimensional atomic coordinates to density functional theory, we obtain more accurate electronic band structures than derived from conventional density functional theory calculations that relies on relaxed three-dimensional atomic coordinates. We anticipate that scanning atomic electron tomography not only will be generally applicable to determine the three-dimensional atomic coordinates of two-dimensional materials, but also will enable ab initio calculations to better predict the physical, chemical and electronic properties of these materials.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [4]; ORCiD logo [5]; ORCiD logo [1];  [3];  [1]; ORCiD logo [4]; ORCiD logo [6]; ORCiD logo [3]; ORCiD logo [1]
  1. Univ. of California, Los Angeles, CA (United States)
  2. Arizona State Univ., Tempe, AZ (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Harvard Univ., Cambridge, MA (United States)
  4. Rice Univ., Houston, TX (United States)
  5. Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of); Univ. of California, Los Angeles, CA (United States)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Univ. of California, Los Angeles, CA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Harvard Univ., Cambridge, MA (United States); Rice Univ., Houston, TX (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); Army Research Office (ARO); US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
1631219
Grant/Contract Number:  
SC0010378; DMR-1548924; DMR-1437263; FA9550-18-1-0072
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 19; Journal Issue: 8; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Tian, Xuezeng, Kim, Dennis S., Yang, Shize, Ciccarino, Christopher J., Gong, Yongji, Yang, Yongsoo, Yang, Yao, Duschatko, Blake, Yuan, Yakun, Ajayan, Pulickel M., Idrobo, Juan Carlos, Narang, Prineha, and Miao, Jianwei. Correlating the three-dimensional atomic defects and electronic properties of two-dimensional transition metal dichalcogenides. United States: N. p., 2020. Web. doi:10.1038/s41563-020-0636-5.
Tian, Xuezeng, Kim, Dennis S., Yang, Shize, Ciccarino, Christopher J., Gong, Yongji, Yang, Yongsoo, Yang, Yao, Duschatko, Blake, Yuan, Yakun, Ajayan, Pulickel M., Idrobo, Juan Carlos, Narang, Prineha, & Miao, Jianwei. Correlating the three-dimensional atomic defects and electronic properties of two-dimensional transition metal dichalcogenides. United States. doi:https://doi.org/10.1038/s41563-020-0636-5
Tian, Xuezeng, Kim, Dennis S., Yang, Shize, Ciccarino, Christopher J., Gong, Yongji, Yang, Yongsoo, Yang, Yao, Duschatko, Blake, Yuan, Yakun, Ajayan, Pulickel M., Idrobo, Juan Carlos, Narang, Prineha, and Miao, Jianwei. Mon . "Correlating the three-dimensional atomic defects and electronic properties of two-dimensional transition metal dichalcogenides". United States. doi:https://doi.org/10.1038/s41563-020-0636-5. https://www.osti.gov/servlets/purl/1631219.
@article{osti_1631219,
title = {Correlating the three-dimensional atomic defects and electronic properties of two-dimensional transition metal dichalcogenides},
author = {Tian, Xuezeng and Kim, Dennis S. and Yang, Shize and Ciccarino, Christopher J. and Gong, Yongji and Yang, Yongsoo and Yang, Yao and Duschatko, Blake and Yuan, Yakun and Ajayan, Pulickel M. and Idrobo, Juan Carlos and Narang, Prineha and Miao, Jianwei},
abstractNote = {The electronic, optical and chemical properties of two-dimensional transition metal dichalcogenides strongly depend on their three-dimensional atomic structure and crystal defects. Using Re-doped MoS2 as a model system, here we present scanning atomic electron tomography as a method to determine three-dimensional atomic positions as well as positions of crystal defects such as dopants, vacancies and ripples with a precision down to 4 pm. We further measure the three-dimensional bond distortion and local strain tensor induced by single dopants. By directly offering these experimental three-dimensional atomic coordinates to density functional theory, we obtain more accurate electronic band structures than derived from conventional density functional theory calculations that relies on relaxed three-dimensional atomic coordinates. We anticipate that scanning atomic electron tomography not only will be generally applicable to determine the three-dimensional atomic coordinates of two-dimensional materials, but also will enable ab initio calculations to better predict the physical, chemical and electronic properties of these materials.},
doi = {10.1038/s41563-020-0636-5},
journal = {Nature Materials},
number = 8,
volume = 19,
place = {United States},
year = {2020},
month = {3}
}

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