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Title: Isoelectronic tungsten doping in monolayer MoSe 2 for carrier type modulation

Doping and alloying are effective ways to engineer the band structure and modulate the optoelectronic functionality of monolayer transition metal dichalcogenides (TMDs). In this work, we explore the synthesis and electronic properties of monolayer Mo 1-xW xSe 2 (0 < x < 0.18) alloys with almost 100% alloying degree. The isoelectronic substitutional doping of tungsten for molybdenum in the monolayer MoSe 2 is shown to suppress its intrinsically n-type conduction behavior, with p-type conduction gradually emerging to become dominant with increasing W concentration in the alloys. Atomic resolution Z-contrast electron microscopy show that W is shown to substitute directly for Mo without the introduction of noticeable vacancy or interstitial defects, however with randomly-distributed W-rich regions ~2 nm in diameter. Scanning tunneling microscopy/spectroscopy measurements reveal that these W-rich regions exhibit a local band structure with the valence band maximum (VBM) closer to the Fermi level as compared with the Mo-rich regions in the monolayer Mo 1-xW xSe 2 crystal. These localized upshifts of the VBM in the local band structure appear responsible for the overall p-type behavior observed for the monolayer Mo 1-xW xSe 2 crystals. Stacked monolayers of n-type MoSe 2 and p-type Mo 1-xW xSe 2 were demonstrated tomore » form atomically thin, vertically stacked p n homojunctions with gate-tunable characteristics, which appear useful for future optoelectronic applications. Lastly, these results indicate that alloying with isoelectronic dopant atoms appears to be an effective and advantageous alternate strategy to doping or alloying with electron donors or acceptors in two-dimensional TMDs.« less
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [3] ;  [4] ;  [4] ;  [1] ;  [1] ;  [1] ;  [4] ;  [1] ;  [1] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Escuela Politecnica Nacional, Quito (Ecuador)
  3. Pusan National Univ., Busan (South Korea)
  4. National Synchrotron Radiation Research Center (NSRRC), Hsinchu (Taiwan)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 28; Journal Issue: 37; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
OSTI Identifier:
1329120

Li, Xufan, Lin, Ming -Wei, Basile, Leonardo, Hus, Saban M., Puretzky, Alexander A., Lee, Jaekwang, Kuo, Yen -Chien, Chang, Lo -Yueh, Wang, Kai, Idrobo, Juan C., Li, An -Ping, Chen, Chia-Hao, Rouleau, Christopher M., Geohegan, David B., and Xiao, Kai. Isoelectronic tungsten doping in monolayer MoSe2 for carrier type modulation. United States: N. p., Web. doi:10.1002/adma.201601991.
Li, Xufan, Lin, Ming -Wei, Basile, Leonardo, Hus, Saban M., Puretzky, Alexander A., Lee, Jaekwang, Kuo, Yen -Chien, Chang, Lo -Yueh, Wang, Kai, Idrobo, Juan C., Li, An -Ping, Chen, Chia-Hao, Rouleau, Christopher M., Geohegan, David B., & Xiao, Kai. Isoelectronic tungsten doping in monolayer MoSe2 for carrier type modulation. United States. doi:10.1002/adma.201601991.
Li, Xufan, Lin, Ming -Wei, Basile, Leonardo, Hus, Saban M., Puretzky, Alexander A., Lee, Jaekwang, Kuo, Yen -Chien, Chang, Lo -Yueh, Wang, Kai, Idrobo, Juan C., Li, An -Ping, Chen, Chia-Hao, Rouleau, Christopher M., Geohegan, David B., and Xiao, Kai. 2016. "Isoelectronic tungsten doping in monolayer MoSe2 for carrier type modulation". United States. doi:10.1002/adma.201601991. https://www.osti.gov/servlets/purl/1329120.
@article{osti_1329120,
title = {Isoelectronic tungsten doping in monolayer MoSe2 for carrier type modulation},
author = {Li, Xufan and Lin, Ming -Wei and Basile, Leonardo and Hus, Saban M. and Puretzky, Alexander A. and Lee, Jaekwang and Kuo, Yen -Chien and Chang, Lo -Yueh and Wang, Kai and Idrobo, Juan C. and Li, An -Ping and Chen, Chia-Hao and Rouleau, Christopher M. and Geohegan, David B. and Xiao, Kai},
abstractNote = {Doping and alloying are effective ways to engineer the band structure and modulate the optoelectronic functionality of monolayer transition metal dichalcogenides (TMDs). In this work, we explore the synthesis and electronic properties of monolayer Mo1-xWxSe2 (0 < x < 0.18) alloys with almost 100% alloying degree. The isoelectronic substitutional doping of tungsten for molybdenum in the monolayer MoSe2 is shown to suppress its intrinsically n-type conduction behavior, with p-type conduction gradually emerging to become dominant with increasing W concentration in the alloys. Atomic resolution Z-contrast electron microscopy show that W is shown to substitute directly for Mo without the introduction of noticeable vacancy or interstitial defects, however with randomly-distributed W-rich regions ~2 nm in diameter. Scanning tunneling microscopy/spectroscopy measurements reveal that these W-rich regions exhibit a local band structure with the valence band maximum (VBM) closer to the Fermi level as compared with the Mo-rich regions in the monolayer Mo1-xWxSe2 crystal. These localized upshifts of the VBM in the local band structure appear responsible for the overall p-type behavior observed for the monolayer Mo1-xWxSe2 crystals. Stacked monolayers of n-type MoSe2 and p-type Mo1-xWxSe2 were demonstrated to form atomically thin, vertically stacked p n homojunctions with gate-tunable characteristics, which appear useful for future optoelectronic applications. Lastly, these results indicate that alloying with isoelectronic dopant atoms appears to be an effective and advantageous alternate strategy to doping or alloying with electron donors or acceptors in two-dimensional TMDs.},
doi = {10.1002/adma.201601991},
journal = {Advanced Materials},
number = 37,
volume = 28,
place = {United States},
year = {2016},
month = {7}
}

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