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Title: PdSe 2: Pentagonal Two-Dimensional Layers with High Air Stability for Electronics

Most studied two-dimensional (2D) materials exhibit isotropic behavior due to high lattice symmetry; however, lower-symmetry 2D materials such as phosphorene and other elemental 2D materials exhibit very interesting anisotropic properties. In this work, we report the atomic structure, electronic properties, and vibrational modes of few-layered PdSe 2, exfoliated from bulk crystals, a pentagonal 2D layered noble transition metal dichalcogenide with a puckered morphology that is air-stable. Micro-absorption optical spectroscopy and first-principles calculations reveal a wide band gap variation in this material from ~0 (bulk) to ~1.3 eV (monolayer). The Raman active vibrational modes of PdSe 2 were identified using polarized Raman spectroscopy, and the strong interlayer interaction was revealed from the large thickness-dependent Raman peak shifts, agreeing with first-principles Raman simulations. Field-effect transistors made from the few-layer PdSe 2 display tunable ambipolar charge carrier conduction with a high electron apparent field-effect mobility of ~158 cm 2V -1s -1, indicating the promise of this anisotropic, air-stable, pentagonal 2D material for 2D electronics.
Authors:
 [1] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [2] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [4] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [7] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Virginia, Charlottesville, VA (United States)
  4. Nayang Technologal Univ. (Singapore)
  5. Univ. of Tennessee, Knoxville, TN (United States)
  6. Univ. of Virginia, Charlottesville, VA (United States)
  7. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 40; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Pentagonal; pucker; anisotropic; two-dimensional crystals; mobility
OSTI Identifier:
1394440

Oyedele, Akinola D., Yang, Shize, Liang, Liangbo, Puretzky, Alexander A., Wang, Kai, Zhang, Jingjie, Yu, Peng, Pudasaini, Pushpa R., Ghosh, Avik W., Liu, Zheng, Rouleau, Christopher M., Sumpter, Bobby G., Chisholm, Matthew F., Zhou, Wu, Rack, Philip D., Geohegan, David B., and Xiao, Kai. PdSe2: Pentagonal Two-Dimensional Layers with High Air Stability for Electronics. United States: N. p., Web. doi:10.1021/jacs.7b04865.
Oyedele, Akinola D., Yang, Shize, Liang, Liangbo, Puretzky, Alexander A., Wang, Kai, Zhang, Jingjie, Yu, Peng, Pudasaini, Pushpa R., Ghosh, Avik W., Liu, Zheng, Rouleau, Christopher M., Sumpter, Bobby G., Chisholm, Matthew F., Zhou, Wu, Rack, Philip D., Geohegan, David B., & Xiao, Kai. PdSe2: Pentagonal Two-Dimensional Layers with High Air Stability for Electronics. United States. doi:10.1021/jacs.7b04865.
Oyedele, Akinola D., Yang, Shize, Liang, Liangbo, Puretzky, Alexander A., Wang, Kai, Zhang, Jingjie, Yu, Peng, Pudasaini, Pushpa R., Ghosh, Avik W., Liu, Zheng, Rouleau, Christopher M., Sumpter, Bobby G., Chisholm, Matthew F., Zhou, Wu, Rack, Philip D., Geohegan, David B., and Xiao, Kai. 2017. "PdSe2: Pentagonal Two-Dimensional Layers with High Air Stability for Electronics". United States. doi:10.1021/jacs.7b04865. https://www.osti.gov/servlets/purl/1394440.
@article{osti_1394440,
title = {PdSe2: Pentagonal Two-Dimensional Layers with High Air Stability for Electronics},
author = {Oyedele, Akinola D. and Yang, Shize and Liang, Liangbo and Puretzky, Alexander A. and Wang, Kai and Zhang, Jingjie and Yu, Peng and Pudasaini, Pushpa R. and Ghosh, Avik W. and Liu, Zheng and Rouleau, Christopher M. and Sumpter, Bobby G. and Chisholm, Matthew F. and Zhou, Wu and Rack, Philip D. and Geohegan, David B. and Xiao, Kai},
abstractNote = {Most studied two-dimensional (2D) materials exhibit isotropic behavior due to high lattice symmetry; however, lower-symmetry 2D materials such as phosphorene and other elemental 2D materials exhibit very interesting anisotropic properties. In this work, we report the atomic structure, electronic properties, and vibrational modes of few-layered PdSe2, exfoliated from bulk crystals, a pentagonal 2D layered noble transition metal dichalcogenide with a puckered morphology that is air-stable. Micro-absorption optical spectroscopy and first-principles calculations reveal a wide band gap variation in this material from ~0 (bulk) to ~1.3 eV (monolayer). The Raman active vibrational modes of PdSe2 were identified using polarized Raman spectroscopy, and the strong interlayer interaction was revealed from the large thickness-dependent Raman peak shifts, agreeing with first-principles Raman simulations. Field-effect transistors made from the few-layer PdSe2 display tunable ambipolar charge carrier conduction with a high electron apparent field-effect mobility of ~158 cm2V-1s-1, indicating the promise of this anisotropic, air-stable, pentagonal 2D material for 2D electronics.},
doi = {10.1021/jacs.7b04865},
journal = {Journal of the American Chemical Society},
number = 40,
volume = 139,
place = {United States},
year = {2017},
month = {9}
}