Defect-Mediated Phase Transformation in Anisotropic Two-Dimensional PdSe2 Crystals for Seamless Electrical Contacts

doi:https://doi.org/10.1021/jacs.9b02593

Title: Defect-Mediated Phase Transformation in Anisotropic Two-Dimensional PdSe ₂ Crystals for Seamless Electrical Contacts

Abstract

The failure to achieve stable Ohmic contacts in two-dimensional material devices currently limits their promised performance and integration. Here we demonstrate that a phase transformation in a region of a layered semiconductor, PdSe ₂, can form a contiguous metallic Pd ₁₇Se ₁₅ phase, leading to the formation of seamless Ohmic contacts for field-effect transistors. This phase transition is driven by defects created by exposure to an argon plasma. Cross-sectional scanning transmission electron microscopy is combined with theoretical calculations to elucidate how plasma-induced Se vacancies mediate the phase transformation. The resulting Pd ₁₇Se ₁₅ phase is stable and shares the same native chemical bonds with the original PdSe2 phase, thereby forming an atomically sharp Pd ₁₇Se ₁₅/PdSe ₂ interface. Furthermore, these Pd ₁₇Se ₁₅ contacts exhibit a low contact resistance of ~0.75 kΩ μm and Schottky barrier height of ~3.3 meV, enabling nearly a 20-fold increase of carrier mobility in PdSe ₂ transistors compared to that of traditional Ti/Au contacts. This finding opens new possibilities in the development of better electrical contacts for practical applications of 2D materials.

Authors:

Oyedele, Akinola ^[1];

^[2];

^[3]; Haglund, Amanda V. ^[4]; Gu, Yiyi ^[5];

^[2];

^[2]; Mandrus, David ^[1];

^[2]; Pantelides, Sokrates T. ^[3];

^[2];

^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Vanderbilt Univ., Nashville, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Chinese Academy of Sciences (CAS), Beijing (China)

Publication Date:: 2019-05-15

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Vanderbilt Univ., Nashville, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1530098

Alternate Identifier(s):: OSTI ID: 1597938

Grant/Contract Number:: AC05-00OR22725; FG02-09ER46554

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 141; Journal Issue: 22; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Oyedele, Akinola, Yang, Shize, Feng, Tianli, Haglund, Amanda V., Gu, Yiyi, Puretzky, Alexander A., Briggs, Dayrl P., Rouleau, Christopher M., Chisholm, Matthew F., Unocic, Raymond R., Mandrus, David, Meyer, III, Harry M., Pantelides, Sokrates T., Geohegan, David B., and Xiao, Kai. Defect-Mediated Phase Transformation in Anisotropic Two-Dimensional PdSe2 Crystals for Seamless Electrical Contacts.  United States: N. p., 2019. 
        Web.  doi:10.1021/jacs.9b02593.

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                    Oyedele, Akinola, Yang, Shize, Feng, Tianli, Haglund, Amanda V., Gu, Yiyi, Puretzky, Alexander A., Briggs, Dayrl P., Rouleau, Christopher M., Chisholm, Matthew F., Unocic, Raymond R., Mandrus, David, Meyer, III, Harry M., Pantelides, Sokrates T., Geohegan, David B., & Xiao, Kai. Defect-Mediated Phase Transformation in Anisotropic Two-Dimensional PdSe2 Crystals for Seamless Electrical Contacts.  United States.  https://doi.org/10.1021/jacs.9b02593

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                    Oyedele, Akinola, Yang, Shize, Feng, Tianli, Haglund, Amanda V., Gu, Yiyi, Puretzky, Alexander A., Briggs, Dayrl P., Rouleau, Christopher M., Chisholm, Matthew F., Unocic, Raymond R., Mandrus, David, Meyer, III, Harry M., Pantelides, Sokrates T., Geohegan, David B., and Xiao, Kai. Wed .  
        "Defect-Mediated Phase Transformation in Anisotropic Two-Dimensional PdSe2 Crystals for Seamless Electrical Contacts".  United States.  https://doi.org/10.1021/jacs.9b02593.  https://www.osti.gov/servlets/purl/1530098.

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@article{osti_1530098,

  title        = {Defect-Mediated Phase Transformation in Anisotropic Two-Dimensional PdSe2 Crystals for Seamless Electrical Contacts},

  author       = {Oyedele, Akinola and Yang, Shize and Feng, Tianli and Haglund, Amanda V. and Gu, Yiyi and Puretzky, Alexander A. and Briggs, Dayrl P. and Rouleau, Christopher M. and Chisholm, Matthew F. and Unocic, Raymond R. and Mandrus, David and Meyer, III, Harry M. and Pantelides, Sokrates T. and Geohegan, David B. and Xiao, Kai},

  abstractNote = {The failure to achieve stable Ohmic contacts in two-dimensional material devices currently limits their promised performance and integration. Here we demonstrate that a phase transformation in a region of a layered semiconductor, PdSe2, can form a contiguous metallic Pd17Se15 phase, leading to the formation of seamless Ohmic contacts for field-effect transistors. This phase transition is driven by defects created by exposure to an argon plasma. Cross-sectional scanning transmission electron microscopy is combined with theoretical calculations to elucidate how plasma-induced Se vacancies mediate the phase transformation. The resulting Pd17Se15 phase is stable and shares the same native chemical bonds with the original PdSe2 phase, thereby forming an atomically sharp Pd17Se15/PdSe2 interface. Furthermore, these Pd17Se15 contacts exhibit a low contact resistance of ~0.75 kΩ μm and Schottky barrier height of ~3.3 meV, enabling nearly a 20-fold increase of carrier mobility in PdSe2 transistors compared to that of traditional Ti/Au contacts. This finding opens new possibilities in the development of better electrical contacts for practical applications of 2D materials.},

  doi          = {10.1021/jacs.9b02593},

  url          = {https://www.osti.gov/biblio/1530098},
  journal      = {Journal of the American Chemical Society},

  issn         = {0002-7863},

  number       = 22,

  volume       = 141,

  place        = {United States},

  year         = {2019},

  month        = {5}

}

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Cited by: 11 works

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Works referencing / citing this record:

Recent Progress on 2D Noble‐Transition‐Metal Dichalcogenides
journal, October 2019

Pi, Lejing; Li, Liang; Liu, Kailang
Advanced Functional Materials, Vol. 29, Issue 51
https://doi.org/10.1002/adfm.201904932

Striated 2D Lattice with Sub‐nm 1D Etch Channels by Controlled Thermally Induced Phase Transformations of PdSe ₂
journal, September 2019

Ryu, Gyeong Hee; Zhu, Taishan; Chen, Jun
Advanced Materials, Vol. 31, Issue 46
https://doi.org/10.1002/adma.201904251

Laser-generated plasmas in length scales relevant for thin film growth and processing: simulation and experiment
journal, January 2019

Harris, S. B.; Paiste, J. H.; Holdsworth, T. J.
Journal of Physics D: Applied Physics, Vol. 53, Issue 1
https://doi.org/10.1088/1361-6463/ab4828

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Title: Defect-Mediated Phase Transformation in Anisotropic Two-Dimensional PdSe 2 Crystals for Seamless Electrical Contacts

Abstract

Citation Formats

Recent Progress on 2D Noble‐Transition‐Metal Dichalcogenides journal, October 2019

Striated 2D Lattice with Sub‐nm 1D Etch Channels by Controlled Thermally Induced Phase Transformations of PdSe 2 journal, September 2019

Laser-generated plasmas in length scales relevant for thin film growth and processing: simulation and experiment journal, January 2019

Title: Defect-Mediated Phase Transformation in Anisotropic Two-Dimensional PdSe ₂ Crystals for Seamless Electrical Contacts

Recent Progress on 2D Noble‐Transition‐Metal Dichalcogenides
journal, October 2019

Striated 2D Lattice with Sub‐nm 1D Etch Channels by Controlled Thermally Induced Phase Transformations of PdSe ₂
journal, September 2019

Laser-generated plasmas in length scales relevant for thin film growth and processing: simulation and experiment
journal, January 2019