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Thickness-Independent Semiconducting-to-Metallic Conversion in Wafer-Scale Two-Dimensional PtSe2 Layers by Plasma-Driven Chalcogen Defect Engineering.

Publication ,  Journal Article
Shawkat, MS; Gil, J; Han, SS; Ko, T-J; Wang, M; Dev, D; Kwon, J; Lee, G-H; Oh, KH; Chung, H-S; Roy, T; Jung, Y; Jung, Y
Published in: ACS applied materials & interfaces
March 2020

Platinum diselenide (PtSe2) is an emerging class of two-dimensional (2D) transition-metal dichalcogenide (TMD) crystals recently gaining substantial interest, owing to its extraordinary properties absent in conventional 2D TMD layers. Most interestingly, it exhibits a thickness-dependent semiconducting-to-metallic transition, i.e., thick 2D PtSe2 layers, which are intrinsically metallic, become semiconducting with their thickness reduced below a certain point. Realizing both semiconducting and metallic phases within identical 2D PtSe2 layers in a spatially well-controlled manner offers unprecedented opportunities toward atomically thin tailored electronic junctions, unattainable with conventional materials. In this study, beyond this thickness-dependent intrinsic semiconducting-to-metallic transition of 2D PtSe2 layers, we demonstrate that controlled plasma irradiation can "externally" achieve such tunable carrier transports. We grew wafer-scale very thin (a few nm) 2D PtSe2 layers by a chemical vapor deposition (CVD) method and confirmed their intrinsic semiconducting properties. We then irradiated the material with argon (Ar) plasma, which was intended to make it more semiconducting by thickness reduction. Surprisingly, we discovered a reversed transition of semiconducting to metallic, which is opposite to the prediction concerning their intrinsic thickness-dependent carrier transports. Through extensive structural and chemical characterization, we identified that the plasma irradiation introduces a large concentration of near-atomic defects and selenium (Se) vacancies in initially stoichiometric 2D PtSe2 layers. Furthermore, we performed density functional theory (DFT) calculations and clarified that the band-gap energy of such defective 2D PtSe2 layers gradually decreases with increasing defect concentration and dimensions, accompanying a large number of midgap energy states. This corroborative experimental and theoretical study decisively verifies the fundamental mechanism for this externally controlled semiconducting-to-metallic transition in large-area CVD-grown 2D PtSe2 layers, greatly broadening their versatility for futuristic electronics.

Duke Scholars

Published In

ACS applied materials & interfaces

DOI

EISSN

1944-8252

ISSN

1944-8244

Publication Date

March 2020

Volume

12

Issue

12

Start / End Page

14341 / 14351

Related Subject Headings

  • Nanoscience & Nanotechnology
  • 51 Physical sciences
  • 40 Engineering
  • 34 Chemical sciences
  • 09 Engineering
  • 03 Chemical Sciences
 

Citation

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Shawkat, M. S., Gil, J., Han, S. S., Ko, T.-J., Wang, M., Dev, D., … Jung, Y. (2020). Thickness-Independent Semiconducting-to-Metallic Conversion in Wafer-Scale Two-Dimensional PtSe2 Layers by Plasma-Driven Chalcogen Defect Engineering. ACS Applied Materials & Interfaces, 12(12), 14341–14351. https://doi.org/10.1021/acsami.0c00116
Shawkat, Mashiyat Sumaiya, Jaeyoung Gil, Sang Sub Han, Tae-Jun Ko, Mengjing Wang, Durjoy Dev, Junyoung Kwon, et al. “Thickness-Independent Semiconducting-to-Metallic Conversion in Wafer-Scale Two-Dimensional PtSe2 Layers by Plasma-Driven Chalcogen Defect Engineering.ACS Applied Materials & Interfaces 12, no. 12 (March 2020): 14341–51. https://doi.org/10.1021/acsami.0c00116.
Shawkat MS, Gil J, Han SS, Ko T-J, Wang M, Dev D, et al. Thickness-Independent Semiconducting-to-Metallic Conversion in Wafer-Scale Two-Dimensional PtSe2 Layers by Plasma-Driven Chalcogen Defect Engineering. ACS applied materials & interfaces. 2020 Mar;12(12):14341–51.
Shawkat, Mashiyat Sumaiya, et al. “Thickness-Independent Semiconducting-to-Metallic Conversion in Wafer-Scale Two-Dimensional PtSe2 Layers by Plasma-Driven Chalcogen Defect Engineering.ACS Applied Materials & Interfaces, vol. 12, no. 12, Mar. 2020, pp. 14341–51. Epmc, doi:10.1021/acsami.0c00116.
Shawkat MS, Gil J, Han SS, Ko T-J, Wang M, Dev D, Kwon J, Lee G-H, Oh KH, Chung H-S, Roy T, Jung Y. Thickness-Independent Semiconducting-to-Metallic Conversion in Wafer-Scale Two-Dimensional PtSe2 Layers by Plasma-Driven Chalcogen Defect Engineering. ACS applied materials & interfaces. 2020 Mar;12(12):14341–14351.
Journal cover image

Published In

ACS applied materials & interfaces

DOI

EISSN

1944-8252

ISSN

1944-8244

Publication Date

March 2020

Volume

12

Issue

12

Start / End Page

14341 / 14351

Related Subject Headings

  • Nanoscience & Nanotechnology
  • 51 Physical sciences
  • 40 Engineering
  • 34 Chemical sciences
  • 09 Engineering
  • 03 Chemical Sciences