Quasi-Van der Waals Epitaxial Growth of γ′-GaSe Nanometer-Thick Films on GaAs(111)B Substrates

GaSe is an important member of the post-transition-metal chalcogenide family and is an emerging two-dimensional (2D) semiconductor material. Because it is a van der Waals material, it can be fabricated into atomic-scale ultrathin films, making it suitable for the preparation of compact, heterostructure devices. In addition, GaSe possesses unusual optical and electronic properties, such as a shift from an indirect-bandgap single-layer film to a direct-bandgap bulk material, rare intrinsic p-type conduction, and nonlinear optical behaviors. These properties make GaSe an appealing candidate for the fabrication of field-effect transistors, photodetectors, and photovoltaics. However, the wafer-scale production of pure GaSe single-crystal thin films remains challenging. This study develops an approach for the direct growth of nanometer-thick GaSe films on GaAs substrates by using molecular beam epitaxy. It yields smooth thin GaSe films with a rare γ′-polymorph. We analyze the formation mechanism of γ′-GaSe using density-functional theory and speculate that it is stabilized by Ga vacancies since the formation enthalpy of γ′-GaSe tends to become lower than that of other polymorphs when the Ga vacancy concentration increases. Finally, we investigate the growth conditions of GaSe, providing valuable insights for exploring 2D/three-dimensional (3D) quasi-van der Waals epitaxial growth.

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Work Title Quasi-Van der Waals Epitaxial Growth of γ′-GaSe Nanometer-Thick Films on GaAs(111)B Substrates
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Open Access
Creators
  1. Mingyu Yu
  2. Sahani Amaya Iddawela
  3. Jiayang Wang
  4. Maria Hilse
  5. Jessica L. Thompson
  6. Danielle Reifsnyder Hickey
  7. Susan B. Sinnott
  8. Stephanie Law
License CC BY-NC-ND 4.0 (Attribution-NonCommercial-NoDerivatives)
Work Type Article
Publisher
  1. ACS Nano
Publication Date July 2, 2024
Publisher Identifier (DOI)
  1. https://doi.org/10.1021/acsnano.4c04194
Related URLs
Deposited November 25, 2024

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Version 1
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  • Created
  • Updated
  • Added Creator Mingyu Yu
  • Added Creator Sahani Amaya Iddawela
  • Added Creator Jiayang Wang
  • Added Creator Maria Hilse
  • Added Creator Jessica L. Thompson
  • Added Creator Danielle Reifsnyder Hickey
  • Added Creator Susan B. Sinnott
  • Added Creator Stephanie Law
  • Updated Work Title, Publisher, Publisher Identifier (DOI), and 3 more Show Changes
    Work Title
    • Quasi-van der Waals Epitaxial Growth of γ'-GaSe Thin Films on GaAs(111)B Substrates
    • Quasi-Van der Waals Epitaxial Growth of γ-GaSe Nanometer-Thick Films on GaAs(111)B Substrates
    Publisher
    • ACS Nano
    Publisher Identifier (DOI)
    • https://doi.org/10.1021/acsnano.4c04194
    Related URLs
    • http://arxiv.org/pdf/2403.12265
    Description
    • <p>GaSe is an important member of the post-transition-metal chalcogenide family and is an emerging two-dimensional (2D) semiconductor material. Because it is a van der Waals material, it can be fabricated into atomic-scale ultrathin films, making it suitable for the preparation of compact, heterostructure devices. In addition, GaSe possesses unusual optical and electronic properties, such as a shift from an indirect-bandgap single-layer film to a direct-bandgap bulk material, rare intrinsic p-type conduction, and nonlinear optical behaviors. These properties make GaSe an appealing candidate for the fabrication of field-effect transistors, photodetectors, and photovoltaics. However, the wafer-scale production of pure GaSe single-crystal thin films remains challenging. This study develops an approach for the direct growth of nanometer-thick GaSe films on GaAs substrates by using molecular beam epitaxy. It yields smooth thin GaSe films with a rare γ′-polymorph. We analyze the formation mechanism of γ′-GaSe using density-functional theory and speculate that it is stabilized by Ga vacancies since the formation enthalpy of γ′-GaSe tends to become lower than that of other polymorphs when the Ga vacancy concentration increases. Finally, we investigate the growth conditions of GaSe, providing valuable insights for exploring 2D/three-dimensional (3D) quasi-van der Waals epitaxial growth.</p>
    Publication Date
    • 2024-07-02
  • Updated
  • Updated
  • Updated Creator Mingyu Yu
  • Updated Creator Sahani Amaya Iddawela
  • Updated Creator Jiayang Wang
  • Updated Creator Maria Hilse
  • Updated Creator Jessica L. Thompson
  • Updated Creator Danielle Reifsnyder Hickey
  • Updated Creator Susan B. Sinnott
  • Updated Creator Stephanie Law
  • Added main_SI.pdf
  • Updated License Show Changes
    License
    • https://creativecommons.org/licenses/by-nc-nd/4.0/
  • Published
  • Updated