Abstract <p>Two-dimensional (2D) materials are emerging as promising semiconductors for ultrascaled FET devices in the post-Moore’s Law era. Achieving precise doping in these materials is critical for fine-tuning of their electronic properties. Similar to traditional semiconductors, such as Si or SiGe, doping concentration plays a key role in modulating performance. In this work, we demonstrate controlled synthesis of <i>n</i>-type rhenium (Re)-doped MoS<sub>2</sub> monolayers via atmospheric pressure chemical vapor deposition, achieving Re concentrations as low as 0.17&#xa0;at.%. Comprehensive spectroscopy and electron microscopy measurements identified distinct changes to the electronic and optical properties of MoS<sub>2</sub> resulting from Re doping. Low doping concentrations maintain the high crystallinity and flat surfaces of MoS<sub>2</sub>, while higher doping levels introduce midgap states, interband transitions, and enhanced spin–orbit coupling. Our scalable synthesis method offers a pathway to customizable 2D semiconductors for advanced electronics and optoelectronics, where doping concentration is key to engineering properties and performance.</p> Impact statement <p>The unique electronic and optical properties of two-dimensional (2D) transition--metal dichalcogenides (TMDs) have made them promising candidates for several applications, including sensing, photovoltaics, and semiconductor devices. Specific to semiconductors, widespread use and incorporation into modern device architectures requires fine-tuning of the materials’ electronic properties by introduction of dopants at dilute levels (&lt;10<sup>18</sup>&#xa0;dopants/cm<sup>3</sup>). Most reported studies on doping of TMDs focus on degenerate doping (&gt;10<sup>20</sup>&#xa0;dopants/cm<sup>3</sup>), which causes the Fermi level of the semiconductor to shift so far that metallic character is induced. In this work, we developed an <i>in</i>&#xa0;<i>situ</i> method for doping MoS<sub>2</sub> monolayers with rhenium during atmospheric pressure chemical vapor deposition, and demonstrate the ability to controllably dope MoS<sub>2</sub> with rhenium concentrations as low as 0.16 at.% (~10<sup>19</sup>&#xa0;dopants/cm<sup>3</sup>). The impacts of rhenium doping on the electronic band structure of MoS<sub>2</sub> have also been further studied using optical and electron spectroscopy techniques. The tunable synthesis method reported here will help pave the way for more controllable engineering of the properties of 2D materials, allowing for their integration into next-generation electronic and optoelectronic devices in the post-Moore’s Law era.</p> Graphical abstract <p></p>

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Tunable n-type rhenium doping in MoS2 monolayers by atmospheric chemical vapor deposition

  • Patrick John Hays,
  • Gigi Jackson,
  • Blake Povilus,
  • Mohammed Sayyad,
  • Jan Kopaczek,
  • Yunbo Ou,
  • Sui Yang,
  • Sandhya Susarla,
  • Seth Ariel Tongay

摘要

Abstract

Two-dimensional (2D) materials are emerging as promising semiconductors for ultrascaled FET devices in the post-Moore’s Law era. Achieving precise doping in these materials is critical for fine-tuning of their electronic properties. Similar to traditional semiconductors, such as Si or SiGe, doping concentration plays a key role in modulating performance. In this work, we demonstrate controlled synthesis of n-type rhenium (Re)-doped MoS2 monolayers via atmospheric pressure chemical vapor deposition, achieving Re concentrations as low as 0.17 at.%. Comprehensive spectroscopy and electron microscopy measurements identified distinct changes to the electronic and optical properties of MoS2 resulting from Re doping. Low doping concentrations maintain the high crystallinity and flat surfaces of MoS2, while higher doping levels introduce midgap states, interband transitions, and enhanced spin–orbit coupling. Our scalable synthesis method offers a pathway to customizable 2D semiconductors for advanced electronics and optoelectronics, where doping concentration is key to engineering properties and performance.

Impact statement

The unique electronic and optical properties of two-dimensional (2D) transition--metal dichalcogenides (TMDs) have made them promising candidates for several applications, including sensing, photovoltaics, and semiconductor devices. Specific to semiconductors, widespread use and incorporation into modern device architectures requires fine-tuning of the materials’ electronic properties by introduction of dopants at dilute levels (<1018 dopants/cm3). Most reported studies on doping of TMDs focus on degenerate doping (>1020 dopants/cm3), which causes the Fermi level of the semiconductor to shift so far that metallic character is induced. In this work, we developed an in situ method for doping MoS2 monolayers with rhenium during atmospheric pressure chemical vapor deposition, and demonstrate the ability to controllably dope MoS2 with rhenium concentrations as low as 0.16 at.% (~1019 dopants/cm3). The impacts of rhenium doping on the electronic band structure of MoS2 have also been further studied using optical and electron spectroscopy techniques. The tunable synthesis method reported here will help pave the way for more controllable engineering of the properties of 2D materials, allowing for their integration into next-generation electronic and optoelectronic devices in the post-Moore’s Law era.

Graphical abstract