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Research Article

Self-inhibition effect of metal incorporation in nanoscaled semiconductors

View ORCID ProfileBin Zhu, View ORCID ProfileDing Yi, Yuxi Wang, Hongyu Sun, Gang Sha, Gong Zheng, View ORCID ProfileErik C. Garnett, View ORCID ProfileBozhi Tian, View ORCID ProfileFeng Ding, and Jia Zhu
  1. aNational Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093, People’s Republic of China;
  2. bJiangsu Key Laboratory of Artificial Functional Materials, Nanjing University, Nanjing 210093, People’s Republic of China;
  3. cCenter for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea;
  4. dDepartment of Physics, School of Science, Beijing Jiaotong University, Beijing 100044, People's Republic of China;
  5. eCenter for Nanophotonics, Fundamental Research on Matter Institute for Atomic and Molecular Physics (AMOLF), 1098 XG Amsterdam, The Netherlands;
  6. fHerbert Gleiter Institute of Nanoscience, Nanjing University of Science and Technology, Nanjing 210094, People's Republic of China;
  7. gMinistry of Industry and Information Technology (MIIT) Key Laboratory of Advanced Metallic and Intermetallic Materials Technology, Nanjing University of Science and Technology, Nanjing 210094, People's Republic of China;
  8. hDepartment of Chemistry, The University of Chicago, Chicago, IL 60637;
  9. iSchool of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea

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PNAS January 26, 2021 118 (4) e2010642118; https://doi.org/10.1073/pnas.2010642118
Bin Zhu
aNational Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093, People’s Republic of China;
bJiangsu Key Laboratory of Artificial Functional Materials, Nanjing University, Nanjing 210093, People’s Republic of China;
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Ding Yi
cCenter for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea;
dDepartment of Physics, School of Science, Beijing Jiaotong University, Beijing 100044, People's Republic of China;
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Yuxi Wang
aNational Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093, People’s Republic of China;
bJiangsu Key Laboratory of Artificial Functional Materials, Nanjing University, Nanjing 210093, People’s Republic of China;
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Hongyu Sun
eCenter for Nanophotonics, Fundamental Research on Matter Institute for Atomic and Molecular Physics (AMOLF), 1098 XG Amsterdam, The Netherlands;
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Gang Sha
fHerbert Gleiter Institute of Nanoscience, Nanjing University of Science and Technology, Nanjing 210094, People's Republic of China;
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Gong Zheng
fHerbert Gleiter Institute of Nanoscience, Nanjing University of Science and Technology, Nanjing 210094, People's Republic of China;
gMinistry of Industry and Information Technology (MIIT) Key Laboratory of Advanced Metallic and Intermetallic Materials Technology, Nanjing University of Science and Technology, Nanjing 210094, People's Republic of China;
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Erik C. Garnett
eCenter for Nanophotonics, Fundamental Research on Matter Institute for Atomic and Molecular Physics (AMOLF), 1098 XG Amsterdam, The Netherlands;
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  • ORCID record for Erik C. Garnett
Bozhi Tian
hDepartment of Chemistry, The University of Chicago, Chicago, IL 60637;
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Feng Ding
cCenter for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea;
iSchool of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
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  • For correspondence: f.ding@unist.ac.kr jiazhu@nju.edu.cn
Jia Zhu
aNational Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093, People’s Republic of China;
bJiangsu Key Laboratory of Artificial Functional Materials, Nanjing University, Nanjing 210093, People’s Republic of China;
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  • For correspondence: f.ding@unist.ac.kr jiazhu@nju.edu.cn
  1. Edited by Peter J. Rossky, Rice University, Houston, TX, and approved December 13, 2020 (received for review May 25, 2020)

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Significance

Understanding and controlling the incorporation of metal into nanoscaled semiconductor is foundational for semiconductor processing. Through theoretical calculation and experimental results, we reveal that the interstitial atoms in the Si lattice such as Mn can quickly diffuse out of Si nanowires conveniently, thus can achieve high purity of Si nanowires. This finding of self-inhibition effect not only provides understanding of impurity incorporation at nanoscale, but also provides an extra knob for rational catalyst designs of nanoscale building blocks, and fine-tuning their electrical, optical, and thermal properties for various applications.

Abstract

There has been a persistent effort to understand and control the incorporation of metal impurities in semiconductors at nanoscale, as it is important for semiconductor processing from growth, doping to making contact. Previously, the injection of metal atoms into nanoscaled semiconductor, with concentrations orders of magnitude higher than the equilibrium solid solubility, has been reported, which is often deemed to be detrimental. Here our theoretical exploration reveals that this colossal injection is because gold or aluminum atoms tend to substitute Si atoms and thus are not mobile in the lattice of Si. In contrast, the interstitial atoms in the Si lattice such as manganese (Mn) are expected to quickly diffuse out conveniently. Experimentally, we confirm the self-inhibition effect of Mn incorporation in nanoscaled silicon, as no metal atoms can be found in the body of silicon (below 1017 atoms per cm−3) by careful three-dimensional atomic mappings using highly focused ultraviolet-laser-assisted atom-probe tomography. As a result of self-inhibition effect of metal incorporation, the corresponding field-effect devices demonstrate superior transport properties. This finding of self-inhibition effect provides a missing piece for understanding the metal incorporation in semiconductor at nanoscale, which is critical not only for growing nanoscale building blocks, but also for designing and processing metal–semiconductor structures and fine-tuning their properties at nanoscale.

  • semiconductor nanowires
  • self-inhibition effect
  • metal catalyst
  • density-functional theory calculation

Footnotes

  • ↵1B.Z., D.Y., and Y.W. contributed equally to this work.

  • ↵2To whom correspondence may be addressed. Email: f.ding{at}unist.ac.kr or jiazhu{at}nju.edu.cn.
  • Author contributions: B.Z., F.D., and J.Z. designed research; B.Z., Y.W., H.S., and G.Z. performed research; B.Z., D.Y., G.S., E.C.G., B.T., and F.D. analyzed data; and B.Z., D.Y., F.D., and J.Z. wrote the paper.

  • The authors declare no competing interest.

  • This article is a PNAS Direct Submission.

  • This article contains supporting information online at https://www.pnas.org/lookup/suppl/doi:10.1073/pnas.2010642118/-/DCSupplemental.

Data Availability.

All study data are included in the article and/or SI Appendix.

Published under the PNAS license.

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Self-inhibition effect of metal incorporation in nanoscaled semiconductors
Bin Zhu, Ding Yi, Yuxi Wang, Hongyu Sun, Gang Sha, Gong Zheng, Erik C. Garnett, Bozhi Tian, Feng Ding, Jia Zhu
Proceedings of the National Academy of Sciences Jan 2021, 118 (4) e2010642118; DOI: 10.1073/pnas.2010642118

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Self-inhibition effect of metal incorporation in nanoscaled semiconductors
Bin Zhu, Ding Yi, Yuxi Wang, Hongyu Sun, Gang Sha, Gong Zheng, Erik C. Garnett, Bozhi Tian, Feng Ding, Jia Zhu
Proceedings of the National Academy of Sciences Jan 2021, 118 (4) e2010642118; DOI: 10.1073/pnas.2010642118
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