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Title: Directed Atom-by-Atom Assembly of Dopants in Silicon

The ability to controllably position single atoms inside materials is key for the ultimate fabrication of devices with functionalities governed by atomic-scale properties. Single bismuth dopant atoms in silicon provide an ideal case study in view of proposals for single-dopant quantum bits. However, bismuth is the least soluble pnictogen in silicon, meaning that the dopant atoms tend to migrate out of position during sample growth. Here, we demonstrate epitaxial growth of thin silicon films doped with bismuth. We use atomic-resolution aberration-corrected imaging to view the as-grown dopant distribution and then to controllably position single dopants inside the film. Atomic-scale quantum-mechanical calculations corroborate the experimental findings. Finally, these results indicate that the scanning transmission electron microscope is of particular interest for assembling functional materials atom-by-atom because it offers both real-time monitoring and atom manipulation. Lastly, we envision electron-beam manipulation of atoms inside materials as an achievable route to controllable assembly of structures of individual dopants.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ;  [3] ;  [2] ; ORCiD logo [4] ;  [3] ; ORCiD logo [5] ; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Inst. for Functional Imaging of Materials
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Vanderbilt Univ., Nashville, TN (United States). Dept. of Physics and Astronomy
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Computational Sciences and Engineering Division
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy
Publication Date:
Grant/Contract Number:
AC05-00OR22725; FG02-09ER46554; AC02-05CH11231
Type:
Published Article
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 6; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; atomic positioning; bismuth in silicon; dopants; quantum computing; quantum materials; scanning transmission electron microscopy (STEM); single-atom manipulation
OSTI Identifier:
1457489
Alternate Identifier(s):
OSTI ID: 1458376

Hudak, Bethany M., Song, Jiaming, Sims, Hunter R., Troparevsky, M. Claudia, Humble, Travis S., Pantelides, Sokrates T., Snijders, Paul C., and Lupini, Andrew R.. Directed Atom-by-Atom Assembly of Dopants in Silicon. United States: N. p., Web. doi:10.1021/acsnano.8b02001.
Hudak, Bethany M., Song, Jiaming, Sims, Hunter R., Troparevsky, M. Claudia, Humble, Travis S., Pantelides, Sokrates T., Snijders, Paul C., & Lupini, Andrew R.. Directed Atom-by-Atom Assembly of Dopants in Silicon. United States. doi:10.1021/acsnano.8b02001.
Hudak, Bethany M., Song, Jiaming, Sims, Hunter R., Troparevsky, M. Claudia, Humble, Travis S., Pantelides, Sokrates T., Snijders, Paul C., and Lupini, Andrew R.. 2018. "Directed Atom-by-Atom Assembly of Dopants in Silicon". United States. doi:10.1021/acsnano.8b02001.
@article{osti_1457489,
title = {Directed Atom-by-Atom Assembly of Dopants in Silicon},
author = {Hudak, Bethany M. and Song, Jiaming and Sims, Hunter R. and Troparevsky, M. Claudia and Humble, Travis S. and Pantelides, Sokrates T. and Snijders, Paul C. and Lupini, Andrew R.},
abstractNote = {The ability to controllably position single atoms inside materials is key for the ultimate fabrication of devices with functionalities governed by atomic-scale properties. Single bismuth dopant atoms in silicon provide an ideal case study in view of proposals for single-dopant quantum bits. However, bismuth is the least soluble pnictogen in silicon, meaning that the dopant atoms tend to migrate out of position during sample growth. Here, we demonstrate epitaxial growth of thin silicon films doped with bismuth. We use atomic-resolution aberration-corrected imaging to view the as-grown dopant distribution and then to controllably position single dopants inside the film. Atomic-scale quantum-mechanical calculations corroborate the experimental findings. Finally, these results indicate that the scanning transmission electron microscope is of particular interest for assembling functional materials atom-by-atom because it offers both real-time monitoring and atom manipulation. Lastly, we envision electron-beam manipulation of atoms inside materials as an achievable route to controllable assembly of structures of individual dopants.},
doi = {10.1021/acsnano.8b02001},
journal = {ACS Nano},
number = 6,
volume = 12,
place = {United States},
year = {2018},
month = {5}
}