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Title: Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies

Abstract

Large-scale assembly of individual atoms over smooth surfaces is difficult to achieve. A configuration of an atom reservoir, in which individual atoms can be readily extracted, may successfully address this challenge. In this work, we demonstrate that a liquid gold-silicon alloy established in classical vapor-liquid-solid growth can deposit ordered and three-dimensional rings of isolated gold atoms over silicon nanowire sidewalls. Here, we perform ab initio molecular dynamics simulation and unveil a surprising single atomic gold-catalyzed chemical etching of silicon. Experimental verification of this catalytic process in silicon nanowires yields dopant-dependent, massive and ordered 3D grooves with spacing down to similar to 5 nm. Finally, we use these grooves as self-labeled and ex situ markers to resolve several complex silicon growths, including the formation of nodes, kinks, scale-like interfaces, and curved backbones.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [1];  [4]; ORCiD logo [5];  [6];  [3];  [5];  [7];  [8]
  1. Univ. of Chicago, IL (United States). Dept. of Chemistry; Univ. of Chicago, IL (United States). James Franck Inst.
  2. Argonne National Lab. (ANL), Argonne, IL (United States). X-Ray Science Division
  3. Univ. of Illinois, Chicago, IL (United States). Research Resources Center
  4. Univ. of Chicago, IL (United States). Dept. of Chemistr
  5. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering; Northwestern Univ., Evanston, IL (United States). Center for Atom-Probe Tomography (NUCAPT)
  6. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  7. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials; Univ. of Chicago, IL (United States). Computation Inst.
  8. Univ. of Chicago, IL (United States). Dept. of Chemistry; Univ. of Chicago, IL (United States). James Franck Inst., and Inst. for Biophysical Dynamics
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF); National Institutes of Health (NIH); Alfred P. Sloan Foundation; US Department of the Navy, Office of Naval Research (ONR)
OSTI Identifier:
1425219
Grant/Contract Number:  
AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Synthesis and processing; Solid-state chemistry; Nanowires; Self-assembly

Citation Formats

Fang, Yin, Jiang, Yuanwen, Cherukara, Mathew J., Shi, Fengyuan, Koehler, Kelliann, Freyermuth, George, Isheim, Dieter, Narayanan, Badri, Nicholls, Alan W., Seidman, David N., Sankaranarayanan, Subramanian K. R. S., and Tian, Bozhi. Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies. United States: N. p., 2017. Web. doi:10.1038/s41467-017-02025-x.
Fang, Yin, Jiang, Yuanwen, Cherukara, Mathew J., Shi, Fengyuan, Koehler, Kelliann, Freyermuth, George, Isheim, Dieter, Narayanan, Badri, Nicholls, Alan W., Seidman, David N., Sankaranarayanan, Subramanian K. R. S., & Tian, Bozhi. Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies. United States. doi:10.1038/s41467-017-02025-x.
Fang, Yin, Jiang, Yuanwen, Cherukara, Mathew J., Shi, Fengyuan, Koehler, Kelliann, Freyermuth, George, Isheim, Dieter, Narayanan, Badri, Nicholls, Alan W., Seidman, David N., Sankaranarayanan, Subramanian K. R. S., and Tian, Bozhi. Fri . "Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies". United States. doi:10.1038/s41467-017-02025-x. https://www.osti.gov/servlets/purl/1425219.
@article{osti_1425219,
title = {Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies},
author = {Fang, Yin and Jiang, Yuanwen and Cherukara, Mathew J. and Shi, Fengyuan and Koehler, Kelliann and Freyermuth, George and Isheim, Dieter and Narayanan, Badri and Nicholls, Alan W. and Seidman, David N. and Sankaranarayanan, Subramanian K. R. S. and Tian, Bozhi},
abstractNote = {Large-scale assembly of individual atoms over smooth surfaces is difficult to achieve. A configuration of an atom reservoir, in which individual atoms can be readily extracted, may successfully address this challenge. In this work, we demonstrate that a liquid gold-silicon alloy established in classical vapor-liquid-solid growth can deposit ordered and three-dimensional rings of isolated gold atoms over silicon nanowire sidewalls. Here, we perform ab initio molecular dynamics simulation and unveil a surprising single atomic gold-catalyzed chemical etching of silicon. Experimental verification of this catalytic process in silicon nanowires yields dopant-dependent, massive and ordered 3D grooves with spacing down to similar to 5 nm. Finally, we use these grooves as self-labeled and ex situ markers to resolve several complex silicon growths, including the formation of nodes, kinks, scale-like interfaces, and curved backbones.},
doi = {10.1038/s41467-017-02025-x},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {12}
}

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