Strain-Induced asymmetry and on-site dynamics of silicon defects in graphene

Ondrej Dyck; Feng Bao; Maxim Ziatdinov; Ali Yousefzadi Nobakht; Kody Law; Artem Maksov; Bobby G. Sumpter; Richard Archibald; Stephen Jesse; Sergei V. Kalinin; David B. Lingerfelt

doi:10.1016/j.cartre.2022.100189

Strain-Induced asymmetry and on-site dynamics of silicon defects in graphene

Ondrej Dyck, Feng Bao, Maxim Ziatdinov, Ali Yousefzadi Nobakht, Kody Law, Artem Maksov, Bobby G. Sumpter, Richard Archibald, Stephen Jesse, Sergei V. Kalinin, David B. Lingerfelt

Research output: Contribution to journal › Article › peer-review

1 Scopus citations

Abstract

In the last decade, the atomically-focused electron beams utilized in scanning transmission electron microscopes (STEMs) have been shown to induce a broad set of local structural transformations in materials, opening pathways for directing material synthesis and modification atom-by-atom. The mechanisms underlying these transformations remain largely unknown, due to the intractability of modeling the myriad of reaction pathways that can be accessed through high-energy electron scattering. The information on materials’ structure and dynamics that can be extracted from STEM images is similarly left underexplored. Here, we report the observation of anomalous on-site dynamics of individual silicon impurity atoms in graphene during STEM imaging. Density functional theory-based structural optimizations of anisotropically-strained molecular nanographenes reveal two distinct (but nearly degenerate) stable structures for four-fold coordinated silicon impurities, where interconversion between the two structures manifests slight changes of the silicon position within the lattice site. Implications for defect-based strain engineering in graphene are discussed.

Original language	English
Article number	100189
Journal	Carbon Trends
Volume	9
DOIs	https://doi.org/10.1016/j.cartre.2022.100189
State	Published - Oct 2022

Funding

The electron microscopy work was supported by the U.S. Department of Energy, Office of Materials Science and Engineering, Basic Energy Sciences (S.V.K. O.D, S.J.) and was performed at Oak Ridge National Laboratory's Center for Nanophase Materials Sciences (CNMS), a US DOE Office of Science User Facility. Theory-based analysis and simulations were supported by CNMS (M.Z. D.B.L. B.G.S). We would like to acknowledge the support by the Scientific Discovery through Advanced Computing (SciDAC) funded by U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research through FASTMath Institutes (R.A. F.B.) and partial support by U.S. National Science Foundation under contract DMS-1720222 (F.B.). This work was also supported by The Alan Turing Institute under the EPSRC grant EP/N510129/1 (K.L. ). A.M. acknowledges fellowship support from the UT/ORNL Bredesen Center for Interdisciplinary Research and Graduate Education. A.Y.N. would like to acknowledge Dr. S. Shin for his advice and support in Nanoheat research lab at UTK. This work also used the Extreme Science and Engineering Discovery Environment (XSEDE) through allocation TG-DMR110037, as well as resources of the Compute and Data Environment for Science (CADES) at the Oak Ridge National Laboratory. The electron microscopy work was supported by the U.S. Department of Energy, Office of Materials Science and Engineering, Basic Energy Sciences (S.V.K., O.D, S.J.) and was performed at Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences (CNMS), a US DOE Office of Science User Facility. Theory-based analysis and simulations were supported by CNMS (M.Z., D.B.L., B.G.S). We would like to acknowledge the support by the Scientific Discovery through Advanced Computing (SciDAC) funded by U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research through FASTMath Institutes (R.A., F.B.) and partial support by U.S. National Science Foundation under contract DMS-1720222 (F.B.). This work was also supported by The Alan Turing Institute under the EPSRC grant EP/N510129/1 (K.L. ). A.M. acknowledges fellowship support from the UT/ORNL Bredesen Center for Interdisciplinary Research and Graduate Education. A.Y.N. would like to acknowledge Dr. S. Shin for his advice and support in Nanoheat research lab at UTK. This work also used the Extreme Science and Engineering Discovery Environment (XSEDE) through allocation TG-DMR110037, as well as resources of the Compute and Data Environment for Science (CADES) at the Oak Ridge National Laboratory.

Funders	Funder number
CADES
CNMS
Data Environment for Science
FASTMath Institutes
Oak Ridge National Laboratory
Oak Ridge National Laboratory
Office of Materials Science and Engineering
UT/ORNL	TG-DMR110037
National Science Foundation	DMS-1720222
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Advanced Scientific Computing Research
Oak Ridge National Laboratory
Alan Turing Institute
Engineering and Physical Sciences Research Council	EP/N510129/1

Keywords

Defect dynamics
Defect microanalysis
On-site asymmetry
Strain engineering
Strain-induced phenomena
Symmetry breaking

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10.1016/j.cartre.2022.100189

Cite this

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title = "Strain-Induced asymmetry and on-site dynamics of silicon defects in graphene",

abstract = "In the last decade, the atomically-focused electron beams utilized in scanning transmission electron microscopes (STEMs) have been shown to induce a broad set of local structural transformations in materials, opening pathways for directing material synthesis and modification atom-by-atom. The mechanisms underlying these transformations remain largely unknown, due to the intractability of modeling the myriad of reaction pathways that can be accessed through high-energy electron scattering. The information on materials{\textquoteright} structure and dynamics that can be extracted from STEM images is similarly left underexplored. Here, we report the observation of anomalous on-site dynamics of individual silicon impurity atoms in graphene during STEM imaging. Density functional theory-based structural optimizations of anisotropically-strained molecular nanographenes reveal two distinct (but nearly degenerate) stable structures for four-fold coordinated silicon impurities, where interconversion between the two structures manifests slight changes of the silicon position within the lattice site. Implications for defect-based strain engineering in graphene are discussed.",

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doi = "10.1016/j.cartre.2022.100189",

language = "English",

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AU - Bao, Feng

AU - Ziatdinov, Maxim

AU - Nobakht, Ali Yousefzadi

AU - Law, Kody

AU - Maksov, Artem

AU - Sumpter, Bobby G.

AU - Archibald, Richard

AU - Jesse, Stephen

AU - Kalinin, Sergei V.

AU - Lingerfelt, David B.

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N2 - In the last decade, the atomically-focused electron beams utilized in scanning transmission electron microscopes (STEMs) have been shown to induce a broad set of local structural transformations in materials, opening pathways for directing material synthesis and modification atom-by-atom. The mechanisms underlying these transformations remain largely unknown, due to the intractability of modeling the myriad of reaction pathways that can be accessed through high-energy electron scattering. The information on materials’ structure and dynamics that can be extracted from STEM images is similarly left underexplored. Here, we report the observation of anomalous on-site dynamics of individual silicon impurity atoms in graphene during STEM imaging. Density functional theory-based structural optimizations of anisotropically-strained molecular nanographenes reveal two distinct (but nearly degenerate) stable structures for four-fold coordinated silicon impurities, where interconversion between the two structures manifests slight changes of the silicon position within the lattice site. Implications for defect-based strain engineering in graphene are discussed.

AB - In the last decade, the atomically-focused electron beams utilized in scanning transmission electron microscopes (STEMs) have been shown to induce a broad set of local structural transformations in materials, opening pathways for directing material synthesis and modification atom-by-atom. The mechanisms underlying these transformations remain largely unknown, due to the intractability of modeling the myriad of reaction pathways that can be accessed through high-energy electron scattering. The information on materials’ structure and dynamics that can be extracted from STEM images is similarly left underexplored. Here, we report the observation of anomalous on-site dynamics of individual silicon impurity atoms in graphene during STEM imaging. Density functional theory-based structural optimizations of anisotropically-strained molecular nanographenes reveal two distinct (but nearly degenerate) stable structures for four-fold coordinated silicon impurities, where interconversion between the two structures manifests slight changes of the silicon position within the lattice site. Implications for defect-based strain engineering in graphene are discussed.

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KW - Defect microanalysis

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Strain-Induced asymmetry and on-site dynamics of silicon defects in graphene

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Keywords

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