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A proposed simulation method for directed self-assembly of nanographene

A methodology for predictive kinetic self-assembly modeling of bottom-up chemical synthesis of nanographene is proposed. The method maintains physical transparency in using a novel array format to efficiently store molecule information and by using array operations to determine reaction possibilitie...

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Autores principales: Geraets, J A, Baldwin, J P C, Twarock, R, Hancock, Y
Formato: Online Artículo Texto
Lenguaje:English
Publicado: IOP Publishing 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5802380/
https://www.ncbi.nlm.nih.gov/pubmed/28653962
http://dx.doi.org/10.1088/1361-648X/aa7c0b
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author Geraets, J A
Baldwin, J P C
Twarock, R
Hancock, Y
author_facet Geraets, J A
Baldwin, J P C
Twarock, R
Hancock, Y
author_sort Geraets, J A
collection PubMed
description A methodology for predictive kinetic self-assembly modeling of bottom-up chemical synthesis of nanographene is proposed. The method maintains physical transparency in using a novel array format to efficiently store molecule information and by using array operations to determine reaction possibilities. Within a minimal model approach, the parameter space for the bond activation energies (i.e. molecule functionalization) at fixed reaction temperature and initial molecule concentrations is explored. Directed self-assembly of nanographene from functionalized tetrabenzanthracene and benzene is studied with regions in the activation energy phase-space showing length-to-width ratio tunability. The degree of defects and reaction reproducibility in the simulations is also determined, with the rate of functionalized benzene addition providing additional control of the dimension and quality of the nanographene. Comparison of the reaction energetics to available density functional theory data suggests the synthesis may be experimentally tenable using aryl-halide cross-coupling and noble metal surface-assisted catalysis. With full access to the intermediate reaction network and with dynamic coupling to density functional theory-informed tight-binding simulation, the method is proposed as a computationally efficient means towards detailed simulation-driven design of new nanographene systems.
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spelling pubmed-58023802018-06-11 A proposed simulation method for directed self-assembly of nanographene Geraets, J A Baldwin, J P C Twarock, R Hancock, Y J Phys Condens Matter Paper A methodology for predictive kinetic self-assembly modeling of bottom-up chemical synthesis of nanographene is proposed. The method maintains physical transparency in using a novel array format to efficiently store molecule information and by using array operations to determine reaction possibilities. Within a minimal model approach, the parameter space for the bond activation energies (i.e. molecule functionalization) at fixed reaction temperature and initial molecule concentrations is explored. Directed self-assembly of nanographene from functionalized tetrabenzanthracene and benzene is studied with regions in the activation energy phase-space showing length-to-width ratio tunability. The degree of defects and reaction reproducibility in the simulations is also determined, with the rate of functionalized benzene addition providing additional control of the dimension and quality of the nanographene. Comparison of the reaction energetics to available density functional theory data suggests the synthesis may be experimentally tenable using aryl-halide cross-coupling and noble metal surface-assisted catalysis. With full access to the intermediate reaction network and with dynamic coupling to density functional theory-informed tight-binding simulation, the method is proposed as a computationally efficient means towards detailed simulation-driven design of new nanographene systems. IOP Publishing 2017-09-06 2017-08-01 /pmc/articles/PMC5802380/ /pubmed/28653962 http://dx.doi.org/10.1088/1361-648X/aa7c0b Text en © 2017 IOP Publishing Ltd http://creativecommons.org/licenses/by/3.0/ Original content from this work may be used under the terms of the Creative Commons Attribution 3.0 licence (http://creativecommons.org/licenses/by/3.0) . Any further distribution of this work must maintain attribution to the author(s) and the title of the work, journal citation and DOI.
spellingShingle Paper
Geraets, J A
Baldwin, J P C
Twarock, R
Hancock, Y
A proposed simulation method for directed self-assembly of nanographene
title A proposed simulation method for directed self-assembly of nanographene
title_full A proposed simulation method for directed self-assembly of nanographene
title_fullStr A proposed simulation method for directed self-assembly of nanographene
title_full_unstemmed A proposed simulation method for directed self-assembly of nanographene
title_short A proposed simulation method for directed self-assembly of nanographene
title_sort proposed simulation method for directed self-assembly of nanographene
topic Paper
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5802380/
https://www.ncbi.nlm.nih.gov/pubmed/28653962
http://dx.doi.org/10.1088/1361-648X/aa7c0b
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