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Gating of Quantum Interference in Molecular Junctions by Heteroatom Substitution
To guide the choice of future synthetic targets for single‐molecule electronics, qualitative design rules are needed, which describe the effect of modifying chemical structure. Here the effect of heteroatom substitution on destructive quantum interference (QI) in single‐molecule junctions is, for th...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
John Wiley and Sons Inc.
2016
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5396325/ https://www.ncbi.nlm.nih.gov/pubmed/27897363 http://dx.doi.org/10.1002/anie.201609051 |
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author | Liu, Xunshan Sangtarash, Sara Reber, David Zhang, Dan Sadeghi, Hatef Shi, Jia Xiao, Zong‐Yuan Hong, Wenjing Lambert, Colin J. Liu, Shi‐Xia |
author_facet | Liu, Xunshan Sangtarash, Sara Reber, David Zhang, Dan Sadeghi, Hatef Shi, Jia Xiao, Zong‐Yuan Hong, Wenjing Lambert, Colin J. Liu, Shi‐Xia |
author_sort | Liu, Xunshan |
collection | PubMed |
description | To guide the choice of future synthetic targets for single‐molecule electronics, qualitative design rules are needed, which describe the effect of modifying chemical structure. Here the effect of heteroatom substitution on destructive quantum interference (QI) in single‐molecule junctions is, for the first time experimentally addressed by investigating the conductance change when a “parent” meta‐phenylene ethylene‐type oligomer (m‐OPE) is modified to yield a “daughter” by inserting one nitrogen atom into the m‐OPE core. We find that if the substituted nitrogen is in a meta position relative to both acetylene linkers, the daughter conductance remains as low as the parent. However, if the substituted nitrogen is in an ortho position relative to one acetylene linker and a para position relative to the other, destructive QI is alleviated and the daughter conductance is high. This behavior contrasts with that of a para‐connected parent, whose conductance is unaffected by heteroatom substitution. These experimental findings are rationalized by transport calculations and also agree with recent “magic ratio rules”, which capture the role of connectivity in determining the electrical conductance of such parents and daughters. |
format | Online Article Text |
id | pubmed-5396325 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2016 |
publisher | John Wiley and Sons Inc. |
record_format | MEDLINE/PubMed |
spelling | pubmed-53963252017-04-25 Gating of Quantum Interference in Molecular Junctions by Heteroatom Substitution Liu, Xunshan Sangtarash, Sara Reber, David Zhang, Dan Sadeghi, Hatef Shi, Jia Xiao, Zong‐Yuan Hong, Wenjing Lambert, Colin J. Liu, Shi‐Xia Angew Chem Int Ed Engl Communications To guide the choice of future synthetic targets for single‐molecule electronics, qualitative design rules are needed, which describe the effect of modifying chemical structure. Here the effect of heteroatom substitution on destructive quantum interference (QI) in single‐molecule junctions is, for the first time experimentally addressed by investigating the conductance change when a “parent” meta‐phenylene ethylene‐type oligomer (m‐OPE) is modified to yield a “daughter” by inserting one nitrogen atom into the m‐OPE core. We find that if the substituted nitrogen is in a meta position relative to both acetylene linkers, the daughter conductance remains as low as the parent. However, if the substituted nitrogen is in an ortho position relative to one acetylene linker and a para position relative to the other, destructive QI is alleviated and the daughter conductance is high. This behavior contrasts with that of a para‐connected parent, whose conductance is unaffected by heteroatom substitution. These experimental findings are rationalized by transport calculations and also agree with recent “magic ratio rules”, which capture the role of connectivity in determining the electrical conductance of such parents and daughters. John Wiley and Sons Inc. 2016-11-29 2017-01-02 /pmc/articles/PMC5396325/ /pubmed/27897363 http://dx.doi.org/10.1002/anie.201609051 Text en © 2016 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution (http://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. |
spellingShingle | Communications Liu, Xunshan Sangtarash, Sara Reber, David Zhang, Dan Sadeghi, Hatef Shi, Jia Xiao, Zong‐Yuan Hong, Wenjing Lambert, Colin J. Liu, Shi‐Xia Gating of Quantum Interference in Molecular Junctions by Heteroatom Substitution |
title | Gating of Quantum Interference in Molecular Junctions by Heteroatom Substitution |
title_full | Gating of Quantum Interference in Molecular Junctions by Heteroatom Substitution |
title_fullStr | Gating of Quantum Interference in Molecular Junctions by Heteroatom Substitution |
title_full_unstemmed | Gating of Quantum Interference in Molecular Junctions by Heteroatom Substitution |
title_short | Gating of Quantum Interference in Molecular Junctions by Heteroatom Substitution |
title_sort | gating of quantum interference in molecular junctions by heteroatom substitution |
topic | Communications |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5396325/ https://www.ncbi.nlm.nih.gov/pubmed/27897363 http://dx.doi.org/10.1002/anie.201609051 |
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