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Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments

The ability of molecules to change colour on account of changes in solvent polarity is known as solvatochromism and used spectroscopically to characterize charge-transfer transitions in donor–acceptor molecules. Here we report that donor–acceptor-substituted molecular wires also exhibit distinct pro...

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Autores principales: Lissau, Henriette, Frisenda, Riccardo, Olsen, Stine T., Jevric, Martyn, Parker, Christian R., Kadziola, Anders, Hansen, Thorsten, van der Zant, Herre S. J., Brøndsted Nielsen, Mogens, Mikkelsen, Kurt V.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group 2015
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4682163/
https://www.ncbi.nlm.nih.gov/pubmed/26667583
http://dx.doi.org/10.1038/ncomms10233
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author Lissau, Henriette
Frisenda, Riccardo
Olsen, Stine T.
Jevric, Martyn
Parker, Christian R.
Kadziola, Anders
Hansen, Thorsten
van der Zant, Herre S. J.
Brøndsted Nielsen, Mogens
Mikkelsen, Kurt V.
author_facet Lissau, Henriette
Frisenda, Riccardo
Olsen, Stine T.
Jevric, Martyn
Parker, Christian R.
Kadziola, Anders
Hansen, Thorsten
van der Zant, Herre S. J.
Brøndsted Nielsen, Mogens
Mikkelsen, Kurt V.
author_sort Lissau, Henriette
collection PubMed
description The ability of molecules to change colour on account of changes in solvent polarity is known as solvatochromism and used spectroscopically to characterize charge-transfer transitions in donor–acceptor molecules. Here we report that donor–acceptor-substituted molecular wires also exhibit distinct properties in single-molecule electronics under the influence of a bias voltage, but in absence of solvent. Two oligo(phenyleneethynylene) wires with donor–acceptor substitution on the central ring (cruciform-like) exhibit remarkably broad conductance peaks measured by the mechanically controlled break-junction technique with gold contacts, in contrast to the sharp peak of simpler molecules. From a theoretical analysis, we explain this by different degrees of charge delocalization and hence cross-conjugation at the central ring. Thus, small variations in the local environment promote the quinoid resonance form (off), the linearly conjugated (on) or any form in between. This shows how the conductance of donor–acceptor cruciforms is tuned by small changes in the environment.
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spelling pubmed-46821632015-12-29 Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments Lissau, Henriette Frisenda, Riccardo Olsen, Stine T. Jevric, Martyn Parker, Christian R. Kadziola, Anders Hansen, Thorsten van der Zant, Herre S. J. Brøndsted Nielsen, Mogens Mikkelsen, Kurt V. Nat Commun Article The ability of molecules to change colour on account of changes in solvent polarity is known as solvatochromism and used spectroscopically to characterize charge-transfer transitions in donor–acceptor molecules. Here we report that donor–acceptor-substituted molecular wires also exhibit distinct properties in single-molecule electronics under the influence of a bias voltage, but in absence of solvent. Two oligo(phenyleneethynylene) wires with donor–acceptor substitution on the central ring (cruciform-like) exhibit remarkably broad conductance peaks measured by the mechanically controlled break-junction technique with gold contacts, in contrast to the sharp peak of simpler molecules. From a theoretical analysis, we explain this by different degrees of charge delocalization and hence cross-conjugation at the central ring. Thus, small variations in the local environment promote the quinoid resonance form (off), the linearly conjugated (on) or any form in between. This shows how the conductance of donor–acceptor cruciforms is tuned by small changes in the environment. Nature Publishing Group 2015-12-15 /pmc/articles/PMC4682163/ /pubmed/26667583 http://dx.doi.org/10.1038/ncomms10233 Text en Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Lissau, Henriette
Frisenda, Riccardo
Olsen, Stine T.
Jevric, Martyn
Parker, Christian R.
Kadziola, Anders
Hansen, Thorsten
van der Zant, Herre S. J.
Brøndsted Nielsen, Mogens
Mikkelsen, Kurt V.
Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments
title Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments
title_full Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments
title_fullStr Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments
title_full_unstemmed Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments
title_short Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments
title_sort tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4682163/
https://www.ncbi.nlm.nih.gov/pubmed/26667583
http://dx.doi.org/10.1038/ncomms10233
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