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Length-independent transport rates in biomolecules by quantum mechanical unfurling

Experiments on hole transfer in DNA between donor and acceptor moieties revealed transfer rates which are independent of the molecular bridge length (within experimental error). However, the physical origin of this intriguing observation is still unclear. The hopping model implies that the hole prop...

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Detalles Bibliográficos
Autores principales: Levine, Ariel D., Iv, Michael, Peskin, Uri
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2016
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5530864/
https://www.ncbi.nlm.nih.gov/pubmed/28808530
http://dx.doi.org/10.1039/c5sc03495g
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author Levine, Ariel D.
Iv, Michael
Peskin, Uri
author_facet Levine, Ariel D.
Iv, Michael
Peskin, Uri
author_sort Levine, Ariel D.
collection PubMed
description Experiments on hole transfer in DNA between donor and acceptor moieties revealed transfer rates which are independent of the molecular bridge length (within experimental error). However, the physical origin of this intriguing observation is still unclear. The hopping model implies that the hole propagates in multiple steps along the bridge from one localized state to another, and therefore the longer the bridge, the slower the transfer. This can explain weak length-dependence but not a length-independent transfer rate. We show that the rigid molecular structure of a poly-A bridge supports single step transitions from a localized hole state to delocalized states, spread over the entire bridge. Since propagation to the bridge end is a single step process (termed quantum unfurling) the transfer rate becomes independent of the bridge length. This explanation is consistent with experimental results, and emphasizes the importance of structural order in charge transfer through bio-molecular systems.
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spelling pubmed-55308642017-08-14 Length-independent transport rates in biomolecules by quantum mechanical unfurling Levine, Ariel D. Iv, Michael Peskin, Uri Chem Sci Chemistry Experiments on hole transfer in DNA between donor and acceptor moieties revealed transfer rates which are independent of the molecular bridge length (within experimental error). However, the physical origin of this intriguing observation is still unclear. The hopping model implies that the hole propagates in multiple steps along the bridge from one localized state to another, and therefore the longer the bridge, the slower the transfer. This can explain weak length-dependence but not a length-independent transfer rate. We show that the rigid molecular structure of a poly-A bridge supports single step transitions from a localized hole state to delocalized states, spread over the entire bridge. Since propagation to the bridge end is a single step process (termed quantum unfurling) the transfer rate becomes independent of the bridge length. This explanation is consistent with experimental results, and emphasizes the importance of structural order in charge transfer through bio-molecular systems. Royal Society of Chemistry 2016-02-01 2015-11-20 /pmc/articles/PMC5530864/ /pubmed/28808530 http://dx.doi.org/10.1039/c5sc03495g Text en This journal is © The Royal Society of Chemistry 2015 http://creativecommons.org/licenses/by-nc/3.0/ This is an Open Access article distributed under the terms of the Creative Commons Attribution-NonCommercial 3.0 Unported License (http://creativecommons.org/licenses/by-nc/3.0/) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is properly cited.
spellingShingle Chemistry
Levine, Ariel D.
Iv, Michael
Peskin, Uri
Length-independent transport rates in biomolecules by quantum mechanical unfurling
title Length-independent transport rates in biomolecules by quantum mechanical unfurling
title_full Length-independent transport rates in biomolecules by quantum mechanical unfurling
title_fullStr Length-independent transport rates in biomolecules by quantum mechanical unfurling
title_full_unstemmed Length-independent transport rates in biomolecules by quantum mechanical unfurling
title_short Length-independent transport rates in biomolecules by quantum mechanical unfurling
title_sort length-independent transport rates in biomolecules by quantum mechanical unfurling
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5530864/
https://www.ncbi.nlm.nih.gov/pubmed/28808530
http://dx.doi.org/10.1039/c5sc03495g
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