Fundamental Limits on Wavelength, Efficiency and Yield of the Charge Separation Triad
Autor(a) principal: | |
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Data de Publicação: | 2012 |
Outros Autores: | , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.1371/journal.pone.0036065 http://hdl.handle.net/11449/24644 |
Resumo: | In an attempt to optimize a high yield, high efficiency artificial photosynthetic protein we have discovered unique energy and spatial architecture limits which apply to all light-activated photosynthetic systems. We have generated an analytical solution for the time behavior of the core three cofactor charge separation element in photosynthesis, the photosynthetic cofactor triad, and explored the functional consequences of its makeup including its architecture, the reduction potentials of its components, and the absorption energy of the light absorbing primary-donor cofactor. Our primary findings are two: First, that a high efficiency, high yield triad will have an absorption frequency more than twice the reorganization energy of the first electron transfer, and second, that the relative distance of the acceptor and the donor from the primary-donor plays an important role in determining the yields, with the highest efficiency, highest yield architecture having the light absorbing cofactor closest to the acceptor. Surprisingly, despite the increased complexity found in natural solar energy conversion proteins, we find that the construction of this central triad in natural systems matches these predictions. Our analysis thus not only suggests explanations for some aspects of the makeup of natural photosynthetic systems, it also provides specific design criteria necessary to create high efficiency, high yield artificial protein-based triads. |
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Fundamental Limits on Wavelength, Efficiency and Yield of the Charge Separation TriadIn an attempt to optimize a high yield, high efficiency artificial photosynthetic protein we have discovered unique energy and spatial architecture limits which apply to all light-activated photosynthetic systems. We have generated an analytical solution for the time behavior of the core three cofactor charge separation element in photosynthesis, the photosynthetic cofactor triad, and explored the functional consequences of its makeup including its architecture, the reduction potentials of its components, and the absorption energy of the light absorbing primary-donor cofactor. Our primary findings are two: First, that a high efficiency, high yield triad will have an absorption frequency more than twice the reorganization energy of the first electron transfer, and second, that the relative distance of the acceptor and the donor from the primary-donor plays an important role in determining the yields, with the highest efficiency, highest yield architecture having the light absorbing cofactor closest to the acceptor. Surprisingly, despite the increased complexity found in natural solar energy conversion proteins, we find that the construction of this central triad in natural systems matches these predictions. Our analysis thus not only suggests explanations for some aspects of the makeup of natural photosynthetic systems, it also provides specific design criteria necessary to create high efficiency, high yield artificial protein-based triads.Air Force Office of Scientific ResearchNIH National Center for Research ResourcesCenter for Exploitation of Nanostructures in Sensor and Energy Systems (CENSES) under NSFUniv Estadual Paulista, Inst Fis Teor, BR-01405 São Paulo, BrazilCUNY City Coll, Dept Phys, New York, NY 10031 USAUniv Estadual Paulista, Inst Fis Teor, BR-01405 São Paulo, BrazilAir Force Office of Scientific Research: FA9550-10-1-0350NIH: 5G12 RR03060CENSES under NSF: 0833180Public Library ScienceUniversidade Estadual Paulista (Unesp)CUNY City CollPunnoose, Alexander [UNESP]McConnell, Liza A.Liu, WeiMutter, Andrew C.Koder, Ronald L.2013-09-30T19:01:52Z2014-05-20T14:13:34Z2013-09-30T19:01:52Z2014-05-20T14:13:34Z2012-06-01info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article11application/pdfhttp://dx.doi.org/10.1371/journal.pone.0036065Plos One. San Francisco: Public Library Science, v. 7, n. 6, p. 11, 2012.1932-6203http://hdl.handle.net/11449/2464410.1371/journal.pone.0036065WOS:000305339900001WOS000305339900001.pdfWeb of Sciencereponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengPLOS ONE2.7661,164info:eu-repo/semantics/openAccess2024-01-23T07:12:09Zoai:repositorio.unesp.br:11449/24644Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462024-08-05T23:47:37.024942Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
Fundamental Limits on Wavelength, Efficiency and Yield of the Charge Separation Triad |
title |
Fundamental Limits on Wavelength, Efficiency and Yield of the Charge Separation Triad |
spellingShingle |
Fundamental Limits on Wavelength, Efficiency and Yield of the Charge Separation Triad Punnoose, Alexander [UNESP] |
title_short |
Fundamental Limits on Wavelength, Efficiency and Yield of the Charge Separation Triad |
title_full |
Fundamental Limits on Wavelength, Efficiency and Yield of the Charge Separation Triad |
title_fullStr |
Fundamental Limits on Wavelength, Efficiency and Yield of the Charge Separation Triad |
title_full_unstemmed |
Fundamental Limits on Wavelength, Efficiency and Yield of the Charge Separation Triad |
title_sort |
Fundamental Limits on Wavelength, Efficiency and Yield of the Charge Separation Triad |
author |
Punnoose, Alexander [UNESP] |
author_facet |
Punnoose, Alexander [UNESP] McConnell, Liza A. Liu, Wei Mutter, Andrew C. Koder, Ronald L. |
author_role |
author |
author2 |
McConnell, Liza A. Liu, Wei Mutter, Andrew C. Koder, Ronald L. |
author2_role |
author author author author |
dc.contributor.none.fl_str_mv |
Universidade Estadual Paulista (Unesp) CUNY City Coll |
dc.contributor.author.fl_str_mv |
Punnoose, Alexander [UNESP] McConnell, Liza A. Liu, Wei Mutter, Andrew C. Koder, Ronald L. |
description |
In an attempt to optimize a high yield, high efficiency artificial photosynthetic protein we have discovered unique energy and spatial architecture limits which apply to all light-activated photosynthetic systems. We have generated an analytical solution for the time behavior of the core three cofactor charge separation element in photosynthesis, the photosynthetic cofactor triad, and explored the functional consequences of its makeup including its architecture, the reduction potentials of its components, and the absorption energy of the light absorbing primary-donor cofactor. Our primary findings are two: First, that a high efficiency, high yield triad will have an absorption frequency more than twice the reorganization energy of the first electron transfer, and second, that the relative distance of the acceptor and the donor from the primary-donor plays an important role in determining the yields, with the highest efficiency, highest yield architecture having the light absorbing cofactor closest to the acceptor. Surprisingly, despite the increased complexity found in natural solar energy conversion proteins, we find that the construction of this central triad in natural systems matches these predictions. Our analysis thus not only suggests explanations for some aspects of the makeup of natural photosynthetic systems, it also provides specific design criteria necessary to create high efficiency, high yield artificial protein-based triads. |
publishDate |
2012 |
dc.date.none.fl_str_mv |
2012-06-01 2013-09-30T19:01:52Z 2013-09-30T19:01:52Z 2014-05-20T14:13:34Z 2014-05-20T14:13:34Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://dx.doi.org/10.1371/journal.pone.0036065 Plos One. San Francisco: Public Library Science, v. 7, n. 6, p. 11, 2012. 1932-6203 http://hdl.handle.net/11449/24644 10.1371/journal.pone.0036065 WOS:000305339900001 WOS000305339900001.pdf |
url |
http://dx.doi.org/10.1371/journal.pone.0036065 http://hdl.handle.net/11449/24644 |
identifier_str_mv |
Plos One. San Francisco: Public Library Science, v. 7, n. 6, p. 11, 2012. 1932-6203 10.1371/journal.pone.0036065 WOS:000305339900001 WOS000305339900001.pdf |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
PLOS ONE 2.766 1,164 |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
11 application/pdf |
dc.publisher.none.fl_str_mv |
Public Library Science |
publisher.none.fl_str_mv |
Public Library Science |
dc.source.none.fl_str_mv |
Web of Science reponame:Repositório Institucional da UNESP instname:Universidade Estadual Paulista (UNESP) instacron:UNESP |
instname_str |
Universidade Estadual Paulista (UNESP) |
instacron_str |
UNESP |
institution |
UNESP |
reponame_str |
Repositório Institucional da UNESP |
collection |
Repositório Institucional da UNESP |
repository.name.fl_str_mv |
Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP) |
repository.mail.fl_str_mv |
|
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1808129552699883520 |