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Twisted Carotenoids Do Not Support Efficient Intramolecular Singlet Fission in the Orange Carotenoid Protein

George A. Sutherland Orcid Logo, James P. Pidgeon Orcid Logo, Harrison Lee, Matthew S. Proctor, Andrew Hitchcock Orcid Logo, Shuangqing Wang, Dimitri Chekulaev, Wing Chung Tsoi Orcid Logo, Matthew P. Johnson, C. Neil Hunter Orcid Logo, Jenny Clark Orcid Logo

The Journal of Physical Chemistry Letters, Volume: 14, Issue: 26, Pages: 6135 - 6142

Swansea University Authors: Harrison Lee, Wing Chung Tsoi Orcid Logo

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Abstract

Singlet exciton fission is the spin-allowed generation of two triplet electronic excited states from a singlet state. Intramolecular singlet fission has been suggested to occur on individual carotenoid molecules within protein complexes provided that the conjugated backbone is twisted out of plane....

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Published in: The Journal of Physical Chemistry Letters
ISSN: 1948-7185 1948-7185
Published: American Chemical Society (ACS) 2023
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URI: https://cronfa.swan.ac.uk/Record/cronfa63765
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Intramolecular singlet fission has been suggested to occur on individual carotenoid molecules within protein complexes provided that the conjugated backbone is twisted out of plane. However, this hypothesis has been forwarded only in protein complexes containing multiple carotenoids and bacteriochlorophylls in close contact. To test the hypothesis on twisted carotenoids in a “minimal” one-carotenoid system, we study the orange carotenoid protein (OCP). OCP exists in two forms: in its orange form (OCPo), the single bound carotenoid is twisted, whereas in its red form (OCPr), the carotenoid is planar. To enable room-temperature spectroscopy on canthaxanthin-binding OCPo and OCPr without laser-induced photoconversion, we trap them in a trehalose glass. Using transient absorption spectroscopy, we show that there is no evidence of long-lived triplet generation through intramolecular singlet fission despite the canthaxanthin twist in OCPo.</abstract><type>Journal Article</type><journal>The Journal of Physical Chemistry Letters</journal><volume>14</volume><journalNumber>26</journalNumber><paginationStart>6135</paginationStart><paginationEnd>6142</paginationEnd><publisher>American Chemical Society (ACS)</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>1948-7185</issnPrint><issnElectronic>1948-7185</issnElectronic><keywords>Carotenoids, orange carotenoid protein, OCP, OCPo, OCPr, intramolecular singlet fission</keywords><publishedDay>6</publishedDay><publishedMonth>7</publishedMonth><publishedYear>2023</publishedYear><publishedDate>2023-07-06</publishedDate><doi>10.1021/acs.jpclett.3c01139</doi><url>http://dx.doi.org/10.1021/acs.jpclett.3c01139</url><notes/><college>COLLEGE NANME</college><department>Materials Science and Engineering</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>MTLS</DepartmentCode><institution>Swansea University</institution><apcterm/><funders>G.A.S. and C.N.H. acknowledge ERC Synergy Grant 854126. J.P.P. thanks the EPSRC for support through a Doctoral Training Partnership Scholarship (EP/R513313/1). The authors thank the EPSRC for a Capital Equipment Award (EP/L022613/1 and EP/R042802/1) which funded the Lord Porter Laser facility used in this study. J.C., C.N.H, G.A.S. and S.W. thank the EPSRC for funding through EP/S002103/1 and EP/T012455/1. J.C. and S.W. also thank the EPSRC for funding through EP/N014022/1. M.S.P. and M.P.J. were supported by Leverhulme Trust award RPG-2019-045. A.H. acknowledges The Royal Society (award URF\R1\191548). 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spelling v2 63765 2023-07-03 Twisted Carotenoids Do Not Support Efficient Intramolecular Singlet Fission in the Orange Carotenoid Protein 0ef65494d0dda7f6aea5ead8bb6ce466 Harrison Lee Harrison Lee true false 7e5f541df6635a9a8e1a579ff2de5d56 0000-0003-3836-5139 Wing Chung Tsoi Wing Chung Tsoi true false 2023-07-03 MTLS Singlet exciton fission is the spin-allowed generation of two triplet electronic excited states from a singlet state. Intramolecular singlet fission has been suggested to occur on individual carotenoid molecules within protein complexes provided that the conjugated backbone is twisted out of plane. However, this hypothesis has been forwarded only in protein complexes containing multiple carotenoids and bacteriochlorophylls in close contact. To test the hypothesis on twisted carotenoids in a “minimal” one-carotenoid system, we study the orange carotenoid protein (OCP). OCP exists in two forms: in its orange form (OCPo), the single bound carotenoid is twisted, whereas in its red form (OCPr), the carotenoid is planar. To enable room-temperature spectroscopy on canthaxanthin-binding OCPo and OCPr without laser-induced photoconversion, we trap them in a trehalose glass. Using transient absorption spectroscopy, we show that there is no evidence of long-lived triplet generation through intramolecular singlet fission despite the canthaxanthin twist in OCPo. Journal Article The Journal of Physical Chemistry Letters 14 26 6135 6142 American Chemical Society (ACS) 1948-7185 1948-7185 Carotenoids, orange carotenoid protein, OCP, OCPo, OCPr, intramolecular singlet fission 6 7 2023 2023-07-06 10.1021/acs.jpclett.3c01139 http://dx.doi.org/10.1021/acs.jpclett.3c01139 COLLEGE NANME Materials Science and Engineering COLLEGE CODE MTLS Swansea University G.A.S. and C.N.H. acknowledge ERC Synergy Grant 854126. J.P.P. thanks the EPSRC for support through a Doctoral Training Partnership Scholarship (EP/R513313/1). The authors thank the EPSRC for a Capital Equipment Award (EP/L022613/1 and EP/R042802/1) which funded the Lord Porter Laser facility used in this study. J.C., C.N.H, G.A.S. and S.W. thank the EPSRC for funding through EP/S002103/1 and EP/T012455/1. J.C. and S.W. also thank the EPSRC for funding through EP/N014022/1. M.S.P. and M.P.J. were supported by Leverhulme Trust award RPG-2019-045. A.H. acknowledges The Royal Society (award URF\R1\191548). H.K.H.L. and W.C.T. acknowledge the SPECIFIC Innovation and Knowledge Centre (EP/N020863/1) grant for providing financial support. 2023-08-16T12:04:00.1216203 2023-07-03T10:52:23.3712530 Faculty of Science and Engineering School of Engineering and Applied Sciences - Materials Science and Engineering George A. Sutherland 0000-0002-6319-4637 1 James P. Pidgeon 0000-0002-1509-5343 2 Harrison Lee 3 Matthew S. Proctor 4 Andrew Hitchcock 0000-0001-6572-434x 5 Shuangqing Wang 6 Dimitri Chekulaev 7 Wing Chung Tsoi 0000-0003-3836-5139 8 Matthew P. Johnson 9 C. Neil Hunter 0000-0003-2533-9783 10 Jenny Clark 0000-0001-9664-967x 11 63765__28283__e6d93d0f5c944078a3858025c3cc5cee.pdf 63765.VOR.pdf 2023-08-09T16:05:32.0831980 Output 2327151 application/pdf Version of Record true © 2023, The Author(s). Published by American Chemical Society. Distributed under the terms of a Creative Commons Attribution 4.0 License (CC BY 4.0). true eng https://creativecommons.org/licenses/by/4.0/
title Twisted Carotenoids Do Not Support Efficient Intramolecular Singlet Fission in the Orange Carotenoid Protein
spellingShingle Twisted Carotenoids Do Not Support Efficient Intramolecular Singlet Fission in the Orange Carotenoid Protein
Harrison Lee
Wing Chung Tsoi
title_short Twisted Carotenoids Do Not Support Efficient Intramolecular Singlet Fission in the Orange Carotenoid Protein
title_full Twisted Carotenoids Do Not Support Efficient Intramolecular Singlet Fission in the Orange Carotenoid Protein
title_fullStr Twisted Carotenoids Do Not Support Efficient Intramolecular Singlet Fission in the Orange Carotenoid Protein
title_full_unstemmed Twisted Carotenoids Do Not Support Efficient Intramolecular Singlet Fission in the Orange Carotenoid Protein
title_sort Twisted Carotenoids Do Not Support Efficient Intramolecular Singlet Fission in the Orange Carotenoid Protein
author_id_str_mv 0ef65494d0dda7f6aea5ead8bb6ce466
7e5f541df6635a9a8e1a579ff2de5d56
author_id_fullname_str_mv 0ef65494d0dda7f6aea5ead8bb6ce466_***_Harrison Lee
7e5f541df6635a9a8e1a579ff2de5d56_***_Wing Chung Tsoi
author Harrison Lee
Wing Chung Tsoi
author2 George A. Sutherland
James P. Pidgeon
Harrison Lee
Matthew S. Proctor
Andrew Hitchcock
Shuangqing Wang
Dimitri Chekulaev
Wing Chung Tsoi
Matthew P. Johnson
C. Neil Hunter
Jenny Clark
format Journal article
container_title The Journal of Physical Chemistry Letters
container_volume 14
container_issue 26
container_start_page 6135
publishDate 2023
institution Swansea University
issn 1948-7185
1948-7185
doi_str_mv 10.1021/acs.jpclett.3c01139
publisher American Chemical Society (ACS)
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Materials Science and Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Materials Science and Engineering
url http://dx.doi.org/10.1021/acs.jpclett.3c01139
document_store_str 1
active_str 0
description Singlet exciton fission is the spin-allowed generation of two triplet electronic excited states from a singlet state. Intramolecular singlet fission has been suggested to occur on individual carotenoid molecules within protein complexes provided that the conjugated backbone is twisted out of plane. However, this hypothesis has been forwarded only in protein complexes containing multiple carotenoids and bacteriochlorophylls in close contact. To test the hypothesis on twisted carotenoids in a “minimal” one-carotenoid system, we study the orange carotenoid protein (OCP). OCP exists in two forms: in its orange form (OCPo), the single bound carotenoid is twisted, whereas in its red form (OCPr), the carotenoid is planar. To enable room-temperature spectroscopy on canthaxanthin-binding OCPo and OCPr without laser-induced photoconversion, we trap them in a trehalose glass. Using transient absorption spectroscopy, we show that there is no evidence of long-lived triplet generation through intramolecular singlet fission despite the canthaxanthin twist in OCPo.
published_date 2023-07-06T12:04:01Z
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