DEER sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field EPR
Claire Motion would like to acknowledge funding from EPSRC as part of the iMR-CDT. Stacey Bell and Janet Lovett thank EPSRC Grant Number EP/LO22044/1. Janet Lovett also thanks the Royal Society for a University Research Fellowship and Research Grant RG120645. Sabine Van Doorslaer acknowledges the Re...
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Online Access: | http://hdl.handle.net/10023/8779 https://doi.org/10.1021/acs.jpclett.6b00456 |
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ftstandrewserep:oai:research-repository.st-andrews.ac.uk:10023/8779 2023-07-02T03:33:47+02:00 DEER sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field EPR Motion, Claire Louise Lovett, Janet Eleanor Bell, Stacey Cassidy, Scott Lindsay Cruickshank, Paul Alexander Sawchuk Bolton, David Robert Hunter, Robert Iain El Mkami, Hassane Van Doorslaer, Sabine Smith, Graham Murray The Wellcome Trust EPSRC The Royal Society University of St Andrews. School of Physics and Astronomy University of St Andrews. Biomedical Sciences Research Complex 2016-05-11T15:30:06Z 5 application/pdf http://hdl.handle.net/10023/8779 https://doi.org/10.1021/acs.jpclett.6b00456 eng eng Journal of Physical Chemistry Letters Motion , C L , Lovett , J E , Bell , S , Cassidy , S L , Cruickshank , P A S , Bolton , D R , Hunter , R I , El Mkami , H , Van Doorslaer , S & Smith , G M 2016 , ' DEER sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field EPR ' , Journal of Physical Chemistry Letters , vol. 7 , no. 8 , pp. 1411-1415 . https://doi.org/10.1021/acs.jpclett.6b00456 1948-7185 PURE: 241652026 PURE UUID: 9edcefd2-4287-4822-a219-d87594cc1154 Scopus: 84967214263 ORCID: /0000-0002-3561-450X/work/40301307 ORCID: /0000-0001-6578-7412/work/59464750 ORCID: /0000-0002-0552-5784/work/60195390 ORCID: /0000-0002-0415-9540/work/60195455 WOS: 000374810800001 http://hdl.handle.net/10023/8779 https://doi.org/10.1021/acs.jpclett.6b00456 099149/Z/12/Z EP/L022044/1 UF100020 UF090121 EP/F039034/1 Copyright 2016 American Chemical Society. This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. QC Physics QD Chemistry NDAS BDC R2C QC QD Journal article 2016 ftstandrewserep https://doi.org/10.1021/acs.jpclett.6b00456 2023-06-13T18:27:14Z Claire Motion would like to acknowledge funding from EPSRC as part of the iMR-CDT. Stacey Bell and Janet Lovett thank EPSRC Grant Number EP/LO22044/1. Janet Lovett also thanks the Royal Society for a University Research Fellowship and Research Grant RG120645. Sabine Van Doorslaer acknowledges the Research Foundation – Flanders (FWO) for financial support (grant G.0687.13). The W-band instrument was developed under the UK Research Council’s Basic Technology Program (grant EP/F039034/1). We also thank the Wellcome Trust (grant 099149/Z/12/Z). This work demonstrates the feasibility of making sensitive nanometer distancemeasurements between Fe(III) heme centers and nitroxide spin labels in proteins using the double electron-electron resonance (DEER) pulsed EPR technique at 94 GHz. Techniques to measure accurately long distances in many classes of heme proteins using DEER are currently strongly limited by sensitivity. In this paper we demonstrate sensitivity gains of more than 30times compared with previous lower frequency (X-band) DEER measurements on both human neuroglobin and sperm whale myoglobin. This is achieved by: taking advantage of recent instrumental advances; employing wideband excitation techniques based on composite pulses and exploiting more favorable relaxation properties of low-spin Fe(III) in high magnetic fields. This gain in sensitivity potentially allows the DEER technique to be routinely used as a sensitive probe of structure and conformation in the large number of heme and many other metalloproteins. Publisher PDF Peer reviewed Article in Journal/Newspaper Sperm whale University of St Andrews: Digital Research Repository The Journal of Physical Chemistry Letters 7 8 1411 1415 |
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Open Polar |
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University of St Andrews: Digital Research Repository |
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ftstandrewserep |
language |
English |
topic |
QC Physics QD Chemistry NDAS BDC R2C QC QD |
spellingShingle |
QC Physics QD Chemistry NDAS BDC R2C QC QD Motion, Claire Louise Lovett, Janet Eleanor Bell, Stacey Cassidy, Scott Lindsay Cruickshank, Paul Alexander Sawchuk Bolton, David Robert Hunter, Robert Iain El Mkami, Hassane Van Doorslaer, Sabine Smith, Graham Murray DEER sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field EPR |
topic_facet |
QC Physics QD Chemistry NDAS BDC R2C QC QD |
description |
Claire Motion would like to acknowledge funding from EPSRC as part of the iMR-CDT. Stacey Bell and Janet Lovett thank EPSRC Grant Number EP/LO22044/1. Janet Lovett also thanks the Royal Society for a University Research Fellowship and Research Grant RG120645. Sabine Van Doorslaer acknowledges the Research Foundation – Flanders (FWO) for financial support (grant G.0687.13). The W-band instrument was developed under the UK Research Council’s Basic Technology Program (grant EP/F039034/1). We also thank the Wellcome Trust (grant 099149/Z/12/Z). This work demonstrates the feasibility of making sensitive nanometer distancemeasurements between Fe(III) heme centers and nitroxide spin labels in proteins using the double electron-electron resonance (DEER) pulsed EPR technique at 94 GHz. Techniques to measure accurately long distances in many classes of heme proteins using DEER are currently strongly limited by sensitivity. In this paper we demonstrate sensitivity gains of more than 30times compared with previous lower frequency (X-band) DEER measurements on both human neuroglobin and sperm whale myoglobin. This is achieved by: taking advantage of recent instrumental advances; employing wideband excitation techniques based on composite pulses and exploiting more favorable relaxation properties of low-spin Fe(III) in high magnetic fields. This gain in sensitivity potentially allows the DEER technique to be routinely used as a sensitive probe of structure and conformation in the large number of heme and many other metalloproteins. Publisher PDF Peer reviewed |
author2 |
The Wellcome Trust EPSRC The Royal Society University of St Andrews. School of Physics and Astronomy University of St Andrews. Biomedical Sciences Research Complex |
format |
Article in Journal/Newspaper |
author |
Motion, Claire Louise Lovett, Janet Eleanor Bell, Stacey Cassidy, Scott Lindsay Cruickshank, Paul Alexander Sawchuk Bolton, David Robert Hunter, Robert Iain El Mkami, Hassane Van Doorslaer, Sabine Smith, Graham Murray |
author_facet |
Motion, Claire Louise Lovett, Janet Eleanor Bell, Stacey Cassidy, Scott Lindsay Cruickshank, Paul Alexander Sawchuk Bolton, David Robert Hunter, Robert Iain El Mkami, Hassane Van Doorslaer, Sabine Smith, Graham Murray |
author_sort |
Motion, Claire Louise |
title |
DEER sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field EPR |
title_short |
DEER sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field EPR |
title_full |
DEER sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field EPR |
title_fullStr |
DEER sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field EPR |
title_full_unstemmed |
DEER sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field EPR |
title_sort |
deer sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field epr |
publishDate |
2016 |
url |
http://hdl.handle.net/10023/8779 https://doi.org/10.1021/acs.jpclett.6b00456 |
genre |
Sperm whale |
genre_facet |
Sperm whale |
op_relation |
Journal of Physical Chemistry Letters Motion , C L , Lovett , J E , Bell , S , Cassidy , S L , Cruickshank , P A S , Bolton , D R , Hunter , R I , El Mkami , H , Van Doorslaer , S & Smith , G M 2016 , ' DEER sensitivity between iron centers and nitroxides in heme-containing proteins improves dramatically using broadband, high-field EPR ' , Journal of Physical Chemistry Letters , vol. 7 , no. 8 , pp. 1411-1415 . https://doi.org/10.1021/acs.jpclett.6b00456 1948-7185 PURE: 241652026 PURE UUID: 9edcefd2-4287-4822-a219-d87594cc1154 Scopus: 84967214263 ORCID: /0000-0002-3561-450X/work/40301307 ORCID: /0000-0001-6578-7412/work/59464750 ORCID: /0000-0002-0552-5784/work/60195390 ORCID: /0000-0002-0415-9540/work/60195455 WOS: 000374810800001 http://hdl.handle.net/10023/8779 https://doi.org/10.1021/acs.jpclett.6b00456 099149/Z/12/Z EP/L022044/1 UF100020 UF090121 EP/F039034/1 |
op_rights |
Copyright 2016 American Chemical Society. This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. |
op_doi |
https://doi.org/10.1021/acs.jpclett.6b00456 |
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The Journal of Physical Chemistry Letters |
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7 |
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8 |
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1411 |
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1415 |
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1770273872751362048 |