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A gadolinium spin label with both a narrow central transition and short tether for use in double electron electron resonance distance measurements

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GdSL_InorgChem.pdf (4.576Mb)
Date
18/02/2019
Author
Shah, Anokhi
Roux, Amandine
Starck, Matthieu
Mosely, Jackie A.
Stevens, Michael
Norman, David G.
Hunter, Robert I.
El Mkami, Hassane
Smith, Graham
Parker, David
Lovett, Janet E.
Funder
EPSRC
The Wellcome Trust
The Royal Society
Grant ID
EP/R013705/1
099149/Z/12/Z
UF150698
Keywords
QC Physics
QD Chemistry
TK Electrical engineering. Electronics Nuclear engineering
DAS
Metadata
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Abstract
The design, synthesis, and application of a nine-coordinate gadolinium(III)-containing spin label, [Gd.sTPATCN]-SL, for use in nanometer-distance measurement experiments by EPR spectroscopy is presented. The spin label links to cysteines via a short thioether tether and has a narrow central transition indicative of small zero-field splitting (ZFS). A protein homodimer, TRIM25cc, was selectively labeled with [Gd.sTPATCN]-SL (70%) and a nitroxide (30%) under mild conditions and measured using the double electron electron resonance (DEER) technique with both commercial Q-band and home-built W-band spectrometers. The label shows great promise for increasing the sensitivity of DEER measurements through both its favorable relaxation parameters and the large DEER modulation depth at both Q- and W-band for the inter-Gd(III) DEER measurement which, at 9%, is the largest recorded under these conditions.
Citation
Shah , A , Roux , A , Starck , M , Mosely , J A , Stevens , M , Norman , D G , Hunter , R I , El Mkami , H , Smith , G , Parker , D & Lovett , J E 2019 , ' A gadolinium spin label with both a narrow central transition and short tether for use in double electron electron resonance distance measurements ' , Inorganic Chemistry , vol. Article ASAP . https://doi.org/10.1021/acs.inorgchem.8b02892
Publication
Inorganic Chemistry
Status
Peer reviewed
DOI
https://doi.org/10.1021/acs.inorgchem.8b02892
ISSN
0020-1669
Type
Journal article
Rights
Copyright © 2019 American Chemical Society. This work has been made available online in accordance with the publisher’s policies. This is the author created, accepted version manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at 10.1021/acs.inorgchem.8b02892
Description
Funding from ERC (266804), EPSRC (EP/R013705/1, EP/M508214/1), Carnegie Trust (RIG007510), Wellcome Trust for a Multi-User Equipment Grant (099149/Z/12/Z), and the Royal Society for a University Research Fellowship to JEL.
Collections
  • University of St Andrews Research
URI
http://hdl.handle.net/10023/19485

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