A Gadolinium Spin Label with Both a Narrow Central Transition and Short Tether for Use in Double Electron Electron Resonance Distance Measurements

Anokhi Shah, Amandine Roux, Matthieu Starck, Jackie A. Mosely, Michael Stevens, David G. Norman, Robert I. Hunter, Hassane El Mkami, Graham M. Smith, David Parker, Janet E. Lovett

Research output: Contribution to journalArticlepeer-review

9 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)3015-3025
Number of pages11
JournalInorganic Chemistry
Volume58
Issue number5
DOIs
Publication statusPublished - 4 Mar 2019

Bibliographical note

Funding Information:
The authors thank the ERC (266804), EPSRC (EP/R013705/ 1, EP/M508214/1), and the Carnegie Trust (RIG007510) for financial support, the Wellcome Trust for a Multi-User Equipment Grant (099149/Z/12/Z), and the Royal Society for a University Research Fellowship to JEL. We also thank Professor Catherine Botting and Dr. Sally Shirran for assistance with MALDI TOF at St Andrews.

Publisher Copyright:
© 2019 American Chemical Society.

Copyright:
Copyright 2019 Elsevier B.V., All rights reserved.

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