A Multidisciplinary Research Centre for Advanced Electron Paramagnetic Resonance

Lead Research Organisation: University of Oxford
Department Name: Oxford Chemistry

Abstract

Electron Paramagnetic Resonance (EPR) is a powerful technique in the study of a wide variety of chemical and biological systems that contain so-called paramagnetic species (ie, systems with unpaired electrons). Within the last decade, the technological advances in the area of high-field and pulsed EPR have equipped the chemist and physicist with fantastic new methods for the study of new materials as well as the potential to develop new technologies such as EPR-based quantum computing algorithms. The technological advances have been accompanied furthermore by the development of sophisticated assays for site directed mutagenesis (which allows the incorporation of paramagnetic spin-labels into any chemical or biochemical system almost at will) which has made EPR exceptionally versatile in many biochemical contexts. It is the major objective of this proposal to use the impressive armory of pulsed and high-field EPR methods to advance our understanding of fundamental chemical and biological processes on the molecular scale and to exploit and develop further EPR in advancing the field of quantum computing research. The 11 investigators propose a variety of projects which can be broadly classified into two major areas, namely (i) Materials Research and (ii) Chemical Biology Research.The development of EPR-based spin manipulation methodology on self-assembling, interacting nanoscale structures such as fullerenes and nanotubes containing atomic nitrogen and other paramagnetic species is driven by the desire to establish new quantum information applications and falls clearly in the first category. Further projects in the Materials Section concentrate on the study of paramagnetic centres crucial for the hydrogen sorption/desorption processes in hydrogen-storage materials such as carbon nanostructures, the investigation of transparent conductors and finally the application of pulsed EPR methods in the elucidation of processes involving the solvated electron in electronic solutions such as the Na-NH3 system.The majority of projects in the biochemical section of this research proposal are based on an exploitation of the ability of EPR to provide information on long-range interactions (up to 8nm) between paramagnetic centres and are focussed on extracting conformational information which are difficult to obtain by other technologies (such as NMR, X-ray crystallography). The paramagnetic sites will typically be introduced to the biochemical system by site-directed mutagenesis (spin-labels) or existing paramagnetic species (such as transition metal ions or organic radicals) will be exploited to deliver this long-range distance information. Pathogen-host interactions in viral complexes as well as protein-protein recognition pathways in enzymatic processes will be elucidated with pulsed EPR techniques. Model systems (such as metal-metal-rulers) will be designed and calibrated to facilitate and guide these biochemical studies. Another application of EPR will be to support an extensive program of research now underway to identify suitable enzymes and characterise modified enzymes for the development of novel fuel-cell catalysts. This project involves hydrogenases (hydrogen cycling) from a diverse range of organisms, and laccases (O2-reduction) that are being modified for attachment to electrodes. EPR is the method of choice for examining the redox centres and catalytic intermediates in these enzymes.

Publications


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Ardavan A (2011) Quantum control in spintronics. in Philosophical transactions. Series A, Mathematical, physical, and engineering sciences
Barry ER (2009) Intersubunit allosteric communication mediated by a conserved loop in the MCM helicase. in Proceedings of the National Academy of Sciences of the United States of America
 
Description The technique of Electron Spin Resonance(ESR) was first discovered close to the end of World War II. Immensely powerful for probing the microscopic aspects of nature, its widespread application to leading problems in science and technology was severely limited. With the advent of of user-friendly instrumentation, its user base broadened considerably. Thus in 2006 the Center for Advanced Electron Spin Resonance (CAESR) was founded in Oxford,involving a collaboration of researchers from the departments of Chemistry, Physics,Materials, Biochemistry and Pathology with substantial support from EPSRC,BBSRC and ERC and the University to provide modern equipment and focus for Oxford's multi-disciplinary research and development in ESR. CAESR has been spectacularly successful in numerous application-orientated challenges including, quantum computing, protein structure determination, bird migration, hydrogen storage materials and advanced optoelectronic materials. Since its establishment,
CAESR has been at the centre of many of the key developments
in the field of ESR. For example, seminal contributions
have been made by CAESR to the subjects of long
range distance measurements using Double Electron Electron
Resonance (DEER), and ESR quantum information
methodologies. These subjects attracted over 1300 citations
and over 700 citations respectively worldwide in 2012; in
1999 there were none at all in either subject. We believe that CAESR has made substantial contributions to propelling these research areas into lively and productive fields.
Exploitation Route Major international interactions have included collaborations with colleagues in the USA Cornell (National Biomedical Center for Advanced ESR Technology (ACERT); Princeton University , ETH Zurich (Switzerland) , Bielefeld (Germany), Hiroshima (Japan). The centre has attracted a multitude of industrial collaborators. In addition
to the founding EPSRC grant, the Oxford CAESR community
has won multiple external grants incorporating work
at CAESR from UK agencies including EPSRC, EMFBRT,
Wellcome, BBSRC and MRC, international funding
sources including DARPA, NSF, EU and UKIERI, and several industrial
sources, totalling over £7M. In 2015 a new state-of-the-art spectrometer was funded by EPSRC through a Strategic Equipment grant and has now attracted many UK and international collaborators.
The centre has been highlighted in articles in the Oxford
Blueprint, Chemistry and Industry and Chemistry World as
a model modern multidisciplinary research centre. The number of ESR users within Oxford itself has grown immensely over the last years following the establishment of CAESR - a lively community of researcher from over 20 groups within Oxford use the centre frequently (and yet more scientists require the services of CAESR on a somewhat less frequent basis).
Sectors Aerospace, Defence and Marine,Agriculture, Food and Drink,Chemicals,Digital/Communication/Information Technologies (including Software),Electronics,Energy,Environment,Healthcare,Manufacturing, including Industrial Biotechology,Pharmaceuticals and Medical Biotechnology,Security and Diplomacy,Transport
URL http://caesr-web.chem.ox.ac.uk/
 
Description Developments arising from research at CAESR have allowed close interactions with Bruker, a world-leading spectroscopic equipment manufacturer , in their further development of advanced instrumentation in ESR. This instrument manufacturer has been a very strong supporter of CAESR and through this interaction Bruker has received continuous ,first-hand feedback on instrument capability and limitations. because of these valued interactions, CAESR has enjoyed preferential technical assistance in operating its instrumentation beyond normal-use cases. We have established several industrial links which are still ongoing and are funding our Centre. Oxford has a service agreement with the National EPR service and we offer our expertise and advise as well as our spectrometers to the whole UK scientific community via this route.
First Year Of Impact 2006
Sector Agriculture, Food and Drink,Chemicals,Digital/Communication/Information Technologies (including Software),Electronics,Energy,Environment,Manufacturing, including Industrial Biotechology,Culture, Heritage, Museums and Collections,Pharmaceuticals and Medical Biotechnology,Transport
Impact Types Cultural,Economic
 
Description BBSRC Grouped
Amount £16,533 (GBP)
Funding ID DMRWIS0 
Organisation Biotechnology and Biological Sciences Research Council (BBSRC) 
Sector Public
Country United Kingdom of Great Britain & Northern Ireland (UK)
Start 05/2012 
End 06/2015
 
Description BBSRC Grouped
Amount £16,533 (GBP)
Funding ID DMRWIS0 
Organisation Biotechnology and Biological Sciences Research Council (BBSRC) 
Sector Public
Country United Kingdom of Great Britain & Northern Ireland (UK)
Start 05/2012 
End 06/2015