Augmenting Oxford's Centre for Advanced Electron Spin Resonance with a Bruker Elexsys E580 X/Q-band pulsed ESR spectrometer

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

Abstract

The Centre for Advanced Electron Spin Resonance (CAESR) is a collaboration of researchers from the Oxford University Departments of Physics, Chemistry, Materials, Biochemistry, and Pathology. It was founded in 2006 with substantial support from EPSRC and the University to provide modern equipment and an academic focus for Oxford's multi-disciplinary research in electron spin resonance (ESR).

CAESR has been spectacularly successful. It has nucleated a world-leading community of ESR spectroscopists in Oxford, and its stakeholders now extend well beyond the original group of co-applicants. It has established a national and international reputation as a centre of excellence in ESR. CAESR's scientific productivity and the research projects that it supports are now significantly constrained by two limitations of the existing equipment: (i) the availability of only two frequencies, 9.5 GHz (X-band) and 95 GHz (W-band); and (ii) a severe shortage of experimental capacity at the "work-horse" X-band frequency.

We propose to reinforce CAESR's facilities with a Bruker Elexsys E580 X/Q-band pulsed electron spin resonance spectrometer. It will augment CAESR's facilities with a third frequency (Q-band, 35 GHz), and it will offer the experimental capacity needed by CAESR's growing community of participants. This instrument will significantly enhance CAESR's existing research projects and enable an exciting portfolio of new activities, covering a wide range of EPSRC priority areas and addressing each of EPSRC's Physics and Chemistry Grand Challenges. It will allow CAESR to apply ESR in innovative ways to new scientific problems and to lead methodological developments in ESR.

The instrument has two features that will make it unique in the UK: high-power at Q-band, offering the shortest, highest-bandwidth pulses available; and an arbitrary waveform generator, allowing the direct synthesis of complex pulses for the first time in a turn-key ESR system. For 20% of the time, the instrument will be accessible to the wider UK ESR community through collaboration with the CAESR community, and via a contract with the EPSRC National EPR Facility based in Manchester. Young scientists from the Integrated Magnetic Resonance Centre for Doctoral Training (based in Warwick) will have the opportunity to explore the cutting-edge experimental capabilities offered by the arbitrary waveform generator and high-power amplifier incorporated in the new instrument, during annual training sessions at CAESR.

The instrument's manufacturer, Bruker, seeks to strengthen links with CAESR by offering salary support for the Technical Manager. Through this interaction Bruker will receive first-hand feedback on instrument limitations, possible upgrades and new technical and methodological developments, and CAESR will receive preferential technical assistance in operating the instrumentation beyond its normal use-cases.

Planned Impact

The primary impact of this proposal is to advance scientific knowledge by equipping researchers with an exquisitely sensitive tool for understanding molecular structure and dynamics in unprecedented detail. The new pulsed X/Q-band spectrometer will impact significantly on the science output of its users in the following ways:
(i) The introduction of an extra intermediate frequency to CAESR's toolkit will allow previously impossible multifrequency studies, facilitating a much wider range of time scales and magnetic interactions to be interrogated.
(ii) Both the number of projects supported by CAESR and the quality of data obtained increase as the new instrument both doubles the number of available spectrometer hours and reduces data acquisition times.
(iii) The increased sensitivity of the spectrometer will hugely impact researchers whose samples were previously too dilute to study at CAESR (e.g., samples that cannot be synthesized in sufficient concentrations or proteins that precipitate at high concentrations).
(iv) The arbitrary waveform generator (AWG) allows much improved control over electron spin manipulation and is therefore of particular interest to CAESR's large community of users developing quantum information processing algorithms.

Either through our contract with the EPSRC National EPR Facility in Manchester, or through collaboration with CAESR members, all UK scientists with an interest in studying paramagnetic systems will benefit from the advantages of the high-power at Q-band and the AWG (both unique in the UK). Thus the facility will support the upwards trajectory of ESR science in the UK in terms of: methodological development (e.g., HiPER, CAESR); theory (e.g., Southampton, CAESR); and ESR-led applications (e.g., Cardiff, Dundee, Edinburgh, Manchester, UCL, UEA, York, Warwick, HiPER and CAESR). The acquisition of the new spectrometer will thereby promote further CAESR's and the UK's scientific impact (both through publications and conferences), expanding the international visibility of UK analytical science in general and the research areas of CAESR's stakeholders in particular.

Our wide portfolio of research interests will have potential long-term impacts in areas as diverse as (i) the design of antibiotic and anti-cancer drugs, (ii) government policy on extremely low frequency magnetic fields, (iii) an understanding of basic bacterial cell biology relevant to pathogenesis, leading to design of therapeutic pathways, (iv) the understanding of how to harvest solar energy efficiently in arrays of dye molecules, leading to efficient photovoltaic cells, (v) the understanding of charge delocalisation in molecular wires, leading to new magneto-optical materials, (vi) the development of a new generation of MRI probes capable of generating contrast through binding to receptors, (viii) the design of future renewable energy technologies and (viii) the construction of the scientific underpinnings of the emerging quantum technologies industry.

Our track record proves our commitment to and ability at training highly skilled researchers. Our programme will expand to include an annual training day for the Integrated Magnetic Resonance Centre for Doctoral Training, providing young scientists with hands-on experience of UK-unique instrumentation and advertising the spectrometer's capabilities to students from a wide variety of research groups.

Through our close relationship with Bruker, we will ensure that our methodological developments will have immediate impact on the R&D sector of the spectrometer's manufacturer. With ESR becoming ever more important in the study of proteins and their complexes, our many commercial partners and sponsors will not only benefit from our ESR-driven progress through collaborative projects but they will also be encouraged to apply the techniques with other project partners or indeed within their own R&D departments.

Publications

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Richert S (2017) Quantifying the exchange coupling in linear copper porphyrin oligomers. in Physical chemistry chemical physics : PCCP

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Peeks MD (2017) Electronic Delocalization in the Radical Cations of Porphyrin Oligomer Molecular Wires. in Journal of the American Chemical Society

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Richert S (2017) On the Influence of the Bridge on Triplet State Delocalization in Linear Porphyrin Oligomers. in Journal of the American Chemical Society

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Hetzke T (2017) ELDOR-detected NMR at Q-Band in Applied Magnetic Resonance

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Richert S (2017) Delocalisation of photoexcited triplet states probed by transient EPR and hyperfine spectroscopy. in Journal of magnetic resonance (San Diego, Calif. : 1997)

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Richert S (2017) On the Importance of Electronic Symmetry for Triplet State Delocalization. in Journal of the American Chemical Society

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Goodwin DL (2018) Feedback control optimisation of ESR experiments. in Journal of magnetic resonance (San Diego, Calif. : 1997)

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Lewis AM (2018) On the low magnetic field effect in radical pair reactions. in The Journal of chemical physics

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Liu J (2019) Electric Field Control of Spins in Molecular Magnets in Physical Review Letters

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Wili N (2019) ELDOR-detected NMR beyond hyperfine couplings: a case study with Cu(ii)-porphyrin dimers. in Physical chemistry chemical physics : PCCP

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Grabarczyk DB (2019) Dioxygen controls the nitrosylation reactions of a protein-bound [4Fe4S] cluster. in Dalton transactions (Cambridge, England : 2003)

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Yang K (2019) Coherent spin manipulation of individual atoms on a surface. in Science (New York, N.Y.)

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Righetto M (2020) The Elusive Nature of Carbon Nanodot Fluorescence: An Unconventional Perspective in The Journal of Physical Chemistry C

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Barendt TA (2020) The Green Box: An Electronically Versatile Perylene Diimide Macrocyclic Host for Fullerenes. in Journal of the American Chemical Society

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Bajada MA (2020) A Precious-Metal-Free Hybrid Electrolyzer for Alcohol Oxidation Coupled to CO -to-Syngas Conversion. in Angewandte Chemie (International ed. in English)

 
Description The Centre for Advanced Electron Spin Resonance (CAESR) is a collaboration of researchers from the Oxford University Departments of Physics, Chemistry, Materials, Biochemistry, and Pathology. It was founded in 2006 with substantial support from EPSRC and the University to provide modern equipment and an academic focus for Oxford's multi-disciplinary research in electron spin resonance (ESR). The purpose of this grant was to augment CAESR's existing facilities with (i) up-to-date equipment, allowing us to continue at the cutting-edge in the development of ESR methodologies, and (ii) extra experimental capacity, allowing an increase in the volume of internationally leading and recognised multidisciplinary research conducted at the Centre.

CAESR's key scientific findings are reported in the numerous peer-reviewed publications (listed at http://caesr-web.chem.ox.ac.uk/publications.aspx) of its users. There were about 90 such publications in international peer-reviewed research journals during the course of the grant, of which six were in the leading journals Science and Nature. In this period, CAESR has trained about 140 scientists PhD and post-doc level, and offered research experience in ESR to about 100 undergraduates.

In addition to facilitating the scientific findings, the grant was pivotal in contributing to CAESR becoming an internationally-recognised and world-leading centre for ESR research: CAESR users engage in numerous national and international scientific collaborations; and CAESR hosted one of the key international research conferences in the subject (the 50th Annual International Meeting of the ESR Spectroscopy Group of the Royal Society of Chemistry, http://www.esr-group.org/conferences/2017-conference-oxford/). This in turn contributes to the UK's internationally-recognised excellence in the field of ESR.
Exploitation Route CAESR continues to offer world-leading research facilities and a concentration of expertise to academic and industrial users in Oxford, the UK, and internationally. The scientific outputs from CAESR continue to underpin international research in a wide range of scientific disciplines.
Sectors Chemicals,Digital/Communication/Information Technologies (including Software),Education,Electronics,Energy,Environment,Healthcare,Manufacturing, including Industrial Biotechology,Pharmaceuticals and Medical Biotechnology

URL http://caesr-web.chem.ox.ac.uk/home