A Multidisciplinary Research Centre for Advanced Electron Paramagnetic Resonance

电子顺磁共振（EPR）是一种强大的技术，用于研究包含所谓顺磁物质（即具有未成对电子的系统）的各种化学和生物系统。在过去的十年中，高场和脉冲EPR领域的技术进步为化学家和物理学家提供了研究新材料的新方法，以及开发新技术的潜力，如基于EPR的量子计算算法。技术进步还伴随着用于定点诱变的复杂测定的发展（其允许顺磁性自旋标记几乎随意地并入任何化学或生物化学系统中），这使得EPR在许多生物化学环境中特别通用。该提案的主要目标是使用令人印象深刻的脉冲和高场EPR方法来促进我们对分子尺度上基本化学和生物过程的理解，并在推进量子计算研究领域中进一步利用和发展EPR。十一名研究人员提出多项研究计划，大致可分为两大范畴，即（i）材料研究及（ii）化学生物学研究。相互作用的纳米级结构，例如含有原子氮和其它顺磁性物质的富勒烯和纳米管，是由建立新的量子信息应用的愿望驱动的，显然是第一类。材料部分的进一步项目集中在研究对储氢材料（如碳纳米结构）中的氢吸附/解吸过程至关重要的顺磁中心，透明导体的研究，最后是脉冲EPR方法在阐明涉及电子溶液中溶剂化电子的过程中的应用，如Na-本研究建议的生物化学部分中的大多数项目是基于利用EPR提供远程相互作用信息的能力（高达8 nm），并且专注于提取通过其他技术（例如NMR、X射线晶体学）难以获得的构象信息。顺磁性位点通常通过定点诱变（自旋标记）引入到生物化学系统中，或者将利用现有的顺磁性物质（例如过渡金属离子或有机自由基）来传递这种长距离信息。病毒复合物中的病原体-宿主相互作用以及酶促过程中的蛋白质-蛋白质识别途径将用脉冲EPR技术阐明。模型系统（如金属-金属-标尺）将被设计和校准，以促进和指导这些生化研究。EPR的另一个应用将是支持目前正在进行的一项广泛的研究计划，以确定合适的酶和经修饰的酶，用于开发新的燃料电池催化剂。该项目涉及来自各种生物的氢化酶（氢循环），以及正在修饰以附着于电极的漆酶（O2还原）。EPR是检查这些酶中氧化还原中心和催化中间体的首选方法。

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.