A Multidisciplinary Research Centre for Advanced Electron Paramagnetic Resonance

电子顺磁共振（EPR）是一种强大的技术，用于研究各种化学和生物系统，这些系统包含所谓的顺磁性物质（即具有未配对电子的系统）。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奇妙新方法，以及开发基于EPR的量子计算算法等新技术的潜力。随着技术的进步，进一步发展了用于定点诱变的复杂分析（它允许将顺磁自旋标签几乎随意地纳入任何化学或生化系统），这使得EPR在许多生化环境中非常通用。本提案的主要目标是利用令人印象深刻的脉冲和高场EPR方法来推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开发和发展EPR。这11位研究人员提出了各种各样的项目，大致可以分为两个主要领域，即(i)材料研究和（ii）化学生物学研究。基于epr的自组装、相互作用纳米级结构（如富勒烯和含原子氮和其他顺磁性物质的纳米管）自旋操纵方法的发展是由建立新的量子信息应用的愿望驱动的，显然属于第一类。材料科的进一步项目集中在顺磁中心的研究上，顺磁中心对于碳纳米结构等储氢材料中的氢吸附/解吸过程至关重要，透明导体的研究以及脉冲EPR方法在电子溶液（如Na-NH3系统）中涉及溶剂化电子的过程的解释中的应用。本研究计划中生化部分的大部分项目都是基于利用EPR提供顺磁中心之间远程相互作用（高达8nm）信息的能力，并专注于提取其他技术（如核磁共振、x射线晶体学）难以获得的构象信息。顺磁位点通常会通过位点定向诱变（自旋标记）引入生化系统，或者利用现有的顺磁物质（如过渡金属离子或有机自由基）来传递这种远距离信息。病毒复合体中的病原体-宿主相互作用以及酶促过程中的蛋白质-蛋白质识别途径将通过脉冲EPR技术得到阐明。模型系统（如金属-金属-尺子）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广泛的研究项目，以确定合适的酶，并表征用于开发新型燃料电池催化剂的修饰酶。该项目涉及来自各种生物的氢化酶（氢循环）和漆酶（o2还原），这些酶正在被修饰以附着在电极上。EPR是检测这些酶的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.