Dynamic Structural Science at the RC@H

RC@H 的动态结构科学

• 批准号: EP/I01974X/1
• 负责人: Paul Robert Raithby
• 金额: $ 190.1万
• 依托单位: University of Bath
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2011
• 资助国家: 英国
• 起止时间: 2011 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FI01974X%2F1
• 关键词: Dynamic; Structural; Science; RC

All chemical reactions and biological processes involve the movement of atoms, molecules or electrons and the speed at which these events occur may range from the very fast (femtoseconds, 10^-15 s) to the rather slow (hours or days). If we are to be able to improve our understanding of all these processes it would be very helpful if we could actually watch the atoms move and make molecular movies showing the progress of a chemical reaction. However, this is not straightforward because of the size of the atoms and molecules involved, which are too small to be seen through a conventional microscope. The techniques that have been available up to now include time resolved spectroscopy, which gives information on how some atoms within a molecule may move, or NMR spectroscopy which provides valuable information about molecular conformations in solution and allows some relatively slow processes to be followed. Ideally, a three dimensional picture of a molecule as it transforms is required. In the solid state it has been possible to obtain a three dimensional picture of a molecule or a biological macromolecule using X-ray or neutron diffraction for about the last 100 years, but both these techniques require minutes, and more often hours or, in the case of neutron diffraction, even days to obtain enough data to obtain this three dimensional picture. Thus, X-ray and neutron diffraction techniques have only been useful for obtaining the structures of molecules before they react or after the reaction is complete. The aim of this proposal is to develop a new technique called time resolved, or dynamic, structural science, which will bring the dimension of time into the crystallographic experiment and allow us to determine the structures of short-lived intermediates, with lifetimes of microseconds or less, or, by taking snapshots of a chemical process as it occurs at 100 picosecond intervals, make a molecular movie and watch the process occur. In order to achieve this aim we propose to assemble a range of experts from the leading structural and time resolved science groups in the UK and centre them at the new Research Complex at Harwell. This multidisciplinary team consisting of chemists, biologists and physicists will use the unique facilities on the Harwell site to develop the dynamic structural methods necessary to make molecular movies and to compare the results obtained by these methods in the solid state with the results obtained by time resolved spectroscopic methods. The Research Complex provides a unique working environment that will facilitate interactions with other physical and life scientists. Occupancy of the Complex also provides easy access to the Diamond Light Source, which generates very high intensity X-rays suitable for the crystallographic studies, the ISIS neutron source, which provides high intensity neutrons that are particularly useful for looking at materials that contain light atoms such as hydrogen, and the Lasers for Science Facility, which has high power lasers, whose very intense and tuneable light beams can be used for photoactivating the molecules to be studied and where the time resolved spectroscopy will be carried out.Once the new methodologies have been developed they will be used to study a range of important chemical and biological processes, that will include catalytic processes, light activated biological processes and reactions involving the movement of hydrogen atoms which are very important in both chemical and biological processes. The information gained will provide a better understanding of the reaction mechanisms and will point the way to the design of new, energy efficient catalysts, smarter sensor materials, new, more effective pharmaceuticals and other new materials. We will also work with scientists outside our consortium to allow our project to do an even wider range of exciting science and watch still more chemistry happen.

所有化学反应和生物过程均涉及原子，分子或电子的运动，这些事件发生的速度可能范围从非常快的（femtseconds，10^-15 s）到相当慢（小时或几天）。如果我们能够提高我们对所有这些过程的理解，那么如果我们可以真正观察原子移动并制作分子电影显示化学反应的进展，那将是非常有帮助的。但是，由于所涉及的原子和分子的大小，这并不简单，这些大小太小，无法通过常规显微镜看到。现在可以使用的技术包括时间分辨的光谱法，该技术提供了有关分子中某些原子如何移动的信息，或NMR光谱法提供了有关溶液中分子构象的有价值信息，并允许遵循一些相对缓慢的过程。理想情况下，需要在分子转换时的三维图像。在固态下，可以在过去的100年中使用X射线或中子衍射获得分子或生物大分子的三维图像，但是这两种技术都需要几分钟，或者更频繁地数小时，或者在中子衍射的情况下，甚至几天，几天才能获得足够的数据以获得这三个维度图片。因此，X射线和中子衍射技术仅在反应之前或反应完成之前获得分子的结构有用。 The aim of this proposal is to develop a new technique called time resolved, or dynamic, structural science, which will bring the dimension of time into the crystallographic experiment and allow us to determine the structures of short-lived intermediates, with lifetimes of microseconds or less, or, by taking snapshots of a chemical process as it occurs at 100 picosecond intervals, make a molecular movie and watch the process occur.为了实现这一目标，我们建议从英国领先的结构和时间解决科学小组组成一系列专家，并将其集中在哈威尔的新研究综合体中。由化学家，生物学家和物理学家组成的这个多学科团队将使用Harwell站点上的独特设施来开发制作分子电影所需的动态结构方法，并比较这些方法在固态中获得的结果与时间分辨的光谱方法获得的结果。研究综合体提供了一个独特的工作环境，将促进与其他身体和生活科学家的互动。该综合体的占用率还可以轻松进入钻石光源，该钻石光源可产生非常高的X射线射线，适合晶体学研究，ISIS中子源，ISIS中子源提供高强度中子，这些中子具有高强度的中子，这些中子对于查看包含氢原子（如氢气）的材料特别有用，例如氢气，以及用于具有高功能光束的较高功能光束的激光器，这些激光量很高，可以使用较高的光束，以使其具有较高的光束，以使其具有较高的光束，并且可以使用较高的光束，并且可以使用较高的光束，并且可以使用较高的光束。将进行分辨的光谱法。一旦开发了新方法，它们将用于研究一系列重要的化学和生物学过程，其中包括催化过程，光活化的生物学过程以及涉及涉及化学和生物学过程非常重要的氢原子运动的反应。获得的信息将更好地理解反应机制，并将指向新的，节能催化剂，更智能的传感器材料，新，更有效的药物和其他新材料的设计。我们还将与我们的财团以外的科学家合作，以允许我们的项目进行更广泛的令人兴奋的科学，并观察更多的化学反应。

项目成果

Comprehensive analysis of the green-to-blue photoconversion of full-length Cyanobacteriochrome Tlr0924.

• DOI: 10.1016/j.bpj.2014.09.020
• 发表时间: 2014-11-04
• 期刊: BIOPHYSICAL JOURNAL
• 影响因子: 3.4
• 作者: Hardman, Samantha J. O.;Hauck, Anna F. E.;Clark, Ian P.;Heyes, Derren J.;Scrutton, Nigel S.
• 通讯作者: Scrutton, Nigel S.

A rapidly-reversible absorptive and emissive vapochromic Pt(II) pincer-based chemical sensor.

• DOI: 10.1038/s41467-017-01941-2
• 发表时间: 2017-11-27
• 期刊: Nature communications
• 影响因子: 16.6
• 作者: Bryant MJ;Skelton JM;Hatcher LE;Stubbs C;Madrid E;Pallipurath AR;Thomas LH;Woodall CH;Christensen J;Fuertes S;Robinson TP;Beavers CM;Teat SJ;Warren MR;Pradaux-Caggiano F;Walsh A;Marken F;Carbery DR;Parker SC;McKeown NB;Malpass-Evans R;Carta M;Raithby PR
• 通讯作者: Raithby PR

Hard X-ray-Induced Valence Tautomeric Interconversion in Cobalt-o-Dioxolene Complexes.

• DOI: 10.1021/acs.jpclett.7b01794
• 发表时间: 2017-09
• 期刊: The journal of physical chemistry letters
• 作者: T. M. Francisco;W. Gee;H. Shepherd;M. Warren;D. Shultz;P. Raithby;C. Pinheiro

Dynamic structure elucidation of chemical reactivity by laser pulses and X-ray probes.

通过激光脉冲和 X 射线探针动态结构阐明化学反应性。

• DOI: 10.1039/c5dt00210a
• 发表时间: 2015
• 期刊: 2003)
• 作者: Bartlett SA