High energy resolution X-ray spectroscopy for air-sensitive actinide compounds

锕系化学的创新总是涉及对空气高度敏感的物种的研究。模型配合物的合成提供了一种方法来询问f块电子结构的基本原理，并可用于挑战有关氧化还原活性，金属配体共价和磁性的既定趋势。这项研究可以通过轨道选择性x射线光谱来加强，为提出的模型提供明确的证据，并定量地使电子结构合理化。最近发展起来的f块单元共振非弹性x射线散射（RIXS）为以前所未有的精度测量电子结构提供了新的机会。到目前为止，由于缺乏合适的运输和测量基础设施，f-block RIXS仅限于空气稳定样品。令人惊讶的是，RIXS尚未被f-block化学社区所采用。该项目将促进对2+、3+和4+氧化态的U和Th有机金属配合物的同工结构家族的重要开创性RIXS研究。学生将执行x射线光谱测量和执行计算来模拟光谱。这一结果将有助于进一步了解锕系元素的电子结构。结果还将包括用于锕系元素研究的RIXS技术的重大发展。

Innovation in actinide chemistry invariably involves the study of highly air-sensitive species. The synthesis of model complexes provides a means to interrogate the fundamentals of f-block electronic structure and can be applied to challenge established trends concerning redox activity, metal-ligand covalency and magnetism. This research can be enhanced with orbital selective X-ray spectroscopies to provide definitive proof for proposed models and to rationalise electronic structure quantitatively. The recent development of f-block element resonant inelastic X-ray scattering (RIXS) provides new opportunities to measure electronic structure with unprecedented precision. So far f-block RIXS has been limited to air-stable samples due to a lack of suitable transport and measurement infrastructure. Astonishingly, RIXS has not yet been adopted by the f-block chemistry community. This studentship will facilitate important seminal RIXS studies of isostructural families of U and Th organometallic complexes in 2+, 3+ and 4+ oxidation states. The student will be performing X-ray spectroscopy measurements and performing calculations to simulate spectra. The results will enable an improved understanding of actinide electronic structure. The results will also include significant development of the RIXS technique for actinide research.