Tackling the Peak Assignment Problem in X-ray Photoelectron Spectroscopy with First Principles Calculations

利用第一原理计算解决 X 射线光电子能谱中的峰分配问题

• 批准号: EP/Y037022/1
• 负责人: Reinhard J. Maurer
• 金额: $ 6.45万
• 依托单位: University of Warwick
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2024
• 资助国家: 英国
• 起止时间: 2024 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FY037022%2F1
• 关键词: Tackling; Peak; Assignment; Problem; ray

X-ray Photoelectron Spectroscopy (XPS) is one of the most widely used methods of characterization in applied surface science. It is applied in studies of heterogeneous catalysis, environmental degradation, corrosion, the manufacture of surface coatings, and various other processes. However, the practical value of XPS measurements is currently negatively affected by widespread problems in the analysis of recorded spectra. These have been extensively discussed in recent scientific literature, and problems with peak fitting and peak assignment in core level XPS have been identified as a source of significant errors in the analysis of XPS spectra. These problems can limit the amount of useful chemical insights that XPS is able to provide, and moreover, incorrect peak assignments can lead to the wrong conclusions being drawn about the underlying chemistry. The aim of this research project is to tackle these problems by enabling and encouraging the more widespread use of computational methods in the interpretation of experimental XPS spectra, and to thereby make XPS a more reliable and more useful method of characterization. Specifically, we want to make existing computational methods for calculating core electron binding energies and simulating core level spectra accessible to a wider community of researchers, and to improve these methods such that they would better meet the needs of XPS users. We will develop new, computationally efficient and user-friendly implementations of the delta-SCF method and the GW+cumulant approach, carry out case-studies that are designed to test the limits of current theories in guiding the analysis of real world spectra, and organize workshops and write tutorials to increase the user base of the computational techniques. The planned work will be carried out by an international, interdisciplinary and intersectoral team of experts in theoretical spectroscopy, developers of electronic structure codes, XPS users, and instrument manufacturers

X 射线光电子能谱 (XPS) 是应用表面科学中最广泛使用的表征方法之一。它应用于多相催化、环境退化、腐蚀、表面涂层制造以及各种其他过程的研究。然而，XPS 测量的实用价值目前受到记录光谱分析中普遍存在的问题的负面影响。这些在最近的科学文献中得到了广泛的讨论，并且核心级 XPS 中的峰值拟合和峰值分配问题已被确定为 XPS 光谱分析中重大误差的来源。这些问题可能会限制 XPS 能够提供的有用化学见解的数量，而且，错误的峰分配可能会导致对基础化学得出错误的结论。本研究项目的目的是通过启用和鼓励在实验 XPS 光谱解释中更广泛地使用计算方法来解决这些问题，从而使 XPS 成为更可靠、更有用的表征方法。具体来说，我们希望使更广泛的研究人员能够使用现有的计算核心电子结合​​能和模拟核心能级光谱的计算方法，并改进这些方法，以便更好地满足 XPS 用户的需求。我们将开发新的、计算高效且用户友好的 delta-SCF 方法和 GW+累积量方法的实现，开展旨在测试当前理论在指导现实世界光谱分析方面的局限性的案例研究，以及组织研讨会并编写教程以增加计算技术的用户群。计划的工作将由理论光谱学专家、电子结构代码开发人员、XPS用户和仪器制造商组成的国际、跨学科和跨部门团队进行