论文标题
Clearix：一种快速准确的第一原理方法，用于模拟和分析谐振非弹性X射线散射
CleaRIXS: A Fast and Accurate First-Principles Method for Simulation and Analysis of Resonant Inelastic X-ray Scattering
论文作者
论文摘要
共振非弹性X射线散射（RIX）以相互关联的方式探测被占用和空置的电子子空间，是在跨物理学，化学和材料科学研究中使用的最详细，最复杂和信息丰富的实验技术之一。我们引入了一个Ab-Initio，准确有效的计算框架，以模拟和分析RIXS Spectra，该框架结合了建模电子激发态的两种多样化和已建立的方法。核心孔线性响应RIX（CLEARIXS）方法不仅可以确保将电子与核心和价孔的相互作用准确融合，而且还可以自动将显着的RIX特征映射到相关的电子激发和降低。通过与先前的甲醇C K-EDGE RIX测量直接比较[J.物理。化学A 120，2260（2016）]，我们展示了形式主义在建模RIX频谱不同区域以及对其起源的物理见解方面的功效。除了在Clearix和基于决定因素的方法之间进行模拟X射线吸收和非共振X射线发射之间的连接之外，还探讨了包括价电子孔相互作用的重要性。还提出了对可能振动介导的过程产生的其他RIX特征的定性讨论。 Clearix为RIX过程的预测和解释提供了一个可靠且可扩展的框架，以及一般的复杂电子激发态的模拟。
Resonant Inelastic X-ray Scattering (RIXS), which probes the occupied and unoccupied electronic subspaces in an interrelated fashion, is one of the most detailed, complex and information-rich experimental techniques employed in the investigation of electronic structure across physics, chemistry and materials science. We introduce an ab-initio, accurate and efficient computational framework for simulation and analysis of RIXS spectra, which combines two diverse and established approaches to modeling electronic excited states. The Core-Hole Linear-Response RIXS (CleaRIXS) method not only ensures accurate incorporation of the interaction of electrons with core and valence holes, but also automatically maps the salient RIXS features to the relevant electronic excitations and de-excitations. Through direct comparison with previous methanol C K-edge RIXS measurements [J. Phys. Chem. A 120, 2260 (2016)], we show the efficacy of the formalism in modeling different regions of the RIXS spectrum and in gaining physical insight regarding their origins. The importance of including the valence electron-hole interactions is explored, in addition to the connection between CleaRIXS and determinant-based approaches for simulating X-ray absorption and non-resonant X-ray emission. A qualitative discussion of additional RIXS features arising from possible vibrationally-mediated processes is also presented. CleaRIXS provides a robust and extendable framework for prediction and interpretation of RIXS processes and for the simulation of complex electronic excited states in general.
