含时密度泛函理论计算共振非弹性X射线散射
A time-dependent density functional theory protocol for resonant inelastic X-ray scattering calculations
摘要：
提出了一种基于含时密度泛函理论（TDDFT）的方法来计算相对于一个共同的基态的两个不同的激发态流形之间的轻物质耦合。这些量是求解共振非弹性X射线散射（RIXS）和其他几种双光子光谱学的Kramers-Heisenberg方程的必要成分。该程序是基于伪波函数的方法，其中TDDFT本征态被视为一个配置相互作用波函数与单激发，并在限制能量窗口的方法，其中的激发态的歧管可以严格定义的基础上所占用的激发过程中所涉及的分子轨道的能量。我们说明了该方法的适用性，通过计算的2 p4 d RIXS地图的三个代表钌配合物，并将它们与实验结果进行比较。该方法是能够准确地捕捉所有的实验功能，在所有三个复合物，相对能量校正到0.6 eV内的两个独立的TDDFT计算的成本。
英文摘要：
We present a time-dependent density functional theory (TDDFT) based approach to compute the light-matter couplings between two different manifolds of excited states relative to a common ground state. These quantities are the necessary ingredients to solve the Kramers--Heisenberg equation for resonant inelastic X-ray scattering (RIXS) and several other types of two-photon spectroscopies. The procedure is based on the pseudo-wavefunction approach, where TDDFT eigenstates are treated as a configuration interaction wavefunction with single excitations, and on the restricted energy window approach, where a manifold of excited states can be rigorously defined based on the energies of the occupied molecular orbitals involved in the excitation process. We illustrate the applicability of the method by calculating the 2p4d RIXS maps of three representative Ruthenium complexes and comparing them to experimental results. The method is able to accurately capture all the experimental features in all three complexes, with relative energies correct to within 0.6 eV at the cost of two independent TDDFT calculations.
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