Real-time cumulant approach for charge-transfer satellites in x-ray photoemission spectra

Article

关键词: PLASMON SATELLITES;    SUDDEN LIMIT;    CORE;    PHOTOELECTRON;    SINGULARITIES;    TRANSITION;    CEO2;    XPS;    NIO;   

DOI  :  10.1103/PhysRevB.91.121112

来源: SCIE

【 摘 要 】

X-ray photoemission spectra generally exhibit satellite features beyond the main peak due to many-body excitations. However, the satellites associated with charge-transfer excitations in correlatedmaterials have proved difficult to calculate from first principles and their interpretation has been controversial. Here we show that these satellites can be attributed to local density fluctuations in response to a suddenly created core hole. Our approach is based on a cumulant representation of the core-hole Green's function with a real-time, time-dependent density functional theory calculation of the cumulant. This approach includes effects that cannot be accounted for by cluster methods and yields a direct real-space, real-time interpretation. Illustrative results for TiO2 and NiO are in good agreement with XPS experiment.

【 授权许可】

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