Charge transfer satellites in x-ray spectra of transition metal oxides

Abstract

Strongly correlated materials such as transition metal oxides (TMOs) often exhibit large satellites in their x-ray photoemission (XPS) and x-ray absorption spectra (XAS). These satellites arise from localized charge-transfer (CT) excitations that accompany the sudden creation of a core hole. Here we use a two-step approach to treat such excitations in a localized system embedded in a condensed system and coupled to a photoelectron. The total XAS is then given by a convolution of a spectral function representing the localized excitations and the XAS of the extended system. The local system is modeled roughly in terms of a simple three-level model, leading to a double-pole approximation for the spectral function that represents dynamically weighted contributions from the dominant neutral and charge-transfer excitations. This method is implemented using a resolvent approach, with potentials, radial wave-functions and matrix elements from the real-space Green's function code FEFF, and parameters fitted to XPS experiments. Representative calculations for several TMOs are found to be in reasonable agreement with experiment.

References in corpus (4)

• The valence electron photoemission spectrum of semiconductors: ab initio description of multiple satellites
• Many-pole model of inelastic losses in x-ray absorption spectra
• The transition from the adiabatic to the sudden limit in core level photoemission: A model study of a localized system
• K-edge X-ray absorption spectra in transition metal oxides beyond the single particle approximation: shake-up many body effects

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• Particle-hole cumulant approach for inelastic losses in x-ray spectra
• Non-linear response in the cumulant expansion for core hole photoemission
• Experimental assignment of many-electron excitations in the photo-ionization of NiO
• Gauge invariance and relativistic effects in photon absorption and scattering by matter
• Elucidating Many-Body Effects in Molecular Core Spectra through Real-Time Approaches: Efficient Classical Approximations and a Quantum Perspective
• Real-space Green's function approach for intrinsic losses in x-ray spectra