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

Abstract

X-ray photoemission spectra generally exhibit satellite features in addition to the quasi-particle peaks due to many-body excitations, which have been of considerable theoretical and experimental interest. However, the satellites attributed to charge-transfer (CT) excitations in correlated materials have proved difficult to calculate from first principles. Here we report a real-time, real-space approach for such calculations based on a cumulant representation of the core-hole Green's function and time-dependent density functional theory. This approach also yields an interpretation of CT satellites in terms of a complex oscillatory, transient response to a suddenly created core hole. Illustrative results for TiO${}_2$ and NiO are in good agreement with experiment.

References in corpus (10)

• The SIESTA method for ab initio order-N materials simulation
• Efficient index handling of multidimensional periodic boundary conditions
• Multiplet ligand-field theory using Wannier orbitals
• Calculation of the optical response of C60 and Na8 using time-dependent density functional theory and local orbitals
• The valence electron photoemission spectrum of semiconductors: ab initio description of multiple satellites
• Physical origin of satellite in photoemission of doped graphene: An ab-initio GW plus cumulant study
• Basis set effects on the hyperpolarizability of CHCl_3: Gaussian-type orbitals, numerical basis sets and real-space grids
• 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
• Charge transfer satellites in x-ray spectra of transition metal oxides

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• Demonstration of resonant inelastic X-ray scattering as a probe of exciton-phonon coupling
• Quantum Many-Body Effects in X-Ray Spectra Efficiently Computed using a Basic Graph Algorithm
• Quasiparticle spectra from molecules to bulk
• Multi-code Benchmark on Simulated Ti K-edge X-ray Absorption Spectra of Ti-O Compounds
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• Ab initio multiplet plus cumulant approach for correlation effects in x-ray photoelectron spectroscopy
• Non-linear response in the cumulant expansion for core hole photoemission
• Experimental assignment of many-electron excitations in the photo-ionization of NiO
• Orbital breathing effects in the computation of x-ray d-ion spectra in solids by ab initio wave-function-based methods
• Coupled Cluster Greens function formulations based on the effective Hamiltonians
• Real-time equation-of-motion CC cumulant and CC Green's function simulations of photoemission spectra of water and water dimer
• Real-space Green's function approach for intrinsic losses in x-ray spectra
• A loss for photoemission is a gain for Auger: Direct experimental evidence of crystal-field splitting and charge transfer in photoelectron spectroscopy