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Spurious oscillations from local self-interaction correction in high-energy photoionization calculations for metal clusters

M E Madjet, Himadri S Chakraborty1 and Jan-M Rost

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LETTER TO THE EDITOR

We find that for simple metal clusters a single-electron description of the ground state employing self-interaction correction (SIC) in the framework of local-density approximation strongly contaminates the high-energy photoionization cross sections with spurious oscillations for a subshell containing node(s). This effect is shown connected to the unphysical structure that SIC generates in ensuing state-dependent radial potentials around a position where the respective orbital density attains nodal zero. Non-local Hartree-Fock that exactly eliminates the electron self-interaction is found entirely free from this effect. It is inferred that while SIC is largely unimportant in high photon energies, any implementation of it within the local frame can induce unphysical oscillations in the high-energy photospectra of metal clusters pointing to a general need for caution in choosing appropriate theoretical tools.


PACS

33.80.Eh Autoionization, photoionization, and photodetachment

31.15.xr Self-consistent-field methods

31.15.E- Density-functional theory

36.40.Vz Optical properties of clusters

31.15.V- Electron correlation calculations for atoms, ions and molecules

33.60.+q Photoelectron spectra

Subjects

Atomic and molecular physics

Computational physics

Dates

Issue 10 (28 May 2001)

Received 7 March 2001



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