Multidimensional photoemission spectroscopy—the space-charge limit

Photoelectron spectroscopy, especially at pulsed sources, is ultimately limited by the Coulomb interaction in the electron cloud, changing energy and angular distribution of the photoelectrons. A detailed understanding of this phenomenon is crucial for future pump–probe photoemission studies at (x-ray) free electron lasers and high-harmonic photon sources. Measurements have been performed for Ir(111) at h ν = 1000 eV with photon flux densities between ∼10 ^2 and 10 ^4 photons per pulse and μ m ^2 (beamline P04/PETRA III, DESY Hamburg), revealing space-charge induced energy shifts of up to 10 eV. In order to correct the essential part of the energy shift and restore the electron distributions close to the Fermi energy, we developed a semi-analytical theory for the space-charge effect in cathode-lens instruments (momentum microscopes, photoemission electron microscopes). The theory predicts a Lorentzian profile of energy isosurfaces and allows us to quantify the charge cloud from measured energy profiles. The correction is essential for the determination of the Fermi surface, as we demonstrate by means of ‘ k -space movies’ for the prototypical high-Z material tungsten. In an energy interval of about 1 eV below the Fermi edge, the bandstructure can be restored up to substantial shifts of ∼7 eV. Scattered photoelectrons strongly enhance the inelastic background in the region several eV below E _F , proving that the majority of scattering events involves a slow electron. The correction yields a gain of two orders of magnitude in usable intensity compared with the uncorrected case (assuming a tolerable shift of 250 meV). The results are particularly important for future experiments at SASE-type free electron lasers, since the correction also works for strongly fluctuating (but known) pulse intensities.