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Spin-filtered time-of-flight photoelectron momentum microscopy reveals asystematic variation of the band structure within a series of highlyspin-polarized ferromagnetic Heusler compounds with increasing number ofvalence electrons (Co2MnGa, Co2MnSi and Co2Fe0.4Mn0.6Si). The positions of theFermi energy for minority and majority electrons deviate strongly from a simpleband-filling model. Photoexcitation at h$\nu$=6.05 eV (4th harmonic of aTi:sapphire laser) gives access to the spin-polarization texture P(EB,kx,ky) ofthe bulk bands in a (kx,ky)-range with diameter 1.4{\AA}$^{-1}$ and energiesfrom the Fermi energy EF to a binding energy of EB=2 eV. The minority bands ofCo2MnGa cross the Fermi level, inhibiting half-metallicity; the crossing pointsallow a precise adjustment of experimental and theoretical majority andminority bands, requiring shifts in opposite directions. The top of theminority band lies only 0.15 eV above EF, i.e. Co2MnGa is much closer to beinghalf-metallic than predicted by calculations. For half-metallic Co2MnSi andCo2Fe0.4Mn0.6Si clear minority band gaps are visible, the topmost occupiedminority bands lie 0.5 and 0.35 eV below EF, in reasonable agreement withtheory; the exchange splitting is significantly smaller than in theory. Thecomparison of all three compounds uncovers the surprising fact that withincreasing number of valence electrons the frontier majority bands (close toEF) exhibit an increasing deficiency in filling, in comparison with theprediction of a DFT calculation. The same trend is visible in comparison with aDMFT calculation. For s-polarized excitation both half-metallic compoundsexhibit nearly complete positive spin polarization close to EF, consistent withprevious work in literature.

physical review. b./physical review. b

Band structure tuning of Heusler compounds revisited: Spin- and  momentum-resolved electronic structure analysis of compounds with different  band filling