  The electronic structure of Me[N(CN)$_2$]$_2$ (Me=Mn, Fe, Co, Ni, Cu)
molecular magnets has been investigated using x-ray emission spectroscopy (XES)
and x-ray photoelectron spectroscopy (XPS) as well as theoretical
density-functional-based methods. Both theory and experiments show that the top
of the valence band is dominated by Me 3d bands, while a strong hybridization
between C 2p and N 2p states determines the valence band electronic structure
away from the top. The 2p contributions from non-equivalent nitrogen sites have
been identified using resonant inelastic x-ray scattering spectroscopy with the
excitation energy tuned near the N 1s threshold. The binding energy of the Me
3d bands and the hybridization between N 2p and Me 3d states both increase in
going across the row from Me = Mn to Me = Cu. Localization of the Cu 3d states
also leads to weak screening of Cu 2p and 3s states, which accounts for shifts
in the core 2p and 3s spectra of the transition metal atoms. Calculations
indicate that the ground-state magnetic ordering, which varies across the
series is largely dependent on the occupation of the metal 3d shell and that
structural differences in the superexchange pathways for different compounds
play a secondary role.
