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We report photoemission experiments revealing the valence electron spectralfunction of Mn, Fe, Co and Ni atoms on the Ag(100) surface. The series ofspectra shows splittings of higher energy features which decrease with thefilling of the 3d shell and a highly non-monotonous evolution of spectralweight near the Fermi edge. First principles calculations demonstrate that twomanifestations of Hund's exchange $J$ are responsible for this evolution.First, there is a monotonous reduction of the effective exchange splittingswith increasing filling of the 3d shell. Second, the amount of chargefluctuations and, thus, the weight of quasiparticle peaks at the Fermi levelvaries non-monotonously through this 3d series due to a distinct occupancydependence of effective charging energies $U_{\rm eff}$.

Excitation spectra of transition metal atoms on the Ag (100) surface controlled by Hund's exchange