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CeMnNi$_4$ exhibits an unusually large spin polarization, but its origin hasbaffled researchers for more than a decade. We use bulk sensitive hard x-rayphotoelectron spectroscopy (HAXPES) and density functional theory based on theGreen's function technique to demonstrate the importance of electron-electroncorrelations of both the Ni 3$d$ ($U_{Ni}$) and Mn 3$d$ ($U_{Mn}$) electrons inexplaining the valence band of this multiply correlated material. We show thatMn-Ni anti-site disorder as well as $U_{Ni}$ play crucial role in enhancing itsspin polarization: anti-site disorder broadens a Ni 3$d$ minority-spin peakclose to the Fermi level ($E_F$), while an increase in $U_{Ni}$ shifts ittowards $E_F$, both leading to a significant increase of minority-spin statesat $E_F$. Furthermore, rare occurrence of a valence state transition betweenthe bulk and the surface is demonstrated highlighting the importance of HAXPESin resolving the electronic structure of materials unhindered by surfaceeffects.

Influence of anti-site disorder and electron-electron correlations on the electronic structure of CeMnNi$_4$