KO2 exhibits concomitant antiferromagnetic (AFM) and structural transitions,
both of which originate from the open-shell 2p electrons of O2−
molecules. The structural transition is accompanied by the coherent tilting of
O2− molecular axes. The interplay among the spin-orbital-lattice
degrees of freedom in KO2 is investigated by employing the first-principles
electronic structure theory and the kinetic-exchange interaction scheme. We
have shown that the insulating nature of the high symmetry phase of KO2 at high
temperature (T) arises from the combined effect of the spin-orbit coupling and
the strong Coulomb correlation of O 2p electrons. In contrast, for the low
symmetry phase of KO2 at low T with the tilted O2− molecular axes, the
band gap and the orbital ordering are driven by the combined effects of the
crystal-field and the strong Coulomb correlation. We have verified that the
emergence of the O 2p ferro-orbital ordering is essential to achieve the
observed AFM structure for KO2