  Unrestricted Hartree-Fock calculations on La0.5Ca0.5MnO3 and La0.33Ca0.67MnO3
in the full magnetic unit cell show that the magnetic ground states of these
compounds consist of 'ferromagnetic molecules' or polarons ordered in
herring-bone patterns. Each polaron consists of either three or five Mn ions
separated by O- ions with a magnetic moment opposed to those of the Mn ions.
Ferromagnetic coupling within the polarons is strong while coupling between
them is relatively weak. Magnetic moments on the Mn ions range between 3.8 and
3.9 Bohr magnetons in La0.5Ca0.5MnO3 and moments on the O- ions are -0.7 Bohr
magnetons. Each polaron has a net magnetic moment of 7.0 Bohr magnetons, in
good agreement with recently reported magnetisation measurements from electron
microscopy. The polaronic nature of the electronic structure reported here is
obviously related to the Zener polaron model recently proposed for
Pr0.6Ca0.4MnO3 on the basis of neutron scattering data.
