Polar Antiferromagnets Produced with Orbital-Order

Polar magnetic states are realized in pseudocubic manganite thin films fabricated on high-index substrates, in which a Jahn-Teller (JT) distortion remains an active variable. Several types of orbital-orders were found to develop large optical second harmonic generation, signaling broken-inversion-symmetry distinct from their bulk forms and films on (100) substrates. The observed symmetry-lifting and first-principles calculation both indicate that the modified JT q2 mode drives Mn-site off-centering upon orbital order, leading to the possible cooperation of "Mn-site polarization" and magnetism.