Charge orbital and spin ordering transitions in La1-Sr MnO3+δ (x = 0.67 & 0.71)

Abstract Structural and magnetic phase-transitions in La1-xSrxMnO3+δ (x = 0.67 & 0.71) have been studied employing x-ray diffraction, neutron diffraction and transmission electron microscopy (TEM) in conjunction with electrical-transport and magnetic studies. These studies reveal a cubic to incommensurate (IC) charge-ordered (CO) tetragonal phase-transition in both the samples with k-vector varying with temperature and thus indicates charge density wave-like nature. Followed by magnetic transition from paramagnetic phase to incommensurate antiferromagnetic phase. The nearly equal expansion of the a,b axes in the ab plane and the contraction of the c-axis (i.e. type-I Jahn-Teller distortion (JTD)) indicate that the CO is accompanied by a planer ferro-ordering of 3 d x 2 − y 2 orbitals in the ab plan, which is different from haring-bone type ordering of 3 d 3 x 2 − r 2 / 3 d 3 y 2 − r 2 orbitals, commonly observed in narrow bandwidth CO manganites. For x = 0.71, a second phase-transition from type-I JTD-CO phase (c   a) was observed. Through EDAX analysis in TEM, a nano-scale marginal composition difference has been observed to lead to nanoscale phase-coexistence. These studies have revealed first microscopic evidence of CO and nano-scale multiphase coexistence in La1-xSrxMnO3-δ with x = 0.67 & 0.71.