Manganite charge and orbitally ordered and disordered states probed by Fe substitution into Mn site in LnBaMn1.96Fe0.04O5, LnBaMn1.96Fe0.04O6 and LnBaMn1.96Fe0.04O5.5 (Ln=Y, Gd, Sm, Nd, Pr, La)

TL;DR

This study investigates how Fe substitution affects charge and orbital order in layered manganites with varying Ln elements, revealing suppression of transition temperatures and insights into Fe site preferences through structural and Mössbauer analysis.

Contribution

It provides detailed analysis of Fe substitution effects on charge and orbital ordering and structural transitions in LnBaMn2O5, 5.5, 6 compounds, including site preferences and domain segmentation.

Findings

Fe substitution suppresses structural and magnetic transition temperatures.

Charge and orbital orderings are confirmed by quadrupole splitting increases.

Most Fe species are undifferentiated, indicating site preference and domain segmentation.

Abstract

The layered manganese oxides LnBaMn1.96Fe0.04Oy (Ln=Y, Gd, Sm, Nd, Pr, La) have been synthesized for y=5, 5.5 and 6. In the oxygen-saturated state (y=6) they exhibit the charge and orbital order at ambient temperature for Ln=Y, Gd, Sm, but unordered eg-electronic system for Ln=La,Pr,Nd. Fourfold increase of quadrupole splitting was observed owing to the charge and orbital ordering. This is in agreement with the jumplike increase in distortion of the reduced perovskite-like cell for the charge and orbitally ordered manganites compared to the unordered ones. Substitution of 2 percents of Mn by Fe suppresses the temperatures of structural and magnetic transitions by 20 to 50 K. Parameters of the crystal lattices and the room-temperature M\"{o}ssbauer spectra were studied on forty samples whose structures were refined within five symmetry groups: P4/mmm, P4/nmm, Pm-3m, Icma and P2/m. Overwhelming majority of the Fe species are undifferentiated in the M\"{o}ssbauer spectra for most of the samples. Such the single-component spectra in the two-site structures are explained by the preference of Fe towards the site of Mn(III) and by the segmentation of the charge and orbitally ordered domains.