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Main Authors: Tragheim, Ben R. M., Simpson, Struan, Liu, En-Pei, Senn, Mark S., Chen, Wei-Tin
Format: Preprint
Published: 2024
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Online Access:https://arxiv.org/abs/2410.08836
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author Tragheim, Ben R. M.
Simpson, Struan
Liu, En-Pei
Senn, Mark S.
Chen, Wei-Tin
author_facet Tragheim, Ben R. M.
Simpson, Struan
Liu, En-Pei
Senn, Mark S.
Chen, Wei-Tin
contents The novel series of hole-doped quadruple manganite perovskites Hg$_{1-x}$Na$_x$Mn$_3$Mn$_4$O$_{12}$ (HNMO) has been synthesized and its charge and orbital order behavior investigated through high-resolution synchrotron powder x-ray diffraction techniques. Through careful Rietveld refinements of structural models $via$ symmetry-motivated approaches, we show that the ground state of HNMO compositions adopts a polar $G$-type charge and orbital ordered state, which is rare in manganite perovskites, and is robust as a sole phase up to a critical doping level. Upon this critical doping, coincident with that in which colossal magnetoresistance (CMR) is maximal in canonical manganite perovskites, electronic phase separation occurs between $G$-type and orbital order with charge disorder-type states. The latter state has recently been identified in Ca$_{1-x}$Na$_x$Mn$_3$Mn$_4$O$_{12}$ perovskites, and proposed to be the competing insulating state from which CMR phenomena emerges. We show the mechanism for the formation of the $G$-type state is due to charge transfer processes which may occur through a coupling of distortions involving structural and charge and orbital degrees of freedom, ultimately driving the polar ground state through an improper-like ferroelectric polarization mechanism. These results will act as an important recipe for designing novel ferroelectric-active materials, in addition to expanding the richness of charge and orbital ordered states in manganite perovskites.
format Preprint
id arxiv_https___arxiv_org_abs_2410_08836
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Intrinsic electronic phase separation and competition between $G$-type, $C$-type and $CE$-type charge and orbital ordering modes in Hg$_{1-x}$Na$_x$Mn$_3$Mn$_4$O$_{12}$
Tragheim, Ben R. M.
Simpson, Struan
Liu, En-Pei
Senn, Mark S.
Chen, Wei-Tin
Strongly Correlated Electrons
The novel series of hole-doped quadruple manganite perovskites Hg$_{1-x}$Na$_x$Mn$_3$Mn$_4$O$_{12}$ (HNMO) has been synthesized and its charge and orbital order behavior investigated through high-resolution synchrotron powder x-ray diffraction techniques. Through careful Rietveld refinements of structural models $via$ symmetry-motivated approaches, we show that the ground state of HNMO compositions adopts a polar $G$-type charge and orbital ordered state, which is rare in manganite perovskites, and is robust as a sole phase up to a critical doping level. Upon this critical doping, coincident with that in which colossal magnetoresistance (CMR) is maximal in canonical manganite perovskites, electronic phase separation occurs between $G$-type and orbital order with charge disorder-type states. The latter state has recently been identified in Ca$_{1-x}$Na$_x$Mn$_3$Mn$_4$O$_{12}$ perovskites, and proposed to be the competing insulating state from which CMR phenomena emerges. We show the mechanism for the formation of the $G$-type state is due to charge transfer processes which may occur through a coupling of distortions involving structural and charge and orbital degrees of freedom, ultimately driving the polar ground state through an improper-like ferroelectric polarization mechanism. These results will act as an important recipe for designing novel ferroelectric-active materials, in addition to expanding the richness of charge and orbital ordered states in manganite perovskites.
title Intrinsic electronic phase separation and competition between $G$-type, $C$-type and $CE$-type charge and orbital ordering modes in Hg$_{1-x}$Na$_x$Mn$_3$Mn$_4$O$_{12}$
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2410.08836