A Local Atomic Mechanism for Monoclinic-Tetragonal Phase Boundary Creation in Li-Doped Na0.5K0.5NbO3 Ferroelectric Solid Solution.

Kong, J; Li, L; Liu, J; Marlton, FP; Jørgensen, MRV; Pramanick, A

A Local Atomic Mechanism for Monoclinic-Tetragonal Phase Boundary Creation in Li-Doped Na0.5K0.5NbO3 Ferroelectric Solid Solution.

Kong, J Li, L Liu, J Marlton, FP Jørgensen, MRV Pramanick, A

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Publisher:: American Chemical Society (ACS)
Publication Type:: Journal Article
Citation:: Inorg Chem, 2022, 61, (10), pp. 4335-4349
Issue Date:: 2022-03-14

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Field	Value	Language
dc.contributor.author	Kong, J
dc.contributor.author	Li, L
dc.contributor.author	Liu, J
dc.contributor.author	Marlton, FP
dc.contributor.author	Jørgensen, MRV
dc.contributor.author	Pramanick, A
dc.date.accessioned	2023-04-13T20:16:05Z
dc.date.available	2023-04-13T20:16:05Z
dc.date.issued	2022-03-14
dc.identifier.citation	Inorg Chem, 2022, 61, (10), pp. 4335-4349
dc.identifier.issn	0020-1669
dc.identifier.issn	1520-510X
dc.identifier.uri	http://hdl.handle.net/10453/169776
dc.description.abstract	ABO3 perovskites display a wide range of phase transitions, which are driven by A/B-site centered polyhedral distortions and/or BO6 octahedral tilting. Since heterogeneous substitutions at the A/B-site can locally alter both polyhedral distortions and/or tilting, they are often used to create phase boundary regions in solid solutions of ABO3, where the functional properties are highly enhanced. However, the relationships between doping-induced atomistic structural changes and the creation of phase boundaries are not always clear. One prominent example of this is the Li-doped K0.5Na0.5NbO3 (KNNL), which is considered a promising alternative to traditional Pb-based ferroelectrics. Although the electromechanical properties of KNNL are enhanced for compositions near the morphotropic phase boundary (MPB), the atomistic mechanism for phase transitions is not well understood. Here, we combined neutron total scattering experiments and density functional theory to investigate the long-range average and short-range (∼10 Å) structural changes in KNNL. We show that the average monoclinic-to-tetragonal (M-T) transition across the MPB in KNNL can be described as an order-disorder-type change, which is driven by competition between a longer-range polarization field of monoclinic structural units and local distortions of the disordered AO12 polyhedra. The current study demonstrates a way to clarify dopant-induced local distortions near phase boundaries in complex solid solution systems, which will be important for the rational design of new environmentally sustainable ferroelectrics.
dc.format	Print-Electronic
dc.language	eng
dc.publisher	American Chemical Society (ACS)
dc.relation.ispartof	Inorg Chem
dc.relation.isbasedon	10.1021/acs.inorgchem.1c03501
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	0302 Inorganic Chemistry, 0306 Physical Chemistry (incl. Structural), 0399 Other Chemical Sciences
dc.subject.classification	Inorganic & Nuclear Chemistry
dc.title	A Local Atomic Mechanism for Monoclinic-Tetragonal Phase Boundary Creation in Li-Doped Na0.5K0.5NbO3 Ferroelectric Solid Solution.
dc.type	Journal Article
utslib.citation.volume	61
utslib.location.activity	United States
utslib.for	0302 Inorganic Chemistry
utslib.for	0306 Physical Chemistry (incl. Structural)
utslib.for	0399 Other Chemical Sciences
pubs.organisational-group	/University of Technology Sydney
pubs.organisational-group	/University of Technology Sydney/Faculty of Science
pubs.organisational-group	/University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
utslib.copyright.status	closed_access	*
dc.date.updated	2023-04-13T20:16:02Z
pubs.issue	10
pubs.publication-status	Published
pubs.volume	61
utslib.citation.issue	10

Abstract:

ABO3 perovskites display a wide range of phase transitions, which are driven by A/B-site centered polyhedral distortions and/or BO6 octahedral tilting. Since heterogeneous substitutions at the A/B-site can locally alter both polyhedral distortions and/or tilting, they are often used to create phase boundary regions in solid solutions of ABO3, where the functional properties are highly enhanced. However, the relationships between doping-induced atomistic structural changes and the creation of phase boundaries are not always clear. One prominent example of this is the Li-doped K0.5Na0.5NbO3 (KNNL), which is considered a promising alternative to traditional Pb-based ferroelectrics. Although the electromechanical properties of KNNL are enhanced for compositions near the morphotropic phase boundary (MPB), the atomistic mechanism for phase transitions is not well understood. Here, we combined neutron total scattering experiments and density functional theory to investigate the long-range average and short-range (∼10 Å) structural changes in KNNL. We show that the average monoclinic-to-tetragonal (M-T) transition across the MPB in KNNL can be described as an order-disorder-type change, which is driven by competition between a longer-range polarization field of monoclinic structural units and local distortions of the disordered AO12 polyhedra. The current study demonstrates a way to clarify dopant-induced local distortions near phase boundaries in complex solid solution systems, which will be important for the rational design of new environmentally sustainable ferroelectrics.

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