Structural relaxation of ferroelectric phase in hard sodium lithium niobate solid solutions studied by solid-state NMR

Abstract Hard sodium lithium niobate (LNN) solid solutions offer a promising environmentally benign alternative to lead-based ferroelectric materials for electronic devices. A major challenge in their practical application is that their ferroelectric phase relaxes over a timescale ranging from weeks...

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Main Authors: Millena Logrado, Changhao Zhao, Hergen Breitzke, Jürgen Rödel, Gerd Buntkowsky
Format: Article
Language:English
Published: Nature Portfolio 2025-08-01
Series:Scientific Reports
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Online Access:https://doi.org/10.1038/s41598-025-15554-z
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author Millena Logrado
Changhao Zhao
Hergen Breitzke
Jürgen Rödel
Gerd Buntkowsky
author_facet Millena Logrado
Changhao Zhao
Hergen Breitzke
Jürgen Rödel
Gerd Buntkowsky
author_sort Millena Logrado
collection DOAJ
description Abstract Hard sodium lithium niobate (LNN) solid solutions offer a promising environmentally benign alternative to lead-based ferroelectric materials for electronic devices. A major challenge in their practical application is that their ferroelectric phase relaxes over a timescale ranging from weeks to years to an orthorhombic phase, limiting their long-term performance. In order to understand the structural changes in the relaxation process, high mechanical quality factor Li x Na1−x NbO3 solid-solutions were deliberately stored under ambient conditions for 24 months, without any specialized hermetic protection, to assess their stability over time. We utilized 1D and 2D 23Na solid-state Nuclear Magnetic Resonance (ssNMR) to investigate short-range structural changes in the 24-months-old aged and unaged Li x Na1−x NbO3 solid-solutions. NMR results reveal a system with phase-changes as a function of aging time and temperature. The samples exhibit a multiphase structure compromised of crystalline R and Q orthorhombic domains, along with two types of amorphous regions. A significant amount of ferroelectric phase persists in the ceramics after 24 months of exposure to ambient conditions. A structural model based on short-range order of sodium was suggested and agrees well with the lattice parameter of the freshly prepared samples.
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spelling doaj-art-942e2d1193a0461cb584cc07cb03cc652025-08-24T11:19:14ZengNature PortfolioScientific Reports2045-23222025-08-011511910.1038/s41598-025-15554-zStructural relaxation of ferroelectric phase in hard sodium lithium niobate solid solutions studied by solid-state NMRMillena Logrado0Changhao Zhao1Hergen Breitzke2Jürgen Rödel3Gerd Buntkowsky4Department of Chemistry, Eduard-Zintl Institute for Inorganic and Physical Chemistry, Technical University of DarmstadtState Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering, Xi’an Jiaotong UniversityDepartment of Chemistry, Eduard-Zintl Institute for Inorganic and Physical Chemistry, Technical University of DarmstadtDivision of Nonmetallic-Inorganic Materials, Department of Materials and Earth Sciences, Technical University of DarmstadtDepartment of Chemistry, Eduard-Zintl Institute for Inorganic and Physical Chemistry, Technical University of DarmstadtAbstract Hard sodium lithium niobate (LNN) solid solutions offer a promising environmentally benign alternative to lead-based ferroelectric materials for electronic devices. A major challenge in their practical application is that their ferroelectric phase relaxes over a timescale ranging from weeks to years to an orthorhombic phase, limiting their long-term performance. In order to understand the structural changes in the relaxation process, high mechanical quality factor Li x Na1−x NbO3 solid-solutions were deliberately stored under ambient conditions for 24 months, without any specialized hermetic protection, to assess their stability over time. We utilized 1D and 2D 23Na solid-state Nuclear Magnetic Resonance (ssNMR) to investigate short-range structural changes in the 24-months-old aged and unaged Li x Na1−x NbO3 solid-solutions. NMR results reveal a system with phase-changes as a function of aging time and temperature. The samples exhibit a multiphase structure compromised of crystalline R and Q orthorhombic domains, along with two types of amorphous regions. A significant amount of ferroelectric phase persists in the ceramics after 24 months of exposure to ambient conditions. A structural model based on short-range order of sodium was suggested and agrees well with the lattice parameter of the freshly prepared samples.https://doi.org/10.1038/s41598-025-15554-zPrecipitatesLNNNMRLiNbO3
spellingShingle Millena Logrado
Changhao Zhao
Hergen Breitzke
Jürgen Rödel
Gerd Buntkowsky
Structural relaxation of ferroelectric phase in hard sodium lithium niobate solid solutions studied by solid-state NMR
Scientific Reports
Precipitates
LNN
NMR
LiNbO3
title Structural relaxation of ferroelectric phase in hard sodium lithium niobate solid solutions studied by solid-state NMR
title_full Structural relaxation of ferroelectric phase in hard sodium lithium niobate solid solutions studied by solid-state NMR
title_fullStr Structural relaxation of ferroelectric phase in hard sodium lithium niobate solid solutions studied by solid-state NMR
title_full_unstemmed Structural relaxation of ferroelectric phase in hard sodium lithium niobate solid solutions studied by solid-state NMR
title_short Structural relaxation of ferroelectric phase in hard sodium lithium niobate solid solutions studied by solid-state NMR
title_sort structural relaxation of ferroelectric phase in hard sodium lithium niobate solid solutions studied by solid state nmr
topic Precipitates
LNN
NMR
LiNbO3
url https://doi.org/10.1038/s41598-025-15554-z
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