Empirical Evidence for A‐Site Order in Perovskites
Models for composition–structure relationships are useful in both the lab and industry, yet few exist for perovskites‐containing extrinsic defects or cation ordering. In this work, an empirical model is used to predict the existence of A‐site cation ordering. Specifically, four compositions in the N...
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| Published in | Journal of the American Ceramic Society Vol. 100; no. 1; pp. 429 - 442 |
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| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
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| Abstract | Models for composition–structure relationships are useful in both the lab and industry, yet few exist for perovskites‐containing extrinsic defects or cation ordering. In this work, an empirical model is used to predict the existence of A‐site cation ordering. Specifically, four compositions in the Na(1−3x)/2La(1+x)/2TiO3 system (x = 0.0, 0.0533, 0.1733 and 0.225) were synthesized using a conventional solid‐state mixed‐oxide method. The structure of the x = 0 end‐member (Na0.5La0.5TiO3) has been reported in various space groups, but always with a random distribution of Na+ and La3+ on the A site; however, empirical modeling suggests that it is not only ordered but also that a small volume increase accompanies the ordering process. While no evidence of long‐range A‐site ordering is observed in this composition via X‐ray or neutron diffraction, electron‐diffraction data indicate short‐range ordering of Na+ and La3+ ions, with the degree of cation ordering decreasing (but the scale of ordered domains and degree of vacancy ordering generally increasing) with increasing x. First‐principles calculations via density functional theory support both conclusions that short‐range ordering in Na0.5La0.5TiO3 is stable and that it results in a volume increase with respect to the disordered analog. A similar analysis has been conducted for the Li(1−3x)/2La(1+x)/2TiO3 and Na(1−3x)/2La(1+x)/2(Mg0.5W0.5)O3 solid solutions. These systems provide additional validation of the accuracy and versatility of the empirical modeling method used. |
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| AbstractList | Models for composition–structure relationships are useful in both the lab and industry, yet few exist for perovskites‐containing extrinsic defects or cation ordering. In this work, an empirical model is used to predict the existence of A‐site cation ordering. Specifically, four compositions in the Na(1−3x)/2La(1+x)/2TiO3 system (x = 0.0, 0.0533, 0.1733 and 0.225) were synthesized using a conventional solid‐state mixed‐oxide method. The structure of the x = 0 end‐member (Na0.5La0.5TiO3) has been reported in various space groups, but always with a random distribution of Na+ and La3+ on the A site; however, empirical modeling suggests that it is not only ordered but also that a small volume increase accompanies the ordering process. While no evidence of long‐range A‐site ordering is observed in this composition via X‐ray or neutron diffraction, electron‐diffraction data indicate short‐range ordering of Na+ and La3+ ions, with the degree of cation ordering decreasing (but the scale of ordered domains and degree of vacancy ordering generally increasing) with increasing x. First‐principles calculations via density functional theory support both conclusions that short‐range ordering in Na0.5La0.5TiO3 is stable and that it results in a volume increase with respect to the disordered analog. A similar analysis has been conducted for the Li(1−3x)/2La(1+x)/2TiO3 and Na(1−3x)/2La(1+x)/2(Mg0.5W0.5)O3 solid solutions. These systems provide additional validation of the accuracy and versatility of the empirical modeling method used. Models for composition-structure relationships are useful in both the lab and industry, yet few exist for perovskites-containing extrinsic defects or cation ordering. In this work, an empirical model is used to predict the existence of A-site cation ordering. Specifically, four compositions in the Na(1-3x)/2La(1+x)/2TiO3 system (x = 0.0, 0.0533, 0.1733 and 0.225) were synthesized using a conventional solid-state mixed-oxide method. The structure of the x = 0 end-member (Na0.5La0.5TiO3) has been reported in various space groups, but always with a random distribution of Na+ and La3+ on the A site; however, empirical modeling suggests that it is not only ordered but also that a small volume increase accompanies the ordering process. While no evidence of long-range A-site ordering is observed in this composition via X-ray or neutron diffraction, electron-diffraction data indicate short-range ordering of Na+ and La3+ ions, with the degree of cation ordering decreasing (but the scale of ordered domains and degree of vacancy ordering generally increasing) with increasing x. First-principles calculations via density functional theory support both conclusions that short-range ordering in Na0.5La0.5TiO3 is stable and that it results in a volume increase with respect to the disordered analog. A similar analysis has been conducted for the Li(1-3x)/2La(1+x)/2TiO3 and Na(1-3x)/2La(1+x)/2(Mg0.5W0.5)O3 solid solutions. These systems provide additional validation of the accuracy and versatility of the empirical modeling method used. Models for composition–structure relationships are useful in both the lab and industry, yet few exist for perovskites‐containing extrinsic defects or cation ordering. In this work, an empirical model is used to predict the existence of A‐site cation ordering. Specifically, four compositions in the Na (1−3 x )/2 La (1+ x )/2 TiO 3 system ( x = 0.0, 0.0533, 0.1733 and 0.225) were synthesized using a conventional solid‐state mixed‐oxide method. The structure of the x = 0 end‐member (Na 0.5 La 0.5 TiO 3 ) has been reported in various space groups, but always with a random distribution of Na + and La 3+ on the A site; however, empirical modeling suggests that it is not only ordered but also that a small volume increase accompanies the ordering process. While no evidence of long‐range A‐site ordering is observed in this composition via X‐ray or neutron diffraction, electron‐diffraction data indicate short‐range ordering of Na + and La 3+ ions, with the degree of cation ordering decreasing (but the scale of ordered domains and degree of vacancy ordering generally increasing) with increasing x . First‐principles calculations via density functional theory support both conclusions that short‐range ordering in Na 0.5 La 0.5 TiO 3 is stable and that it results in a volume increase with respect to the disordered analog. A similar analysis has been conducted for the Li (1−3 x )/2 La (1+ x )/2 TiO 3 and Na (1−3 x )/2 La (1+ x )/2 (Mg 0.5 W 0.5 )O 3 solid solutions. These systems provide additional validation of the accuracy and versatility of the empirical modeling method used. Models for composition-structure relationships are useful in both the lab and industry, yet few exist for perovskites-containing extrinsic defects or cation ordering. In this work, an empirical model is used to predict the existence of A-site cation ordering. Specifically, four compositions in the Na sub((1-3x)/2)La sub((1+x)/2)TiO sub(3) system (x = 0.0, 0.0533, 0.1733 and 0.225) were synthesized using a conventional solid-state mixed-oxide method. The structure of the x = 0 end-member (Na sub(0.5)La sub(0.5)TiO sub(3)) has been reported in various space groups, but always with a random distribution of Na super(+) and La super(3+) on the A site; however, empirical modeling suggests that it is not only ordered but also that a small volume increase accompanies the ordering process. While no evidence of long-range A-site ordering is observed in this composition via X-ray or neutron diffraction, electron-diffraction data indicate short-range ordering of Na super(+) and La super(3+) ions, with the degree of cation ordering decreasing (but the scale of ordered domains and degree of vacancy ordering generally increasing) with increasing x. First-principles calculations via density functional theory support both conclusions that short-range ordering in Na sub(0.5)La sub(0.5)TiO sub(3) is stable and that it results in a volume increase with respect to the disordered analog. A similar analysis has been conducted for the Li sub((1-3x)/2)La sub((1+x)/2)TiO sub(3) and Na sub((1-3x)/2)La sub((1+x)/2)(Mg sub(0.5) W sub(0.5))O sub(3) solid solutions. These systems provide additional validation of the accuracy and versatility of the empirical modeling method used. |
| Author | Liu, Bing Ubic, Rick Williamson, Izaak Tolman, Kevin Dickey, E. Chen, Xiang Ming Bedke, Katherine Li, Lan Nelson, Eric B. |
| Author_xml | – sequence: 1 givenname: Kevin surname: Tolman fullname: Tolman, Kevin email: kevintolman@boisestate.edu organization: Boise State University – sequence: 2 givenname: Rick surname: Ubic fullname: Ubic, Rick organization: Boise State University – sequence: 3 givenname: Bing surname: Liu fullname: Liu, Bing organization: Zhejiang University – sequence: 4 givenname: Izaak surname: Williamson fullname: Williamson, Izaak organization: Boise State University – sequence: 5 givenname: Katherine surname: Bedke fullname: Bedke, Katherine organization: Boise State University – sequence: 6 givenname: Eric B. surname: Nelson fullname: Nelson, Eric B. organization: Boise State University – sequence: 7 givenname: Lan surname: Li fullname: Li, Lan organization: Center for Advanced Energy Studies – sequence: 8 givenname: Xiang Ming surname: Chen fullname: Chen, Xiang Ming organization: Zhejiang University – sequence: 9 givenname: E. surname: Dickey fullname: Dickey, E. |
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| CitedBy_id | crossref_primary_10_1111_jace_20264 crossref_primary_10_1021_acs_inorgchem_4c04267 crossref_primary_10_1016_j_jallcom_2020_156106 crossref_primary_10_1111_jace_16695 crossref_primary_10_1111_jace_16168 crossref_primary_10_1016_j_jallcom_2017_11_333 crossref_primary_10_1016_j_materresbull_2025_113318 |
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| Snippet | Models for composition–structure relationships are useful in both the lab and industry, yet few exist for perovskites‐containing extrinsic defects or cation... Models for composition-structure relationships are useful in both the lab and industry, yet few exist for perovskites-containing extrinsic defects or cation... |
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| SubjectTerms | Cations Ceramics Density functional theory Diffraction Empirical analysis Mathematical models modeling/model Modelling Neutron diffraction Order disorder Perovskite perovskites Solid solutions vacancies |
| Title | Empirical Evidence for A‐Site Order in Perovskites |
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