Local structure and order-disorder transitions in "empty" ferroelectric tetragonal tungsten bronzes

Jason A. McNulty; David Pesquera; Jonathan Gardner; Andrei Rotaru; Helen Y. Playford; Matthew G. Tucker; Michael A. Carpenter; Finlay D. Morrison

doi:10.1021/acs.chemmater.0c02639

Local structure and order-disorder transitions in "empty" ferroelectric tetragonal tungsten bronzes

Jason A. McNulty, David Pesquera, Jonathan Gardner, Andrei Rotaru, Helen Y. Playford, Matthew G. Tucker, Michael A. Carpenter, Finlay D. Morrison^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

Abstract

The ‘empty’ tetragonal tungsten bronze Ba₄La_0.67 _1.33Nb₁₀O₃₀ displays both relaxor-like and normal dielectric anomalies as a function of temperature; the former is associated with loss of ferroelectricity and was proposed to originate from anion disordering [Chem. Mater., 2016, 28, 4616-4627]. Here we present total neutron scattering and pair distribution function (PDF) analysis which shows an increase in the distribution of oxygen-oxygen distances at the relaxor transition and which supports the proposed anion disordering mechanism. The disordering process can be destabilised by reducing the average A-cation size (i.e. Nd-doping: Ba₄(La_1-xNd_x)_0.67Nb₁₀O₃₀); this introduces a more strongly propagating tilt system in line with the previously reported crystal-chemical framework model [Chem. Mater., 2015, 27, 3250-3261]. Mechanical loss data obtained using resonant ultrasound spectroscopy also indicate destabilisation of the disordering process with increasing Nd-substitution.

Original language	English
Pages (from-to)	8492-8501
Journal	Chemistry of Materials
Volume	32
Issue number	19
Early online date	9 Sept 2020
DOIs	https://doi.org/10.1021/acs.chemmater.0c02639
Publication status	Published - 13 Oct 2020

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10.1021/acs.chemmater.0c02639

McNulty TTB-disorder accepted
Copyright © 2020 American Chemical Society. This work has been made available online in accordance with publisher policies or with permission. Permission for further reuse of this content should be sought from the publisher or the rights holder. This is the author created accepted manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at https://doi.org/10.1021/acs.chemmater.0c02639
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Cite this

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title = "Local structure and order-disorder transitions in {"}empty{"} ferroelectric tetragonal tungsten bronzes",

abstract = "The {\textquoteleft}empty{\textquoteright} tetragonal tungsten bronze Ba4La0.67 1.33Nb10O30 displays both relaxor-like and normal dielectric anomalies as a function of temperature; the former is associated with loss of ferroelectricity and was proposed to originate from anion disordering [Chem. Mater., 2016, 28, 4616-4627]. Here we present total neutron scattering and pair distribution function (PDF) analysis which shows an increase in the distribution of oxygen-oxygen distances at the relaxor transition and which supports the proposed anion disordering mechanism. The disordering process can be destabilised by reducing the average A-cation size (i.e. Nd-doping: Ba4(La1-xNdx)0.67Nb10O30); this introduces a more strongly propagating tilt system in line with the previously reported crystal-chemical framework model [Chem. Mater., 2015, 27, 3250-3261]. Mechanical loss data obtained using resonant ultrasound spectroscopy also indicate destabilisation of the disordering process with increasing Nd-substitution.",

author = "McNulty, {Jason A.} and David Pesquera and Jonathan Gardner and Andrei Rotaru and Playford, {Helen Y.} and Tucker, {Matthew G.} and Carpenter, {Michael A.} and Morrison, {Finlay D.}",

note = "JAM would like to acknowledge the School of Chemistry, University of St Andrews for the allocation of a PhD studentship through the EPSRC doctoral training grant (EP/K503162/1). AR would like to acknowledge support through the Strategic Grant POSDRU/159/1.5/S/133255, Project ID 133255 (2014), co-financed by the European Social Fund within the Sectorial Operational Program Human Resources Development 2007–2013 and also the University of Craiova and University of Cambridge for the mobility grant “Resonant ultrasound spectroscopy. (RUS) characterization of dielectric and ferroelectric tetragonal tungsten bronzes”. The work carried out at the University of St Andrews and University of Cambridge is part of an EPSRC- funded collaboration (EP/P02453X/1 and EP/P024904/1).",

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language = "English",

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T1 - Local structure and order-disorder transitions in "empty" ferroelectric tetragonal tungsten bronzes

AU - McNulty, Jason A.

AU - Pesquera, David

AU - Gardner, Jonathan

AU - Rotaru, Andrei

AU - Playford, Helen Y.

AU - Tucker, Matthew G.

AU - Carpenter, Michael A.

AU - Morrison, Finlay D.

N1 - JAM would like to acknowledge the School of Chemistry, University of St Andrews for the allocation of a PhD studentship through the EPSRC doctoral training grant (EP/K503162/1). AR would like to acknowledge support through the Strategic Grant POSDRU/159/1.5/S/133255, Project ID 133255 (2014), co-financed by the European Social Fund within the Sectorial Operational Program Human Resources Development 2007–2013 and also the University of Craiova and University of Cambridge for the mobility grant “Resonant ultrasound spectroscopy. (RUS) characterization of dielectric and ferroelectric tetragonal tungsten bronzes”. The work carried out at the University of St Andrews and University of Cambridge is part of an EPSRC- funded collaboration (EP/P02453X/1 and EP/P024904/1).

PY - 2020/10/13

Y1 - 2020/10/13

N2 - The ‘empty’ tetragonal tungsten bronze Ba4La0.67 1.33Nb10O30 displays both relaxor-like and normal dielectric anomalies as a function of temperature; the former is associated with loss of ferroelectricity and was proposed to originate from anion disordering [Chem. Mater., 2016, 28, 4616-4627]. Here we present total neutron scattering and pair distribution function (PDF) analysis which shows an increase in the distribution of oxygen-oxygen distances at the relaxor transition and which supports the proposed anion disordering mechanism. The disordering process can be destabilised by reducing the average A-cation size (i.e. Nd-doping: Ba4(La1-xNdx)0.67Nb10O30); this introduces a more strongly propagating tilt system in line with the previously reported crystal-chemical framework model [Chem. Mater., 2015, 27, 3250-3261]. Mechanical loss data obtained using resonant ultrasound spectroscopy also indicate destabilisation of the disordering process with increasing Nd-substitution.

AB - The ‘empty’ tetragonal tungsten bronze Ba4La0.67 1.33Nb10O30 displays both relaxor-like and normal dielectric anomalies as a function of temperature; the former is associated with loss of ferroelectricity and was proposed to originate from anion disordering [Chem. Mater., 2016, 28, 4616-4627]. Here we present total neutron scattering and pair distribution function (PDF) analysis which shows an increase in the distribution of oxygen-oxygen distances at the relaxor transition and which supports the proposed anion disordering mechanism. The disordering process can be destabilised by reducing the average A-cation size (i.e. Nd-doping: Ba4(La1-xNdx)0.67Nb10O30); this introduces a more strongly propagating tilt system in line with the previously reported crystal-chemical framework model [Chem. Mater., 2015, 27, 3250-3261]. Mechanical loss data obtained using resonant ultrasound spectroscopy also indicate destabilisation of the disordering process with increasing Nd-substitution.

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U2 - 10.1021/acs.chemmater.0c02639

DO - 10.1021/acs.chemmater.0c02639

M3 - Article

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SP - 8492

EP - 8501

JO - Chemistry of Materials

JF - Chemistry of Materials

IS - 19

ER -

Local structure and order-disorder transitions in "empty" ferroelectric tetragonal tungsten bronzes

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