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Quantum critical points in ferroelectric relaxors : stuffed tungsten bronze K3Li2Ta5O15 and lead pyrochlore (Pb2Nb2O7)

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PhysRevMaterials.2.084409.pdf (3.954Mb)
Date
08/2018
Author
Smith, Rebecca Mary
Gardner, Jonathan
Morrison, Finlay D.
Rowley, S. E.
Ferraz, Catarina
Carpenter, M. A.
Chen, Jiasheng
Hodkinson, Jack
Dutton, Siân E.
Scott, James Floyd
Keywords
Ferroelectricity
Dielectric properties
Quantum criticality
Relaxor ferroelectrics
QC Physics
TK Electrical engineering. Electronics Nuclear engineering
DAS
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Abstract
We have synthesized ceramic specimens of the tetragonal tungsten bronze K3Li2Ta5O15 (KLT) and characterized its phase transition via X-ray diffraction, dielectric permittivity, resonant ultrasonic spectroscopy, and heat capacity measurements. The space group of KLT is reported as both P4/mbm and Cmmm with the orthorhombic distortion occurring when there are higher partial pressures of volatile K and Li used inside the closed crucibles for the solid state synthesis. The data show strong relaxor behavior, with the temperature at which the two dielectric relative permittivity peaks decreasing, with 104 ≥ Tm1 ≥ 69 K and 69 ≥ Tm2 ≥ 46 K as probe frequency f is reduced from 1 MHz to 316 Hz. F tests show that the data satisfies a Vogel-Fulcher model better than Arrhenius with an extrapolated freezing temperature for ε’ and ε” of Tf1 = +15.8 and –11.8 K and Tf2 = –5.0 and –15.0 K for f -> 0 (tending to dc). This difference between Tf from real and imaginary values, albeit counterintuitive, is mandatory, according to the theory of Tagantsev. Therefore, by tuning frequency, the transition could be shifted to absolute zero, suggesting KLT has a relaxor-type quantum critical point. In addition, we have reanalyzed the conflicting literature for Pb2Nb2O7 pyrochlore which suggests that this also has a relaxor-type quantum critical point since the freezing temperature from the Vogel-Fulcher fitting is below absolute zero. Since the transition temperature evidenced in the dielectric data at approximately 100 kHz shifts below 0 K for very low frequencies, this transition would not be seen with heat capacity data collected in the zero-frequency (dc) limit. Both of these materials show promise for possible new relaxor-type quantum critical points with non-perovskite based structures.
Citation
Smith , R M , Gardner , J , Morrison , F D , Rowley , S E , Ferraz , C , Carpenter , M A , Chen , J , Hodkinson , J , Dutton , S E & Scott , J F 2018 , ' Quantum critical points in ferroelectric relaxors : stuffed tungsten bronze K 3 Li 2 Ta 5 O 15 and lead pyrochlore (Pb 2 Nb 2 O 7 ) ' , Physical Review Materials , vol. 2 , no. 8 , 084409 . https://doi.org/10.1103/PhysRevMaterials.2.084409
Publication
Physical Review Materials
Status
Peer reviewed
DOI
https://doi.org/10.1103/PhysRevMaterials.2.084409
ISSN
2475-9953
Type
Journal article
Rights
© 2018, American Physical Society. This work has been made available online in accordance with the publisher’s policies. This is the author created accepted version manuscript following peer review and as such may differ slightly from the final published version. The final published version of this work is available at https://doi.org/10.1103/PhysRevMaterials.2.084409
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  • University of St Andrews Research
URI
http://hdl.handle.net/10023/15896

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