Large‐scale quantum chemical modeling of the phase transitions in KTN solid solutions
作者:
R. I. Eglitis,
D. Fuks,
S. Dorfman,
E. A. Kotomin,
G. Borstel,
V. A. Trepakov,
期刊:
AIP Conference Proceedings
(AIP Available online 1903)
卷期:
Volume 677,
issue 1
页码: 231-240
ISSN:0094-243X
年代: 1903
DOI:10.1063/1.1609958
出版商: AIP
数据来源: AIP
摘要:
The large‐scale modeling of the atomic and electronic structure of KNbxTa1−xO3(KTN) perovskite solid solutions is performed using the Intermediate Neglect of the Differential Overlap (INDO) method based on the Hartree‐Fock formalism. It is found that periodic Nb impurities in KTaO3reveal coherent off‐center displacements already at the smallest calculated concentration,x=0.125. The calculated magnitude of 〈 111 〉 Nb off‐center displacement is 0.27 a.u., which is close to the XAFS observation at 70 K andx=0.09. In contrast, Ta impurities in KNbO3remain on‐center, due to higher ionicity of Ta, as compared to Nb. Using the calculated energy gain caused by the off‐center displacements of Nb atoms, the non‐empirical Ginzburg‐Landau‐Devonshire functional with concentration‐dependent coefficients is constructed. Analysis of INDO results for several Nb concentrations in KTN allows calculate the lowest critical Nb concentration,xcr=0.025, corresponding to the quantum displacive limit for the paraelectric‐ferroelectric transition at 0 K. This value is only slightly higher than the experimental one. © 2003 American Institute of Physics
点击下载:
PDF
(626KB)
返 回