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Electron diffraction analysis, nuclear magnetic resonance measurements, structure determinations and refinements were performed on two ferroelectric lead-containing ceramics (classical and relaxor), with tetragonal tungsten bronze structure, in order to investigate the origin of the relaxor behaviour in such compounds. In both compounds the lead atoms are found to be off-centred in the CN (coordination number) 15 (A2) site. The main difference between the two compositions is the proportion of lead in this site: in the relaxor composition, the A2 site is at least half occupied by lead atoms. Disorder in the repartition of lead and potassium atoms in the A1 (CN 12) and A2 sites was also studied via combinatorial calculations to correlate the evolution of the relaxor behaviour in the Pb5Ta10O30-Li10Ta10O30-K10Ta10O30 ternary system with composition. The combinatorial study demonstrated that the relaxor behaviour is enhanced by the disorder in cationic repartition.

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