Chemical nature of giant strain in Mn-doped 0.94(Na0.5Bi0.5)(4)

will result in theflattening of the free energy profile and increase the distortion of[(Ti,Mn)O6]octahedral(i.e. Jahn–Teller distortion)by lengthening the off-center dis-placement in the perovskite structure.However,the im-provedfield-induced strain in VS cannot be attributed to this mechanism because the size of Mn3+(0.58A˚)ions is close to Ti4+(0.61A˚)ions.The“charge effect”model is proposed to explain the enhancedfield-induced strain in

VS samples.The formation of½Mn00

Ti ÀV

O

defect di-

poles will introduce a tetragonal crystalfield and en-hance the tetragonality,i.e.the c/a ratio.Upon the application of an externalfield,these defect dipoles act as anisotropy centers and promote the development of a0a0c+in-phase octahedral tilted regions[38].Therefore, when a sufficient high externalfield is applied,a large ionic displacement accompanied byfield-induced phase transition can be expected.

In summary,the chemical nature of the giantfield-in-duced strain of Mn:NBBT6single crystals was systemat-ically studied.The concentrations of oxygen vacancies in OS and VS samples decrease and increase,respectively. XPS results reveal that different local coordination envi-ronments for Na+and Bi3+ions coexist in the crystal lattice.However,only one oxidation state presents for titannate,i.e.Ti4+.The Mn2+ions substitute Ti4+at the B-site and act as acceptors in the as-grown single crystals.They were partly oxidized to Mn4+in OS,

and form½Mn00

Ti ÀV

O

defect dipoles in VS.Based on

these results,“size effect”and“charge effect”models were proposed to explain the improvedfield-induced strains in OS and VS samples,respectively.

This work wasfinancially supported by the Ministry of Science and Technology of China through 973Program(Nos.2013CB632902-3,2009CB623305, 2013CB6329052and2013CB632906),the Natural Science Foundation of China(Nos.51332009,51372258, 11304333,61001041,11090332and51272268),Science and Technology Commission of Shanghai Municipality (No.12DZ0501000),Shanghai Rising-Star Program (No.11QA1407500),Open Project from Shanghai Insti-tute of Technical Physics,CAS(No.IIMDKFJJ-11–08), the Fund of Shanghai Institute of Ceramics(No. Y29ZC4140G and Y39ZC4140G)and Shanghai Muni-cipal Electric Power Company(No.52091413502W).

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