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Fujii et al. Microstructures 2023;3:2023045  https://dx.doi.org/10.20517/microstructures.2023.43   Page 5 of 14





























                Figure 2. P-E loops measured at room temperature for (A) undoped BaTiO  ceramics with a grain size of 1.2 µm and 76 µm, (B)
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                undoped BaTiO  ceramics sintered at 10  atm pO  and 10  atm  pO , (C) formulated BaTiO  ceramics sintered 10  atm pO  and 10
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                atm pO , and (D) model MLCCs with various grain sizes. The ac frequency was 10 Hz.
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                Figure 3. Temperature and the ac field dependence of the dielectric constant of a BaTiO  ceramics with a grain size of 1.2 mm. The ac
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                field frequency was 100 Hz. The peaks in the permittivity correspond to the phase transition in BaTiO ; on increasing temperature, the
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                material transforms from a rhombohedral ferroelectric to an orthorhombic ferroelectric to a tetragonal ferroelectric to a paraelectric
                cubic structure.
               nonlinearity is observed in the rhombohedral, orthorhombic, and tetragonal ferroelectric phases of BaTiO .
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               Although not shown here, the domain wall motion contributions to the small signal properties are gradually
               lost as the temperature approaches 0 K .
                                                [29]

               The magnitude of the temperature dependence of the extrinsic contributions to the properties is a function
               of the grain size of the ceramics, as can be seen in comparing the data in Figures 3-5 (Figure 3 uses the same
               data as Figure 5, and Figure 5 has more data). Figure 4 shows selected data for the dielectric nonlinearity for
               a large-grained (76 mm average grain size) BaTiO  ceramics. One consequence of the increased domain wall
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               mobility in large-grained materials is that the electric fields at which the materials transition from Rayleigh-
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