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Supplementary information Room temperature multiferrocity and magnetodielectric properties of ternary (1-x) (0.94Bi 0.5 Na 0.5 TiO 3 - 0.06BaTiO 3 ) - xBiFeO 3 (0 ≤ x ≤ 0.9) solid solutions W. J. Huang, 1, 2 J. Yang, 1, a) Y. F. Qin, 1, 2 P. Xiong, 1, 2 D. Wang, 1, 2 L. H. Yin, 1 X. W. Tang, 1 W. H. Song, 1 P. Tong, 1 X. B. Zhu, 1 and Y. P. Sun 3, 1, 4 1 Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, People’s Republic of China 2 University of Science and Technology of China, Hefei 230026, People’s Republic of China 3 High Magnetic Field Laboratory, Chinese Academy of Sciences, Hefei 230031, People’s Republic of China 4 Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, People’s Republic of China

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Supplementary information

Room temperature multiferrocity and magnetodielectric

properties of ternary (1-x) (0.94Bi0.5Na0.5TiO3 - 0.06BaTiO3) -

xBiFeO3 (0 ≤ x ≤ 0.9) solid solutions

W. J. Huang,1, 2 J. Yang,1, a) Y. F. Qin,1, 2 P. Xiong,1, 2 D. Wang,1, 2 L. H. Yin,1 X. W. Tang,1 W. H.

Song,1 P. Tong,1 X. B. Zhu,1 and Y. P. Sun3, 1, 4

1Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of

Sciences, Hefei 230031,

People’s Republic of China

2 University of Science and Technology of China, Hefei 230026, People’s Republic of China

3 High Magnetic Field Laboratory, Chinese Academy of Sciences, Hefei 230031, People’s

Republic of China

4 Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing

210093,

People’s Republic of China

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a) Author to whom correspondence should be addressed. Electronic mail: [email protected]

Fig. S1. XRD patterns of the (1–x) BNBT–xBFO (0≤x≤0.9) ceramics.

Fig. S2. XRD patterns of the (1–x) BNBT–xBFO ceramics in the 2θ ranges of 37.5–41.5 and

44.5–48.5.

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Fig. S3. Temperature dependence of the zero-field-cooled (ZFC) and field-cooled (FC) magnetization for the BNBT-BFO ceramics with x = 0.7. This is done by cooling the sample from 410 K to 5 K in H=0, and then a magnetic field of 1000 Oe was applied and the moment was measured as a function of temperature from 5 to 360 K during the warming process. This is the ZFC part. Next, the sample is cooled in a magnetic field of 1000 Oe to 5 K, and again the moment was measured as a function of temperature during the warming process. This is the FC part. The inset shows first derivative of magnetization with respect to temperature (dM/dT).

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Fig. S4. Temperature dependence of dielectric loss tanδ at different frequencies in the range of 1 -

100 kHz for the samples with (a) x = 0.1, (b) x = 0.3, (c) x = 0.6 (d) x = 0.7, (e) x = 0.8, (f) x = 0.9

Fig. S5. The combined temperature vs. concentration diagram of magnetic and dielectric

phase. The four Néel temperatures are obtained from Ref. 10 of the main paper.

Fig. S6. Arrhenius plot of relaxation frequency vs. temperature for the BNBT–xBFO ceramics.

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Fig. S7. Representative SEM images of (1–x) (0.94Bi0.5Na0.5TiO3–0.06BaTiO3) – xBiFeO3 with (a)

0.05, (b) 0.3, (c) 0.6, (d) 0.8

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TABLE S1. The comparison of remanent polarization (Pr), remanent magnetization (Mr),

magnetodielectric (MD) effect, and critical temperature with reported data on other lead-free

BFO-based ceramics at 300 K.

CeramicsPr

(μC/cm2)

Mr

(emu/g)

MD

(%)

critical

temperature (K)Ref.

BiFeO3 ~12 6

BiFeO3 ~19 34

BiFeO3-PbFe0.5Nb0.5O3-

PbTiO3

~21 TC:423~573 31

(1-x)Na0.5Bi0.5TiO3-xBiFeO3 0.11Td: ~473

TC: 623~793

17,

27

(1-x)Na0.5Bi0.5TiO3-xBiFeO3 30-35 0.12Td: 477~586

TC: 604~676

18,

19

0.722BiFeO3-0.275BaTiO3-

0.03Na0.5Bi0.5TiO3

27.4 0.19 TC: 876 20

(1-x)(0.94Na0.5Bi0.5TiO3-

0.06BaTiO3)-

xBiFeO3(0~0.15)

23Td: 393

TC: 535~585

14,

15

(1-x)BiTi(1-y)/2FeyMg(1-y)/2O3-

xCaTiO3

49.9 16

Bi1-xLaxFeO3 32 0.09 1.2(8T,300Hz) 7

(1-x)(0.94Na0.5Bi0.5TiO3-

0.06BaTiO3)-

xBiFeO3(0~0.9)

44.7 0.160.07

(8T,300Hz)

Td: 400

TC: 600-890

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