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1 Supplementary Information Structural manipulation and tailoring of dielectric properties in SrTi -x Fe x Ta x O 3 perovskites: Design of new lead free relaxors R. Shukla, S. J. Patwe, S. K. Deshpande 2, S. N. Achary, P. S. R. Krishna 3, A. B. Shinde 3, J. Gopalakrishnan 4 and A. K. Tyagi * Chemistry Division, Bhabha Atomic Research Centre, Mumbai-485, India 2 UGC-DAE Consortium for Scientific Research, Bhabha Atomic Research Centre, Mumbai-485, India 3 Solid State Physics Division, Bhabha Atomic Research Centre, Mumbai-485, India 4 Solid State and Structural Chemistry Unit, Indian Institute of Science, Bangalore-56 2 India
2 Supplementary Tables Table S: Refined structural parameters of selected SrTi -2x Fe x Ta x O 3 (. x ) compositions. (PND: Powder Neutron diffraction, XRD: powder XRD data) (a). for. x.75 (Cubic solid solution); C: Cubic (Pm3m); Sr: (,,); Ti: (½,½,½);O: (½,½,) (b). for.333 x (Orthorhombic solid solution); O: Orthorhombic (Pbnm) Sr: (x,y,¼); M: (½,, ½); O: (x,y,z); O2: (x,y,¼) (c). for. x.25 (Coexisting Cubic and Orthorhombic solid solution) Table S2: Typical inter-atomic distances (Å) and angles ( o ) in SrTi -2x Fe x Ta x O 3 compositions. Supplementary Figures Fig. S-I(a-j). Rietveld refinement plot of powder neutron diffraction data for SrTi -2x Fe x Ta x O 3 (a). Rietveld refinement plot for x =. (SrTi. Fe. Ta. O 3 ). Cubic (Pm3m) (b). Rietveld refinement plot for x =.5 (SrTi.95 Fe.25 Ta.25 O 3 ). Cubic (Pm3m) (c).rietveld refinement plot for x =.5 (SrTi.9 Fe.5 Ta.5 O 3 ). Cubic (Pm3m). (d).rietveld refinement plot for x =.75 (SrTi.85 Fe.75 Ta.75 O 3 ). Cubic (Pm3m) (e).rietveld refinement plot for x =. (SrTi.8 Fe. Ta. O 3 ) (vertical ticks for Bragg position: Cubic (upper) and Orthorhombic (lower)) (f).rietveld refinement plot for x =.25 (SrTi.75 Fe.25 Ta.25 O 3 ), (vertical ticks for Bragg position: Cubic (upper) and Orthorhombic (lower)) (g).rietveld refinement plot for x =.25 (SrTi Fe.25 Ta.25 O 3 ), (vertical ticks for Bragg position: Cubic (upper) and Orthorhombic (lower)) (h).rietveld refinement plot for x =.333 (SrTi.333 Fe.333 Ta.333 O 3 ): Orthorhombic (Pbnm) (i).rietveld refinement plot for x =.375 (SrTi.25 Fe.375 Ta.375 O 3 ): Orthorhombic (Pbnm) (j).rietveld refinement plot for x = (SrTi. Fe Ta O 3 ): Orthorhombic (Pbnm) Figure S-II: Polarization vs Electric field loops of cubic solid solution phases of SrTi - 2xFe x Ta x O 3 (. x.75) compositions. Measured at the frequency 5 Hz and at ambient temperature by using Aixacct TF2 (Aixacct GmbH, Germany) ferroelectric analyzer.
3 Table S: Refined structural parameters of selected SrTi -2x Fe x Ta x O 3 (. x ) compositions. (PND: Powder Neutron diffraction, XRD: powder XRD data) (a). for. x.75 (Cubic solid solution); : C: Cubic (Pm3m); Sr: (,,); Ti: (½,½,½);O: (½,½,) Sr x = Data PND PND PND PND Phase C C C C Str. Pm3m Pm3m Pm3m Pm3m B (Å) 2 (2) Ti/Fe/Ta Occ (Ti:Fe:Ta).:.:. B (Å) 2.9(4) O.74(3).95:.25:.25.25(5).77(3).9:.5:.5.(5) 3(4).85:.75:.75.6(6) B(Å) 2.6(2).74(2).85(2).98(2) a (Å) 3.949() 3.978() 3.96() 3.96() V (Å) (3) 59.85(3) 6.55(4) Rp Rwp Rexp χ R B
4 (b). for.333 x (Orthorhombic solid solution);, O: Orthorhombic (Pbnm) Sr (x,y,¼); M: (½,, ½); O: (x,y,z); O2 : (x,y,¼) x = Data PND PND XRD XRD PND Phase O O O O O Str. Pbnm Pbnm Pbnm Pbnm Pbnm Sr (x,y,/4) B (Å) 2 Ti/Fe/Ta (/2,,/2) Occ (Ti:Fe:Ta) B (Å) 2 O O2 B(Å) 2 B(Å) 2 a (Å) b (Å) c (Å).69(5).93(5).25.84(2).33:.33:.33.76(3).2435(4).2455(4).9(3).65(2).9573(4) 54(6).25.53(7) 5.65() 5.58() 7.888().8(5).3(5).25.79(2).25:.375: (3).242(4).2446(4).2(3).67(3).959(5) 67(6).25.25(8) 5.6() 5.585() 7.898(2) -.3(8).36(6).25.2:.4:.4.248(8).2442(8).52(6) -.959(9) 3(7).25.9(6).72(3).25 -.:.45: (8).2443(8).45(6) (8) 4(4).25 - B ov :.42() (Å) 2 B ov :.42() (Å) () 5.67() () 5.668() 7.932() 7.924().53(5).29(5).25.83(2).:: 9(2).2386(4).247(4).59(3).63(4).9525(5) 99(6).25.3() 5.69() 5.66() 7.928(2) V (Å) () 247.5() 248.7() () 25.2() R p, R wp, R exp, χ 2.64, 2.36, 2.3, , 3.4,.92, , 8.2,.9, , 8.2, 9.9, , 3.68, 2.2, 3.32 R B
5 (c). for. x.25 (Coexisting Cubic and Orthorhombic solid solution) x = Data PND PND PND Phase C O C O C O Str. Pm3m Pbnm* Pm3m Pbnm Pm3m Pbnm Wt.(%) 98() % 2()% 53() 47() 22() 78 Sr (x,y,z) B (Å) 2 Ti/Fe/Ta Occ (Ti:Fe:Ta) B (Å) 2 O (4).8:.:.: :.7:.7 5(5).8:.:..87(8).9(8).6(2).66(2):.7(2):.7(2).84(5).8:.: (2).2(5) 8.3(6) 8(2).2(6).44(3) (7).2436(5) (7).2453(5).66.66(6).9(7) B(Å) 2.3(2).4).7(7).4().64(5).94(3) O (9).96(5) 39 39() 5(7) B(Å) (2).96(4) a (Å) 3.996(2) (2) 5.597(2) () 5.67(2) b (Å) 3.996(2) (2) 5.543(2) () (2) c (Å) 3.996(2) (2) 7.848(4) () (4) V (Å) (4) () 243.5(2) 6.498() 246.2(5) R p, R wp, χ , 5.3, , 3.3, , 5.8, 7.7 R B * Structural parameters observed at x =.25 were used..46(2):.22(2):.22(2)
6 Table S2: Typical inter-atomic distances (Å) and angles ( o ) in SrTi -2x Fe x Ta x O 3 compositions. x = Str. Pm3m Pm3 Pm3m Pm3 Pm3 Pm3m Pbnm Pm3 Pbnm Pbnm Pbnm Pbnm m m m m M-O (2).972(2).972(2) M-O (2).992(2).987(2) M-O ().993().987(3) M-O ().986().982() <M-O> Distortion Sr-O (3) 2.64(3) 2.656(3) Sr-O (3) 2.895(3) 2.868(3) Sr-O (3) 2.775(3) 2.772(3) Sr-O (3) 2.877(3) 2.879(3) Sr-O (4) 2.83(4) 2.826(4) Sr-O (4) 2.79(4) 2.782(4) Sr-O (4) 2.58(4) 2.62(4) Sr-O (4) 3.3(4) 3.4(4) Sr-O () 2.8() 2.797() <Sr-O> Distortion: Ti-O-Ti () 73.73() 74.4(9) M-O-M 64.34(6) 65.29(6) 66.5(2) M-O2-M
7 Supplementary Figures Fig. S-I(a). Rietveld refinement plot for x =. (SrTi. Fe. Ta. O 3 ). Cubic (Pm3m) Fig. S-I(b). Rietveld refinement plot for x =.5 (SrTi.95 Fe.25 Ta.25 O 3 ). Cubic (Pm3m)
8 Fig. S-I(c).Rietveld refinement plot for x =.5 (SrTi.9 Fe.5 Ta.5 O 3 ). Cubic (Pm3m). Fig. S-I(d).Rietveld refinement plot for x =.75 (SrTi.85 Fe.75 Ta.75 O 3 ). Cubic (Pm3m)
9 Fig. S-I(e).Rietveld refinement plot for x =. (SrTi.8 Fe. Ta. O 3 ) (vertical ticks for Bragg position: Cubic (upper) and Orthorhombic (lower)) Fig. S-I(f).Rietveld refinement plot for x =.25 (SrTi.75 Fe.25 Ta.25 O 3 ), (vertical ticks for Bragg position: Cubic (upper) and Orthorhombic (lower))
10 Fig. S-I(g).Rietveld refinement plot for x =.25 (SrTi Fe.25 Ta.25 O 3 ), (vertical ticks for Bragg position: Cubic (upper) and Orthorhombic (lower)) Fig. S-I(h).Rietveld refinement plot for x =.333 (SrTi.333 Fe.333 Ta.333 O 3 ): Orthorhombic (Pbnm)
11 Fig. S-I(i).Rietveld refinement plot for x =.375 (SrTi.25 Fe.375 Ta.375 O 3 ): Orthorhombic (Pbnm) Fig. S-I(j).Rietveld refinement plot for x = (SrTi. Fe Ta O 3 ): Orthorhombic (Pbnm) ( vertical ticks for Bragg position)
12 Figure S-II: Polarization vs Electric field loops of cubic solid solution phases of SrTi -2x Fe x Ta x O 3 (. x.75) compositions. Measured at the frequency 5 Hz and at ambient temperature by using Aixacct TF2 (Aixacct GmbH, Germany) ferroelectric analyzer.
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