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[SupportingDocs-Iodine doped.docx](https://mdr.nims.go.jp/filesets/ca88a35e-ea8d-4e6e-90e8-b14bdf73f9dc/download)
## Creator
Raphael Fortulan, [Sima Aminorroaya Yamini](https://orcid.org/0000-0002-2312-8272), Azib Juri, [Illia Serhiienko](https://orcid.org/0000-0002-3072-9412), [Takao Mori](https://orcid.org/0000-0003-2682-1846)
## Rights
This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in ACS Applied Electronic Materials, copyright © 2024 American Chemical Society after peer review. To access the final edited and published work see https://doi.org/10.1021/acsaelm.3c01615[In Copyright](http://rightsstatements.org/vocab/InC/1.0/)
## Other metadata
[Thermoelectric Properties of Single-Phase n-Type Bi14Te13S8](https://mdr.nims.go.jp/datasets/ce68af8f-db61-42d1-ae1f-08b39f1aa27a)
## Fulltext
Supporting file Figure S1 XRD patterns of Fe2+xVAl1-x with x = 0, 0.03, 0.05, and 0.1 before annealing (just after SPS) in a powder form. These data were collected using MiniFlex Cr-source (λ = 2.2909 Å) and converted into a Cu-source (λ = 1.54 Å) XRD patterns. Figure S2 Rietveld refinement of Fe2VAl annealed at 1330 C (a) with 25% occupation exchange between V and Al, and (b) with varying occupancy of V & Al.Table S1 The goodness of fit (weighted profile R-factor (Rwp) and Chi2) and lattice parameter obtained from Rietveld refinement of Fe2VAl (ann. 1330C) by exchanging the occupation of Al and V. A clear improvement in fitting was noticed, reflecting in goodness of fit. VAl or AlV Rwp Chi2 a (Å) 0% 10.2 2.582 5.7624 10% 9.44 2.208 5.7624 20% 9.07 2.045 5.7624 25% 9.02 2.022 5.7624 30% 9.07 2.045 5.7624Table S2 The obtained parameters from Rietveld refinement of powder XRD data for annealed samples, Fe2+xVAl1-x; x = 0, 0.03, 0.05 and 0.1. Errors are written in parentheses. Sample code Chi2 Rwp a (Å) Volume (Å3) Mass density (g/cm3) x = 0 (Ann. 1330C) 2.582 10.2 5.7624(1) 191.34 6.58 x = 0.03 (Ann. 1330C) 2.514 11.4 5.7711(1) 192.21 6.78 x = 0.05(Ann. 1330C) 3.997 12.4 5.7727(1) 192.37 6.96 x = 0.1(Ann. 1330C) 3.025 12.7 5.7775(1) 192.85 7.37 Fe2VAl (Ann. 1375C) 3.524 10.9 5.7772(1) 192.82 6.53 Figure S3 (a-d) field dependence of magnetization collected at various temperatures, the temperature dependence of (e-h) magnetization M and 𝜕M/𝜕T collected at H = 0.1T, which gives transition temperature TC, and (i-k) M and H/M collected at H = 1T which gives Qurie temperature θ for all Fe2+xVAl1-x samples, where x is written on the figures. (l) The obtained Qurie temperature θ for x = 0, 0.05, 0.1 and 0.125.Figure S4 Rhodes-Wohlfarth plot for ferromagnetic compounds, including some magnetic Heusler-type compounds [3,45,46]. In ferromagnetic compounds, pC/pS is nearly equal to 1 for localized moment systems and greater than 1 for itinerant electron systems. Compounds with pC/pS>>1 are classified as weak ferromagnets. We plotted the obtained pC/pS of studied Fe-doped Fe2VAl samples in the Rhodes-Wohlfarth plot, falling in the weak ferromagnet region. Table S3 Obtained parameters from magnetization study of Fe2+xVAl1-x. x TC (K) ps (μB/Fe) θ (K) C (emu-K/mol-Oe) peff (μB/Fe) pc (μB/Fe) pc/ps 0 40.1 0.132 53.9 0.584 1.528 0.826 6.241 0.03 53.1 0.165 0.05 114.5 0.260 131.7 1.800 2.650 1.832 7.040 0.10 223 0.410 226.7 5.186 4.444 3.555 8.669 0.125 240 0.423 243.4 4.206 3.979 3.102 7.333 Figure S5 Temperature dependence of electrical resistivity (a-c), Seebeck coefficient (d-f), thermoelectric power factor (g-i), -S/T vs T plot (j-l) and thermal conductivity (m-p) at H = 0 T and 7T for Fe2+xVAl1-x where x = 0-0.1, are written in the figures.Figure S6 (a) Plot of ρxy/H versus M/H which gives R0 and RS through linear fitting. Temperature dependence of (b) carrier mobility and (b) anomalous Hall coefficient for Fe2.1VAl0.1. Figure S7 Temperature dependence of Seebeck coefficient (a) including both low and high T measured data and (b) after adding a constant correction factor of 10 μV/K in high T data for Fe doped samples, i.e., x = 0.03, 0.05 and 0.1 which aligned the high T data with low T and included in multiband model fitting for contentment of low temperature S-fitting. Figure S8 Multiband model fitting of temperature-dependent Seebeck coefficient x = 0.05 (a) and x =0.1 (b), and electrical resistivity of all Fe2+xVAl1-x; x = 0-0.1 (c).Figure S9 Magneto-transport of Fe2VAl annealed at 1375 oC. (a) Magnetic field dependence of magnetization M at T = 2 K and (b) temperature dependence of M and 𝜕M/𝜕T measured at H = 0.1 T. The temperature dependence of (c) Seebeck coefficient and (d) –S/T versus T plot at H =0 T and 7 T. Table S4 Obtained parameters from multi-band model fitting of thermoelectric data. Here EF is representing the position of Fermi level with respect to top of valence band. Similarly, Eg1 and Eg2 are represent the energy gap between the top of the valence band to the bottom 1st and 2nd conduction bands, respectively. In this modeling, the DOS effective mass of the valence band is taken at m1 = -1, which doesn’t affect the EF and band gaps. The relative mass of the 1st and 2nd conduction bands are denoted by m1 and m2, respectively. We have considered acoustic phonon scattering and alloy scattering in electrical resistivity and obtained the pre-factor (K) and temperature exponent (r), where r = 0 and 1 for acoustic and alloy scattering, respectively [2]. EF, Eg1 and Eg2 and given in K, which can be converted into eV by multiplying kB (8.61733e-5 eV/K). Fe2+xVAl1-x No. of Bands EF(K) Eg1(K) Eg2(K) m1 m2 m3 K1 K2 r1 r2 x = 0 2 1110.07 761.93 -1 2.5 3 1110.07 1115.22 43.15 -1 2.5 15.69 1e-6.92 1e-26.78 0 0.859 x = 0.03 2 1019.87 556 -1 2.52 3 1019.87 1028.59 -142.45 -1 2.52 12.16 1e-2.67 1e-26.86 0 0.857 x = 0.05 2 1053.43 357 -1 2.6 3 1053.43 1104.79 -473.91 -1 2.6 10.71 1e-8.11 1e-26.78 0 0.812 x = 0.1 2 1076 688.8 -1 2.4 3 1075.97 1484 -853.66 -1 2.4 7.537 1e-2.47 1e-26.69 0 0.781 Figure S10 Temperature dependence of (a) electronic thermal conductivity κe and (b) lattice thermal conductivity κL for all Fe-doped Fe2VAl samples. image4.tiffimage5.tiffimage6.tiffimage7.tiffimage8.tiffimage9.tiffimage10.tiffimage11.tiffimage12.tiffimage13.tiffimage14.tiffimage15.tiffimage16.emf0 200 400 600 800 100002468101214 This work, Fe2+xVAl1-x x = 0 x = 0.05 x = 0.10 x = 0.125Sc-InPd-Rh-FeNi-CuFeNiMnBiFeBMnSbCo-BCrTeGdCrB3Pd2MnSn (FeCo)Si Pb-Fe Pb-Co Pb-Ni Fe2V0.9Cr0.1Al0.9Si0.1 Fe2.2V0.8Al1-ySiypC/pSTC (K)ZrZn2EuOoleObject4.binimage17.emf0 50 100 150 200 250 300789101112(a) at 7T at 0T (m)T (K)x = 0oleObject5.binimage18.emf0 50 100 150 200 250 300789101112 x = 0.03 7 T 0 T(-m)T (K)(b)oleObject6.binimage19.emf0 50 100 150 200 250 3006.06.57.07.58.08.59.0 x = 0.05(c)(-m)T (K) 7 T 0 ToleObject7.binimage20.emf0 50 100 150 200 250 300-125-100-75-50-250 x = 0(d) at 7T at 0TS (V/K)T (K)oleObject8.binimage21.emf0 50 100 150 200 250 300-100-80-60-40-200 x = 0.03(e)T (K)S (V/K) 7 T 0 ToleObject9.binimage22.emf0 50 100 150 200 250 300-100-80-60-40-200 x = 0.05(f) 7 T 0 TS (V/K)T (K)oleObject10.binimage23.emf0 50 100 150 200 250 3000.00.51.01.52.0 x = 0(g) at 7T at 0TS2/ (mW/mK2)T (K)oleObject11.binimage24.emf0 50 100 150 200 250 3000.00.40.81.2x = 0.03(h) 7 T 0 TT (K)S2/ (mW/mK2)oleObject12.binimage1.emf20 30 40 50 60 70 80x = 0x = 0.03x = 0.05x = 0.10Intensity (arb. unit)2 (deg)image25.emf0 50 100 150 200 250 3000.00.20.40.60.81.01.2 x = 0.05(i) 7 T 0 TT (K)S2/ (mW/mK2)oleObject13.binimage26.emf0 50 100 150 200 250 3000.40.50.60.70.80.9x = 0(j) at 7T at 0T-S/T (V/K2)T (K)oleObject14.binimage27.emf0 50 100 150 200 250 3000.30.40.50.60.7(k)T (K)-S/T (V/K2) 7 T 0 Tx = 0.03oleObject15.binimage28.emf0 50 100 150 200 250 3000.250.300.350.400.45x = 0.05(l) 7 T 0 T-S/T (V/K2)T (K)oleObject16.binimage29.emf0 50 100 150 200 250 30005101520x = 0(m) at 7T at 0T (W/mK)T (K)oleObject17.binoleObject1.binimage30.emf0 50 100 150 200 250 300048121620 (n)T (K) 7 T 0 T (W/mK)x = 0.03 oleObject18.binimage31.emf0 50 100 150 200 250 300024681012141618(o) 7 T 0 TT (K) (W/mK)x = 0.05oleObject19.binimage32.emf0 50 100 150 200 250 30003691215(p) (W/mK)T (K) 0 T 7 Tx = 0.1oleObject20.binimage33.tiffimage34.tiffimage35.tiffimage36.tiffimage2.emf20 30 40 50 60 70 80 90VAl & AlV = 25%(511)(422)(420)(331)(400)(222)(311)(220)(200)(111)Intensity (arb. unit)2 (deg) I_obs (Fe2VAl_1330C) I_cal (I_obs - I_cal) Bragg's peaks(a)image37.tiffimage38.tiffimage39.tiffimage40.tiffimage41.tiffimage42.tiffimage43.tiffimage44.tiffimage45.emf0 50 100 150 200 250 3000.00.51.01.52.02.53.0(a) Fe2VAl (Ann. 1375C)e (W/mK)T (K) x = 0 x = 0.03 x = 0.05 x = 0.10 Fe2+xVAl1-x (1330C)oleObject21.binoleObject2.binimage46.emf0 50 100 150 200 250 30004812162024 (b) x = 0 x = 0.03 x = 0.05 x = 0.10L (W/mK)T (K)Fe2+xVAl1-x (Ann. 1330C) Fe2VAl (Ann. 1375C)oleObject22.binimage47.emf0 50 100 150 200 250 3000.000.020.040.060.080.10 (c)T (K)Fe2+xVAl1-x (Ann. 1330C) x = 0 x = 0.03 x = 0.05 x = 0.10oleObject23.binimage3.emf20 25 30 35(b)VAl & AlV(I_obs - I_cal)I_cal(200)(111) I_obs (Fe2VAl_1330C) Bragg's peaksIntensity (arb. unit)2 (deg) 0% 10% 20% 30 %oleObject3.bin