Effect of sintering temperature on the chemical bonding, electronic structure and electrical transport properties of β-Ga1.9Fe0.1O3 compounds

doi:10.1016/j.jmst.2020.05.072

Abstract

Abstract:

A model system, which is based on iron (Fe) doped gallium oxide (Ga₂O₃) (Ga_1.9Fe_0.1O₃), has been considered to elucidate the combined effect of transition-metal ion doping and processing temperature on the chemistry, local structure and chemical bonding, and electrical transport properties of a wide band gap oxide (Ga₂O₃). The Ga_1.9Fe_0.1O₃ compounds were synthesized using standard high-temperature solid state reaction method. The effect of processing conditions in terms of different calcination and sintering environments on the structural and electrical properties of Ga_1.9Fe_0.1O₃ compounds is studied in detail. Structural characterization by Raman spectroscopy revealed that Ga_1.9Fe_0.1O₃ compounds exhibit monoclinic crystal symmetry, which is quite similar to the intrinsic parental crystal structure, though Fe-doping induces lattice strain. Sintering temperature (T_sint) which was varied in the range of 900-1200 °C, has significant impact on the structure, chemical bonding, and electrical properties of Ga_1.9Fe_0.1O₃ compounds. Raman spectroscopic measurements indicate the proper densification of the Ga_1.9Fe_0.1O₃ compounds achieved through complete Fe diffusion into the parent Ga₂O₃ lattice which is evident at the highest sintering temperature. The X-ray photoelectron spectroscopy validates the chemical states of the constituent elements in Ga_1.9Fe_0.1O₃ compounds. The electrical properties of Ga_1.9Fe_0.1O₃ fully controlled by T_sint, which governed the grain size and microstructural evolution. The temperature and frequency dependent electrical measurements demonstrated the salient features of the Fe doped Ga₂O₃ compounds. The activation energy determined from Arrhenius equation is ~0.5 eV. The results demonstrate that control over structure, morphology, chemistry and electrical properties of the Ga_1.9Fe_0.1O₃ compounds can be achieved by optimizing T_sint.

Key words: Ga₂O₃ compounds, Fe-doping, Raman spectroscopy, Chemical bonding, Electrical properties

Swadipta Roy, C.V. Ramana. Effect of sintering temperature on the chemical bonding, electronic structure and electrical transport properties of β-Ga_1.9Fe_0.1O₃ compounds[J]. J. Mater. Sci. Technol., 2021, 67: 135-144.

Figures/Tables 11

Fig. 1. a). Raman spectra of differently sintered GFO compounds.b). Representative case of Raman spectral peak-fitting procedure. The data shown are for GFO sample sintered at 1200 °C. The peak fitting procedure has been indicated for different frequency regions of the spectrum collected.c). Expanded region of the Raman peak corresponding to Fe-O bonding. It is evident that the sintering temperature strongly influences the evolution of Fe-O bonds in GFO compounds. The peak corresponding to Fe-O bonding completely disappears for the samples sintered under optimum sintering temperature.

Table 1 Raman data for Ga1.9Fe0.1O3 ceramics at various Tsint. The data of Ga1.9Fe0.1O3 ceramics is compared with that of bulk Ga2O3.

Serial No.	Mode Symmetry	Rao et al [29].		This Work (Sintering Temperature) (^oC)
Serial No.	Mode Symmetry	Bulk Empirical Calculation (cm^-1)	Bulk Experimental Data (cm^-1)	900 (cm^-1)		Frequency Shift (cm^-1)	1000 (cm^-1)	Frequency Shift (cm^-1)	1100 (cm^-1)	Frequency Shift (cm^-1)	1200 (cm^-1)		Frequency Shift (cm^-1)
1	A_Z	104	-	-	-		-	-	-	-	-	-
2	B_Z	113	-	112	-		112	-	112	-	-	-
3	B_Z	150	144	140	-4		143	-1	143	-1	140	-4
4	A_Z	166	169	165	-4		165	-4	168	-1	168	-1
5	A_Z	207	200	196	-4		196	-4	202	+2	199	-4
6	A_Z	317	317	-	-		317	0	320	+3	317	0
7	A_Z	348	344	342	-2		345	+1	345	+1	343	-1
8	B_Z	356	-	-	-		-	-	-	-	-	-
9	A_Z	414	416	413	-3		413	-3	413	-3	412	-4
10	A_Z	469	472	-	-		472	0	-	-	472	0
11	B_Z	474	-	-	-		-	-	475	+1	-	-
12	A_Z	601	629	611	-18		-	-	-	-	-	-
13	B_Z	624	-	-	-		627	-	627	-	622	-
14	A_Z	635	654	652	-2		649	-5	652	-2	655	+1
15	A_Z	732	767	754	-13		760	-7	763	-4	763	-4

Fig. 2. Survey spectra of Ga1.9Fe0.1O3 ceramics at various sintering temperature.

Fig. 3. Deconvoluted high-resolution XPS spectra of (a) Ga 2p, (b) Fe2p, and (c) O 1s.

Table 2 Comparison of B.E. of Ga 2p, O 1s and Fe 2p core level spectra of Ga1.9Fe0.1O3 ceramics prepared under various sintering temperatures.

Sintering Temperature (^oC)	Binding Energy (B.E.) (eV)
	Ga 2p_3/2 (Ga₂O₃)	O 1 s (Fe_xO_y, Ga₂O₃)		Fe 2p_3/2 (Fe_xO_y)
	Ga 2p_3/2 (Ga₂O₃)	Fe_xO_y	Ga₂O₃	FeO	Fe₂O₃
900	1117.34	530.21	530.87	-	710.94
1000	1117.35	530.25	530.83	-	711.10
1100	1117.35	530.29	530.87	708.71	711.06
1200	1117.37	530.25	530.86	708.76	711.00

Table 3 Comparison of FWHM of Ga 2p, O 1s and Fe 2p core level spectra of differently sintered samples.

Sintering Temperature (^oC)	FWHM
	Ga 2p_3/2 (Ga₂O₃)	O 1 s (Fe_xO_y, Ga₂O₃)		Fe 2p_3/2 (Fe_xO_y)
	Ga 2p_3/2 (Ga₂O₃)	Fe_xO_y	Ga₂O₃	FeO	Fe₂O₃
900	1.40	1.51	1.45	-	1.40
1000	1.40	1.49	1.47	-	1.43
1100	1.40	1.51	1.44	1.51	1.41
1200	1.40	1.50	1.48	1.50	1.42

Fig. 4. Frequency dependent room-temperature ac conductivity of Ga1.9Fe0.1O3 ceramics sintered at different conditions. Conductivity variation is not significant throughout the whole frequency range while increasing trend can be noticed at higher frequency level.

Fig. 5. log(σac-σdc) versus log ω2 plots for Ga1.9Fe0.1O3 ceramics. The initial linear plots are evident of small polaron hopping mechanism.

Fig. 6. Variation of ac electrical resistivity with temperature at different frequencies. The data shown are for Ga1.9Fe0.1O3 ceramics sintered at above mentioned temperatures. It can be seen that ac resistivity decreases continuously with increasing sintering temperature.

Fig. 7. Comparison of ac electrical resistivity of Ga1.9Fe0.1O3 ceramics at various frequency.

Fig. 8. Temperature dependent dc conductivity plot of Ga1.9Fe0.1O3 ceramics sintered at different conditions.

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Effect of sintering temperature on the chemical bonding, electronic structure and electrical transport properties of β-Ga_1.9Fe_0.1O₃ compounds

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