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The electrical transport properties of anatase TiO2 polycrystalline have been systematically investigated by using high pressure in-situ impedance spectroscopy measurements. The anomalous behaviors of resistance, parameter factor and relaxation frequency of grain and grain boundary can be found at 6.4, 11.5 and 24.6 GPa. The results indicate that the first two discontinuous points (6.4 and 11.5 GPa) correspond to the phase transitions of TiO2 from anatase to α-PbO2 and then to baddeleyite, respectively. Above 24.6 GPa, TiO2 completely transforms into the baddeleyite phase. Based on the change of grain resistance and grain boundary resistance under pressure, intrinsic defects play a crucial effect in the electrical transport properties of TiO2 at high pressures. At 6.4 GPa, the occurrence of phase transition gives rise to the variation of defects’ role, from a deep energy level defect (as a recombination centre) changes into a shallow energy level defect (providing carriers for the conduction and valence bands). In addition, the position of defect in energy band changes with pressure increasing. The phase transition of TiO2 at 6.4 GPa is the rearrangement of TiO6 octahedron, while the other one at 11.5 GPa can be attributed to the migration of oxygen Schottky defects from inner to surface. Combining the packing factor and relaxation frequency, the electrical transport properties of TiO2 under pressure are revealed, the packing factor and the relaxation frequency are closely related to the mobility and the carrier concentration, respectively. The activation energy of grain and grain boundary decrease with the pressure elevating, indicating that the transport of carriers in grain and grain boundary become easier under pressure, and the former is smoother than the latter owing to the activation energy of grain being smaller than that of grain boundary in the same pressure range. Moreover, the relaxation frequency ratio of TiO2 grain and TiO2 grain boundary decreases with pressure increasing, and the grain boundary effect under high pressure is not obvious.
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Keywords:
- high pressure /
- TiO2 /
- defects /
- grain boundary
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Liu E K, Zhu B S, Luo J S 2012 The Physics of Semiconductors (Vol. 7) (Beijing: Electronic Industry Press) p109 (in Chinese)
[52] Ohta S, Sekiya T, Kurita S 2001 Phys. Status. Solidi. (b) 223 265
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图 1 TiO2在不同压力下的Nyquist谱图 (a) 4.9—7.6 GPa; (b) 7.6—13.0 GPa; (c) 13.0—20.3 GPa; (d) 20.3—24.6 GPa; (e) 24.6—30.1 GPa; (f) 30.1—38.9 GPa
Figure 1. Nyquist impedance spectra of TiO2 at different pressures: (a) 4.9–7.6 GPa; (b) 7.6–13.0 GPa; (c) 13.0–20.3 GPa; (d) 20.3–24.6 GPa; (e) 24.6–30.1 GPa; (f) 30.1–38.9 GPa.
图 2 不同压力下TiO2阻抗谱实验和拟合数据对比 (a) 5.4 GPa; (b) 20.3 GPa
Figure 2. Experimental and fitting data for TiO2 impedance spectra at different pressures: (a) 5.4 GPa; (b) 20.3 GPa.
图 3 TiO2参数因子随压力的变化关系
Figure 3. Pressure dependence of parameter factor for TiO2.
图 4 TiO2电阻随压力的变化关系
Figure 4. Pressure dependence of resistance for TiO2.
图 5 TiO2弛豫频率随压力的变化关系
Figure 5. Pressure dependence of the relaxation frequency for TiO2.
图 6 不同压力区间TiO2缺陷能级分布
Figure 6. Distribution of TiO2 defect energy levels in different pressure intervals.
表 1 激活能随压力的变化关系
Table 1. Pressure dependence of activation energy.
Pressure region/GPa dE/dP/(meV·GPa–1) Grain Grain boundary 0—6.4 –11.51 –22.79 6.4—11.5 –7.59 –9.33 11.5—24.6 –6.16 –6.82 24.6—38.9 –3.54 –4.91 
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[1] Augustynski J 1993 Electrochim. Acta. 38 43
Google Scholar
[2] Pezhooli N, Rahimi J, Hasti F, Maleki A 2022 Sci. Rep. 12 9885
Google Scholar
[3] Crossland E J W, Noel N, Sivaram V, Leijtens T, Alexander-Webber J A, Snaith H J 2013 Nature 495 215
Google Scholar
[4] Reza K M, Kurny A, Gulshan F 2017 Appl. Water. Sci. 7 1569
Google Scholar
[5] 韩迪仪, 顾阳, 胡涛政, 董雯, 倪亚贤 2021 70 038103
Google Scholar
Han D Y, Gu Y, Hu T Z, Dong W, Ni Y X 2021 Acta Phys. Sin. 70 038103
Google Scholar
[6] Liu L, Chan J, Sham T K 2010 J. Phys. Chem. C 114 21353
Google Scholar
[7] San-Miguel A 2006 Chem. Soc. Rev. 35 876
Google Scholar
[8] Lu X, Yang W, Quan Z, Lin T, Bai L, Wang L, Huang F, Zhao Y 2014 J. Am. Chem. Soc. 136 419
Google Scholar
[9] Dong Z, Xiao F, Zhao A, Liu L, Sham T K, Song Y 2016 RSC Adv. 6 76142
Google Scholar
[10] Liu F, Dong Z H, Liu L L 2019 J. Phys.: Condens. Matter 31 395403
Google Scholar
[11] Huang Y, Chen F, Li X, Yuan Y, Dong H, Samanta S, Zhang J, Yang K 2016 J. Appl. Phys. 119 184
Google Scholar
[12] Dong Z H, Song Y 2015 Can. J. Chem. 93 165
Google Scholar
[13] Ji T, Gao Y, Qin T, Yue D, Gao C 2021 J. Phys. Chem. C 125 3364
Google Scholar
[14] Li Q J, Liu B B 2016 Chin. Phys. B 25 076107
Google Scholar
[15] Hearne G R, Zhao J, Dawe A M, Pischedda V, Maaza M, Nieuwoudt M K, Kibasomba P, Nemraoui O, Comins J D, Witcomb M J 2004 Phys. Rev. B 70 134102
Google Scholar
[16] Haines J, Leger J M 1993 Physica B 192 233
Google Scholar
[17] Kurita S, Ohta S, Sekiya T 2002 High Pressure Res. 22 319
Google Scholar
[18] Ohsaka T, Yamaoka S, Shimomura O 1979 Solid State Commun. 30 34
Google Scholar
[19] Liu L G, Mernagh T P 1992 Eur. J. Mineral. 4 45
Google Scholar
[20] Lagarec K, Desgreniers S 1995 Solid State Commun. 94 519
Google Scholar
[21] Sekiya T, Ohta S, Kamei S, Hanakawa M, KuritaS 2001 J. Phys. Chem. Solids 62 717
Google Scholar
[22] Arlt T, Bermejo M, Blanco M A, Gerward L, Jiang J Z, Olsen J S, Recio J M 2000 Phys. Rev. B 61 14414
Google Scholar
[23] Swamy V, Dubrovinsky L S, Dubrovinskaia N A, Langenhorst F, Simionovici A S, Drakopoulos M, Dmitriev V, Weber H P 2005 Solid State Commun. 134 541
Google Scholar
[24] Swamy V, Dubrovinsky L S, Dubrovinskaia N A, Simionovici A S, Drakopoulos M, Dmitriev V, Weber H P 2003 Solid State Commun. 125 111
Google Scholar
[25] Swamy V, Kuznetsov A, Dubrovinsky L S, McMillan P F, Prakapenka V B, Shen G, Muddle B C 2006 Phys. Rev. Lett. 96 135702
Google Scholar
[26] Li Q, Cheng B, Yang X, Liu R, Zou B 2013 J. Phys. Chem. C 117 8516
Google Scholar
[27] Li Q, Cheng B, Tian B, Liu R, Liu B, Wang F, Chen Z, Zou B, Cui T, Liu B 2014 RSC Adv. 4 12873
Google Scholar
[28] Wang Q, Wang X, Li J, Qin T, Sang D, Liu J, Ke F, Wang X, Li Y, Liu C 2021 J. Mater. Chem. C 9 4764
Google Scholar
[29] Zhang H, Zhang G, Wang J, Wang Q, Liu C 2021 J. Alloys Compd. 857 157482
Google Scholar
[30] Su N, Sun M, Wang Q, Jin J, Sui J, Liu C, Gao C 2021 J. Phys. Chem. C 125 2713
Google Scholar
[31] 王春杰, 王月, 高春晓 2020 69 147202
Google Scholar
Wang C J, Wang Y, Gao C X 2020 Acta Phys. Sin. 69 147202
Google Scholar
[32] Wang J, Zhang G, Liu H, Wang Q, Shen W, Yan Y, Liu C, Han Y, Gao C 2017 Appl. Phys. Lett. 111 031907
Google Scholar
[33] Duan S, Wang Q, Zou B, Jiang J, Liu K, Zhang G, Zhang, Sang D, Xu Z, Geng Y, Li J, Wang X, Li Y, Liu C 2022 Appl. Phys. Lett. 121 263904
Google Scholar
[34] Piermarini G J, Block S, Barnett J D, Forman R A, 1975 J. Appl. Phys. 46 2774
Google Scholar
[35] 曹楚南, 张鉴清 2002 电化学阻抗谱导论 (典藏版 1) (北京: 科学出版社) 第21页
Cao C N, Zhang J Q 2002 Introduction to Electrochemical Impedance Spectroscopy (Vol. 1) (Beijing: Science Press) p21 (in Chinese)
[36] Guo X, Yoshino T 2013 Earth Planet. Sci. Lett. 369–370 239
[37] Guo X, Yoshino T, Katayama I 2011 Phys. Earth Planet. Inter. 188 69
Google Scholar
[38] Rahman A U, Rafiq M A, Maaz K, Karim S, Cho S O, Hasan M M 2012 J. Appl. Phys. 112 063718
Google Scholar
[39] Ali H, Karim S, Rafiq M A, Maaz K, Ahmad M 2014 J. Alloys Compd. 612 64
Google Scholar
[40] Rahman A U, Rafifiq M A, Hasan M M, Maaz K, Karim S, Cho S O 2013 J. Nanopart Res. 15 1703
Google Scholar
[41] Liu J, Yan J, Shi Q, Dong H, Zhang J, Wang Z, Huang W, Chen B, Zhang H 2019 J. Phys. Chem. C 123 4094
Google Scholar
[42] Ma X G, Liang P, Miao L, Bie S W, Zhang C K, Xu L, Jiang J J 2009 Phys. Status. Solidi. (b) 246 2132
Google Scholar
[43] Sekiya T, Ohta S, Kurita S 2008 Int. J. Mod. Phys. B 15 3952
[44] Zhu T, Gao S P 2014 J. Phys. Chem. C 118 11385
Google Scholar
[45] Liu Q J, Zhang N C, Liu F S, Liu Z T 2014 Phys. Scr. 89 075703
Google Scholar
[46] Lin X, Wu J, Lu X, Shan Z, Wang W, Huang F 2009 Phys. Chem. Chem. Phys. 11 10047
Google Scholar
[47] Wu J, Huang F, Shan Z, Wang Y 2011 Dalton Trans. 40 6906
Google Scholar
[48] Keyan H U, Zian X U, Liu Y, Huang F 2020 Chem. Res. Chin. Univ. 36 1102
Google Scholar
[49] Plata J J, Márquez A M, Sanz J F 2013 J. Phys. Chem. C 117 14502
Google Scholar
[50] Park N G, van de Lagemaa J, Frank A J 2000 J. Phys. Chem. B 104 8989
Google Scholar
[51] 刘恩科, 朱秉升, 罗晋生 2012 半导体物理学 (第7版) (北京: 电子工业出版社) 第109页
Liu E K, Zhu B S, Luo J S 2012 The Physics of Semiconductors (Vol. 7) (Beijing: Electronic Industry Press) p109 (in Chinese)
[52] Ohta S, Sekiya T, Kurita S 2001 Phys. Status. Solidi. (b) 223 265
Google Scholar
[53] Muscat J, Swamy V, Harrison N M 2002 Phys. Rev. B 65 224112
Google Scholar
[54] Wang Q, Lian G, Dickey E C 2004 Acta Mater. 52 809
Google Scholar
[55] Bharathi K K, Markandeyulu G, Ramana C V 2011 J. Electrochem. Soc. 158 G71
Google Scholar
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