高压下缺陷对锐钛矿相TiO<sub>2</sub>多晶电输运性能的影响: 交流阻抗测量

王月; 邵渤淮; 陈双龙; 王春杰; 高春晓

doi:10.7498/aps.72.20230020

摘要

采用高压原位阻抗谱测量技术对锐钛矿TiO₂多晶的电输运性质进行了系统研究. 在6.4, 11.5和24.6 GPa压力处发现了晶粒和晶界的电阻、参数因子和弛豫频率的反常变化行为. 研究分析表明: 6.4和11.5 GPa压力点分别对应着TiO₂由锐钛矿转变为α-PbO₂, 再转变为斜锆石的结构相变, 当压力高于24.6 GPa时, TiO₂完全转变为斜锆石相. 通过分析晶粒和晶界电阻在压力作用下的变化行为可知, 本征缺陷的存在对TiO₂高压下电输运性质的变化起着关键的作用. 在6.4 GPa压力处, 相变的发生导致缺陷的作用发生了变化, 由作为复合中心的深能级缺陷转变为向导带和价带提供载流子的浅能级缺陷, 并且作为浅能级缺陷存在至实验最高压力点38.9 GPa, 浅能级缺陷在能带中的位置也随着相变发生而改变. 晶粒和晶界的激活能随着压力升高而降低, 表明高压下载流子在晶粒和晶界的输运变得更加容易. 此外, TiO₂晶粒和晶界的弛豫频率比值随压力的升高而不断减小, 高压下的晶界效应不明显.

关键词:

高压 /
TiO₂ /
缺陷 /
晶界

Abstract

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.

Keywords:

作者及机构信息

1.
渤海大学物理科学与技术学院, 锦州　121013

2.
吉林大学, 超硬材料国家重点实验室, 长春　130012

通信作者: 王春杰, cjwang@foxmail.com

基金项目: 国家自然科学基金(批准号: 12004050)和辽宁省教育厅项目(批准号: LJKMZ20221493)资助的课题.

Authors and contacts

1.
College of Physical Science and Technology, Bohai University, Jinzhou 121013, China

2.
State Key Laboratory of Superhard Materials, Jilin University, Changchun 130012, China

Corresponding author: Wang Chun-Jie, cjwang@foxmail.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 12004050) and the Research Foundation of the Education Department of Liaoning Province, China (Grant No. LJKMZ20221493).

文章全文 : translate this paragraph

参考文献

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施引文献

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

Fig. 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.

下载: 全尺寸图片幻灯片

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

Fig. 2. Experimental and fitting data for TiO₂ impedance spectra at different pressures: (a) 5.4 GPa; (b) 20.3 GPa.

下载: 全尺寸图片幻灯片

图 3 TiO₂参数因子随压力的变化关系

Fig. 3. Pressure dependence of parameter factor for TiO₂.

下载: 全尺寸图片幻灯片

图 4 TiO₂电阻随压力的变化关系

Fig. 4. Pressure dependence of resistance for TiO₂.

下载: 全尺寸图片幻灯片

图 5 TiO₂弛豫频率随压力的变化关系

Fig. 5. Pressure dependence of the relaxation frequency for TiO₂.

下载: 全尺寸图片幻灯片

图 6 不同压力区间TiO₂缺陷能级分布

Fig. 6. Distribution of TiO₂ defect energy levels in different pressure intervals.

下载: 全尺寸图片幻灯片

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

下载: 导出CSV

[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 物理学报 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 物理学报 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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高压下缺陷对锐钛矿相TiO₂多晶电输运性能的影响: 交流阻抗测量