高压下纳米晶ZnS晶粒和晶界性质及相变机理

王春杰; 王月; 高春晓

doi:10.7498/aps.69.20200240

摘要

采用高压在位交流阻抗谱技术, 研究了ZnS纳米晶在0—29.8 GPa压力范围内的晶粒和晶界性质变化及相关相变机理. 从晶粒和晶界的模谱图像中观察到, 随着压力的增加, 象征晶界影响的圆弧逐渐增加, 而代表晶粒作用的圆弧逐渐减弱. 此外, 晶粒电阻和晶界电阻随压力的升高呈现不同的变化速率, 并在11和15 GPa处出现了不连续变化点, 分别对应着由纤锌矿到闪锌矿到岩盐相结构转变的压力点. 进一步通过分析相变过程中晶界弛豫频率随压力的线性变化关系, 研究了ZnS由纤锌矿到闪锌矿到岩盐相的相变机理.

关键词:

高压 /
ZnS /
阻抗谱 /
相变

Abstract

In this paper, the grain and grain boundary characteristics and mechanisms of phase transition (from wurtzite to zinc-blende to rock-salt phase structure) of ZnS nanocrystallines are investigated via in situ impedance measurement under pressure up to 29.8 GPa. It should be noted that there are two semiarcs can be found from the modulus plots of ZnS under different pressures. The semiarc in high frequency region represents the grain characteristic, and another one in low frequency region refers to the grain boundary characteristic. The former decreases gradually with pressure increasing and the latter shows an opposite trend. This fact indicates that the effect of grain characteristic becomes weaker and weaker, and the role of grain boundary characteristic is just on the contrary. The grain resistance and grain boundary resistance of ZnS nanocrystalline are also studied. In the low pressure region, both resistances increase with different increment rate with pressure increasing, which can be attributed to the enhanced ability of trap charge carriers due to the small size effect of nanoparticles. In addition, two discontinuous points (about 11 and 15 GPa) can be observed in both resistance curves, corresponding to the points of phase transition from wurtzite to zinc-blende to rock-salt phase structure. With pressure increasing, both resistances decrease gradually until 21 GPa, and this point corresponds to the end of transition from zinc-blende to rock-salt phase structure. Their consequent variations are different, grain boundary resistance gradually decreases with the pressure increasing, while the grain resistance is almost a constant. Additionally, the relaxation frequency, as an intrinsic characteristic, is not affected by the geometrical parameters. According to the linear relation between the grain boundary relaxation frequency and pressure in the pressure range of phase transformation, the mechanism of structure transition from wurtzite to zinc-blende to rock-salt phase structure is also discussed in detail. Based on the investigations, the in situ impedance spectroscopy can not only be used to accurately measure the grain and grain boundary characteristics, but also provide information for studying the phase transformation under pressure.

Keywords:

作者及机构信息

1.
渤海大学工学院, 锦州　121013

2.
渤海大学新能源学院, 锦州　121013

3.
吉林大学, 超硬材料国家重点实验室, 长春　130012

通信作者: 王月, wangsuiyue@foxmail.com

基金项目: 国家级-国家自然科学基金(11404032)

Authors and contacts

1.
College of Engineering, Bohai University, Jinzhou 121013, China

2.
College of New Energy, Bohai University, Jinzhou 121013, China

3.
State Key Laboratory of Superhard Materials, Jilin University, Changchun 130012, China

Corresponding author: Wang Yue, wangsuiyue@foxmail.com

文章全文 : translate this paragraph

参考文献

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[22]	Zhang H Z, Huang F, Gilbert B, Banfield J F 2003 J. Phys. Chem. B 107 13051 Google Scholar
[23]	Zhao M, Zheng W T, Li J C, Wen Z, Gu M X, Sun C Q 2007 Phys. Rev. B 75 085427 Google Scholar
[24]	Kodiyalam S, Rajiv K K, Hideaki K, Aiichiro N, Fuyuki S, Vashishta P 2001 Phys. Rev. Lett. 86 55 Google Scholar
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施引文献

图 1 纤锌矿ZnS纳米晶XRD谱图

Fig. 1. XRD pattern of wurtzite ZnS nanocrystals.

下载: 全尺寸图片幻灯片

图 2 (a) 金刚石对顶砧薄膜电极示意图: 1, Mo电极; 2, 裸露的金刚石砧面; 3, 沉积在金刚石砧面的Al₂O₃薄膜; 4, 沉积在Mo薄膜上的Al₂O₃薄膜; (b)金刚石对顶砧剖面示意图

Fig. 2. (a) The configuration of a complete microcircuit on a diamond anvil: 1, the Mo electrodes; 2, the exposed diamond anvil; 3, the Al₂O₃ layer deposited on the diamond anvil; 4, the Al₂O₃ layer deposited on the Mo film; (b) the cross section of the designed diamond-anvil-cell.

下载: 全尺寸图片幻灯片

图 3 不同压力下ZnS纳米晶的模谱图　(a) 8.4 GPa; (b) 12.6 GPa; (c) 18.3 GPa; (d) 29.8 GPa

Fig. 3. The modulus plots of ZnS nanocrystallines under different pressures: (a) 8.4 GPa; (b) 12.6 GPa; (c) 18.3 GPa; (d) 29.8 GPa.

下载: 全尺寸图片幻灯片

图 4 晶粒电阻(R_g)和晶界电阻(R_gb)随压力的变化关系

Fig. 4. Pressure dependence of grain resistance (R_g) and grain boundary resistance (R_gb) under high pressure.

下载: 全尺寸图片幻灯片

图 5 晶界弛豫频率随压力的变化

Fig. 5. The change of grain boundary relaxation frequency of ZnS nanocrystalline as a function of pressure.

下载: 全尺寸图片幻灯片

map

[1]	Ding Z, Quinn B M, Haram S K, Pell L E, Korgel B A, Bard A J 2002 Science 296 1293 Google Scholar
[2]	Stoica T, Sutter E, Meijers R J, Debnath R K, Calarco R, Luth H, Grutzmacher D 2008 Small 4 751 Google Scholar
[3]	Bai F, Bian K, Huang X 2019 Chem. Rev. 119 7673 Google Scholar
[4]	Haase M, Alivisatos A P 1992 J. Phys. Chem. 96 6756 Google Scholar
[5]	Cui X Y, Hu T J, Wang J S, Zhang J K, Zhao R, Li F F 2017 RSC Adv. 7 12098 Google Scholar
[6]	Ono S, Kikegawa T 2018 Phase Transitions 91 9 Google Scholar
[7]	Biering S, Schwerdtfeger P 2012 J. Chem. Phys. 137 034705 Google Scholar
[8]	Bilge M, Özdemir S, Kart H H 2008 Mater. Chem. Phys. 111 559 Google Scholar
[9]	Wang Z, Guo Q 2009 J. Phys. Chem.C 113 4286 Google Scholar
[10]	Pan Y W, Qu S, Dong S, Cui Q L, Gao C X, Zou G T 2002 J. Phys. Condens. Mater. 14 10487 Google Scholar
[11]	Bi C, Pan L Q, Guo Z G, Zhao Y L, Huang M F, Xin J 2010 Mater. Lett. 64 1681 Google Scholar
[12]	Wang Y, Han Y H, Gao C X, Ma Y Z, Liu C L, Peng G, Wu B J, Liu B, Hu T J, Cui X Y, Ren W B, Li Y, Su N N, Liu H W, Zou G T 2010 Rev. Sci. Instrum 81 013904 Google Scholar
[13]	王月, 张凤霞, 王春杰, 高春晓 2014 63 216401 Google Scholar Wang Y, Zhang F X, Wang C J, Gao C X 2014 Acta Phys. Sin. 63 216401 Google Scholar
[14]	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)
[15]	Li J, Wang W 2005 Phys. Rev. B 72 125325 Google Scholar
[16]	Maier J 1987 Solid State Ionics 23 59 Google Scholar
[17]	Fleig J, Maier J 1998 J. Electrochem. Soc. 145 2081 Google Scholar
[18]	Fleig, J 2002 Solid State Ionics 150 181 Google Scholar
[19]	Tolbert S H, Alivisatos A P 1994 Science 265 373 Google Scholar
[20]	Tolbert S H, Alivisatos A P 1995 J. Chem. Phys. 102 4642 Google Scholar
[21]	Tolbert S H, Herhold A B, Brus L E, Alivisatos A P 1996 Phys. Rev. Lett. 76 4384 Google Scholar
[22]	Zhang H Z, Huang F, Gilbert B, Banfield J F 2003 J. Phys. Chem. B 107 13051 Google Scholar
[23]	Zhao M, Zheng W T, Li J C, Wen Z, Gu M X, Sun C Q 2007 Phys. Rev. B 75 085427 Google Scholar
[24]	Kodiyalam S, Rajiv K K, Hideaki K, Aiichiro N, Fuyuki S, Vashishta P 2001 Phys. Rev. Lett. 86 55 Google Scholar
[25]	Ye X, Sun D Y, Gong X G 2008 Phys. Rev. B 77 094108 Google Scholar
[26]	Wickham J N, Herhold A B, Alivisators A P 2000 Phys. Rev. Lett. 84 923 Google Scholar
[27]	Goldstein A N, Echer C M, Alivisatos A P 1992 Science 256 1425 Google Scholar
[28]	Brus L E, Harkless J A W, Stillinger F H 1996 J. Am. Chem. Soc. 118 4834 Google Scholar
[29]	Macdonald J R 1987 Impedance Spectrum (New York: Wiley) pp13–14, 205
[30]	Chen C C, Herhold A B, Johnson C S, Alivisatos A P 1997 Science 276 398 Google Scholar
[31]	Wang Z W, Daemen L L, Zhao Y S, Zha C S, Downs R T, Wang X, Wang Z L 2005 Nat. Mater. 4 922 Google Scholar
[32]	Gilbert B, Frazer B H, Zhang H, Huang F, Banfield J F, Haskel D, Lang J C, Srajer G, de Stasio G 2002 Phys. Rev. B 66 245205 Google Scholar

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高压下纳米晶ZnS晶粒和晶界性质及相变机理