基于Weiss分子场理论对极性液体中静态介电常数随温度变化及其相应取向关联的研究

张丽丽; 黄心茹; 周恒为; 黄以能

doi:10.7498/aps.61.187701

摘要

迄今为止,并没有被普遍接受的液体静态介电常数的微观理论模型, 主要原因是对属于强关联系统的液体中分子之间的取向关联特征仍不十分清楚. 本文基于Weiss分子场理论(WMFT), 对水(water, H2O)、甲醇(methanol, CH4O)、乙醇(ethanol, C2H6O)和正丙醇(1-propanol, C3H8O)等4种极性液体中静态介电常数, 具体为Curie-Weiss常数、Curie温度和Weiss分子场因子随温度变化规律进行分析研究, 得出上述液体中: 1)铁电关联(ferroelectric correlation, FC)和反铁电关联(anti-ferroelectric correlation, AFC)共存, 且FC比AFC强得多, 以及随温度降低FC减弱和/或AFC增强; 2)结构均匀的WMFT不能定量描述上述液体中足够低的温度下反常大的静态介电常数. 可以想象FC和较弱AFC的共存必然导致极性液体中关联序的空间不均匀, 由此作者提出了空间不均匀关联序的粗粒近似的Weiss分子场理论, 并用此理论对上述液体中静态介电常数随温度快速变化的行为进行了解释. 上述结果对深入认知液体物理学, 包括玻璃化转变机制的探索, 无疑是有价值的.

关键词:

Abstract

There is no widely accepted microscopic theoretical model of the static dielectric constant of liquids so far. This is mainly because the orientational correlation between molecules in liquids, belonging to the strong correlation systems, is still not clear. In this paper, the variations of the static dielectric constants of 4 kinds of polar liquids, i.e., water, methanol, ethanol and 1-propanol, specifically the Curie-Weiss constant, Curie temperature and Weiss molecular field factor with temperature are studied according to the Weiss's molecular field theory (WMFT), and it is concluded that 1) ferroelectric correlations (FCs) and anti-ferroelectric correlations (AFCs) between molecules coexist in the liquids, and FC is stronger than AFC, as well as FC becomes weak and/or AFC stronger with temperature decreasing; 2) WMFT of homogeneous structure cannot quantitatively describe the abnormally large values of εs of the liquids at low enough T. It can be expected that the coexistence of FC and weak AFC must lead to the spatial distribution of the correlation orders, and consequently, we propose an WMFT of coarse grain approximation of the spatial distribution correlation orders, and use the WMFT to explain why the static dielectric constant varies rapidly with temperature. The above results can benefit the understanding of the liquid physics, including the glass transition mechanism.

Keywords:

作者及机构信息

1.
伊犁师范学院物理科学与技术学院, 新疆凝聚态相变与微结构实验室, 伊宁 835000;

2.
南京大学物理学院, 国家固体微结构实验室, 南京 210093;

3.
石河子大学物理系, 石河子 832003

基金项目: 国家自然科学基金(批准号: 10774064, 30860076);国家重点基础研究发展计划(批准号: 2012CB821503); 新疆自治区高技术发展项目(批准号: 200916126)和新疆自治区科技厅自然基金(批准号: 200821104, 200821184).

Authors and contacts

1.
Xinjiang Laboratory of Phase Transitions and Microstructures in Condensed Matters, College of Physical Science and Technology, Yili Normal University, Yining 835000, China;

2.
National Laboratory of Solid State Microstructures, School of Physics, Nanjing University, Nanjing 210093, China;

3.
Department of Physics, Shihezi University, Shihezi 832003, China

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 10774064, 30860076), the National Basic Research Program of China (Grant No. 2012CB821500), the Science and Technology Program of Xinjiang Uygur Autonomous Region, China (Grant No. 200916126), and the Natural Science Foundations of Xinjiang Uygur Autonomous Region, China (Grant Nos. 200821104, 200821184).

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[35]	Zhou H W, Zhang J L, Huang Y N, Ying X N, Zhang L, Wu W H, Shen Y F 2007 Acta Phys. Sin. 56 6547 (in Chinese) [周恒为, 张晋鲁, 黄以能, 应学农, 张亮, 吴文惠, 沈异凡 2007 物理学报 56 6547]
[36]	Wang Z Y, Yang Y S, Tong W H, Li H Q, Hu Z L 2007 Acta Phys. Sin. 56 1543 (in Chinese) [王珍玉, 杨院生, 童文辉, 李会强, 胡壮麒 2007 56 1543]
[37]	Yi X H, Liu R S, Tian Z A, Hou Z Y, Wang X, Zhou Q Y 2006 Acta Phys. Sin. 55 5386 (in Chinese) [易学华, 刘让苏, 田泽安, 侯兆阳, 王鑫, 周群益 2006 物理学报 55 5386]
[38]	Xia M X, Meng Q G, Zhang S G, Ma C L, Li J G 2006 Acta Phys. Sin. 55 6543 (in Chinese) [夏明许, 孟庆格, 张曙光, 马朝利, 李建国 2006 物理学报 55 6543]
[39]	Yu P, Bai H Y, Tang M B, Wang W L, Wang W H 2005 Acta Phys. Sin. 54 3284 (in Chinese) [余鹏, 白海洋, 汤美波, 王万录, 汪卫华 2005 物理学报 54 3284]
[40]	Hou Z Y, Liu R S, Li C S, Zhou Q Y, Zheng C X 2005 Acta Phys. Sin. 54 5723 (in Chinese) [侯兆阳, 刘让苏, 李琛珊, 周群益, 郑采星 2005 物理学报 54 5723]
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[47]	Oster G, Kirkwood J G 1943 J. Chem. Phys. 11 175
[48]	Dannhauser W, Cole R H 1955 J. Chem. Phys. 23 1762
[49]	Suresh S J, Naik V M 2000 J. Chem. Phys. 113 9727
[50]	Wohlfarth C 1991 Static Dielectric Constants of Pure Liquids and Binary Liquid Mixtures, (Vol. 6) (Berlin: Springer-Verlag)
[51]	Weber M J 2003 Handbook of Optical Materials (CRC Press, Lawrence Berkeley National Laboratory)
[52]	Cardarelli F 2005 Materials Handbook, (2nd Ed.) (Berlin: Springer-Verlag)
[53]	Zhang L L, Huang X R, Zhou H W, Huang Y N 2012 Acta Phys. Sin. 6 077701 (in Chinese) [张丽丽, 黄心茹, 周恒为, 黄以能 2012 物理学报 6 077701]
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[55]	Weiss P 1908 Physikalische Zeitschrift 9 358

施引文献

[1]	Donth E 2001 The Glass Transition (Berlin: Spring)
[2]	Yin Z W 2003 Dielectrics Physics (2nd Ed.) (Beijing: Scientific Publication)
[3]	Fröhlich H 1958 Theory of Dielectrics (2nd Ed.) (Oxford: Oxford University Press)
[4]	Böttcher C F J, Bordewijk P 1978 Theory of Electric Polarization (vol. II) (Amsterdam: Elsevier)
[5]	Anderson P W 1995 Science 267 1615
[6]	Liu Y H, Wang G, Wang R J, Zhao D Q, Pan M X, Wang W H 2007 Science 315 1385
[7]	Zhao Z F, Wen P, Sheck C H, Wang W H 2007 Phys. Rev. B 75 174201
[8]	Huang Y N, Wang C J, Riande E 2005 J. Chem. Phys. 122 144502
[9]	Wu W H, Zhang J L, Zhou H W, Huang Y N, Zhang L, Ying X N 2008 Appl. Phys. Lett. 92 011918
[10]	Zhang J L, Zhou H W, Wu W H, Huang Y N 2008 Appl. Phys. Lett. 92 131906
[11]	Huang Y N, Zhang J L, Ying X N 2006 Prog. Phys. 26 359 (in Chinese) [黄以能, 张晋鲁, 应学农 2006 物理学进展 26 359]
[12]	Huang Y N 2006 J. Yili Normal University 3 39 (in Chinese) [黄以能 2006 伊犁师范学院学报 3 39]
[13]	Zhang J L, Wang L N, Zhou H W, Zhang L L, Zhao X Y, Huang Y N 2010 Chin. Phys. B 19 056403
[14]	Zhang J L, Wang L N, Zhao X Y, Zhang L L, Zhou H W, Wei L, Huang Y N 2011 Chin. Phys. B 20 026401
[15]	Zhao X Y, Wang L N, Fan X H, Zhang L L, Wei L, Zhang J L, Huang Y N 2011 Acta Phys. Sin. 60 036403 (in Chinese) [赵兴宇, 王丽娜, 樊小辉, 张丽丽, 卫来, 张晋鲁, 黄以能 2011 物理学报 60 036403]
[16]	Zhang L L, Zhang J L, Jiang J G, Zhou H W, Huang Y N 2008 Acta Phys. Sin. 57 5817 (in Chinese) [张丽丽, 张晋鲁, 蒋建国, 周恒为, 黄以能 2008 物理学报 57 5817]
[17]	Jiang J G, Huang Y N 2009 Comp. Phys. Commun. 180 177
[18]	Jiang J G, Huang Y N, Wu J C 2009 J. Stat. Phys. 136 984
[19]	Guo X Z, Zhou H W, Zhang L L, Wu W H, Zhang J L, Huang Y N 2010 Acta Phys. Sin. 59 417 (in Chinese) [郭秀珍, 周恒为, 张丽丽, 吴文慧, 张晋鲁, 黄以能 2010 物理学报 59 417]
[20]	Chen Z H, Liu L J, Zhang B, Xi Y, Wang Q, Zu F Q 2004 Acta Phys. Sin. 53 3839 (in Chinese) [陈志浩, 刘兰俊, 张博, 席赟, 王强, 祖方遒 2004 物理学报 53 3839]
[21]	Dong Z G, Shen M R, Xu R, Gan Z Q, Ge S B 2002 Acta Phys. Sin. 51 2896 (in Chinese) [董正高, 沈明荣, 徐闰, 甘肇强, 葛水兵 2002 物理学报 51 2896]
[22]	Shao S F, Zheng P, Zhang J L, Niu X K, Wang C L, Zhong W L 2006 Acta Phys. Sin. 55 6661 (in Chinese) [邵守福, 郑鹏, 张家良, 钮效鹍, 王春雷, 钟维烈 2006 物理学报 55 6661]
[23]	Liu P, He Y, Li J, Zhu G Q, Bian X B 2007 Acta Phys. Sin. 56 5489 (in Chinese) [刘鹏, 贺颖, 李俊, 朱刚强, 边小兵 2007 物理学报 56 5489]
[24]	Zhao M L, Zhong W L, Wang C L, Wang J F, Zhang P L 2002 Acta Phys. Sin. 51 1856 (in Chinese) [赵明磊, 钟维烈, 王春雷, 王矜奉, 张沛霖 2002 物理学报 51 1856]
[25]	Li S T, Cheng P F, Zhao L, Li J Y 2009 Acta Phys. Sin. 58 523 (in Chinese) [李盛涛, 成鹏飞, 赵雷, 李建英 2009 物理学报 58 523]
[26]	Zhao S C, Li G R, Zhang L N, Wang T B, Ding A L 2006 Acta Phys. Sin. 55 3711 (in Chinese) [赵苏串, 李国荣, 张丽娜, 王天宝, 丁爱丽 2006 物理学报 55 3711]
[27]	Jiang X P, Fang J W, Zeng H R, Pan X M, Chen D R, Yin Q R 2000 Acta Phys. Sin. 49 802 (in Chinese) [江向平, 方健文, 曾华荣, 潘晓明, 陈大任, 殷庆瑞 2000 物理学报 49 802]
[28]	Zhao M L, Wang C L, Zhong W L, Zhang P L, Wang J F 2002 Acta Phys. Sin. 51 420 (in Chinese) [赵明磊, 王春雷, 钟维烈, 张沛霖, 王矜奉 2002 物理学报 51 420]
[29]	Zhao M L, Yi X J, Wang C L, Wang J F, Zhang J L 2006 Chin. Phys. 15 1611
[30]	Wen C 1995 Chin. Phys. 4 54
[31]	Zhao H P, Liu Z Y, Liu Y Y 2001 Chin. Phys. 10 35
[32]	Wang X J, Gong Z Q, Qian Y F, Zhu J, Chen X B 2007 Chin. Phys. 16 2131
[33]	Wang Q, Qiang J B, Wang Y M, Xia J H, Lin Z, Zhang X F, Dong C 2006 Acta Phys. Sin. 55 378 (in Chinese) [王清, 羌建兵, 王英敏, 夏俊海, 林哲, 张新房, 董闯 2006 物理学报 55 378]
[34]	Zhang H T, Liu R S, Hou Z Y, Zhang A L, Chen X Y, Du S H 2006 Acta Phys. Sin. 55 2409 (in Chinese) [张海涛, 刘让苏, 侯兆阳, 张爱龙, 陈晓莹, 杜生海 2006 物理学报 55 2409]
[35]	Zhou H W, Zhang J L, Huang Y N, Ying X N, Zhang L, Wu W H, Shen Y F 2007 Acta Phys. Sin. 56 6547 (in Chinese) [周恒为, 张晋鲁, 黄以能, 应学农, 张亮, 吴文惠, 沈异凡 2007 物理学报 56 6547]
[36]	Wang Z Y, Yang Y S, Tong W H, Li H Q, Hu Z L 2007 Acta Phys. Sin. 56 1543 (in Chinese) [王珍玉, 杨院生, 童文辉, 李会强, 胡壮麒 2007 56 1543]
[37]	Yi X H, Liu R S, Tian Z A, Hou Z Y, Wang X, Zhou Q Y 2006 Acta Phys. Sin. 55 5386 (in Chinese) [易学华, 刘让苏, 田泽安, 侯兆阳, 王鑫, 周群益 2006 物理学报 55 5386]
[38]	Xia M X, Meng Q G, Zhang S G, Ma C L, Li J G 2006 Acta Phys. Sin. 55 6543 (in Chinese) [夏明许, 孟庆格, 张曙光, 马朝利, 李建国 2006 物理学报 55 6543]
[39]	Yu P, Bai H Y, Tang M B, Wang W L, Wang W H 2005 Acta Phys. Sin. 54 3284 (in Chinese) [余鹏, 白海洋, 汤美波, 王万录, 汪卫华 2005 物理学报 54 3284]
[40]	Hou Z Y, Liu R S, Li C S, Zhou Q Y, Zheng C X 2005 Acta Phys. Sin. 54 5723 (in Chinese) [侯兆阳, 刘让苏, 李琛珊, 周群益, 郑采星 2005 物理学报 54 5723]
[41]	Wei H Q, Long Z L, Zhang Z C, Li X A, Peng J, Zhang P 2009 Acta Phys. Sin. 58 2556 (in Chinese) [危洪清, 龙志林, 张志纯, 李乡安, 彭建, 张平 2009 物理学报 58 2556]
[42]	Hou Z Y, Liu R S, Wang X, Tian Z A, Zhou Q Y, Chen Z H 2007 Acta Phys. Sin. 56 376 (in Chinese) [侯兆阳, 刘让苏, 王鑫, 田泽安, 周群益, 陈振华 2007 物理学报 56 376]
[43]	Li J, Zhang Y, Zhang S C 1996 Acta Phys. Sin. 45 1359 (in Chinese) [李健, 张烨, 张声春 1996 物理学报 45 1359]
[44]	Zhao J Z, Liu J, Zhao Y, Hu Z Q 2007 Acta Phys. Sin. 56 443 (in Chinese) [赵九洲, 刘俊, 赵毅, 胡壮麒 2007 物理学报 56 443]
[45]	Zhao Z F, Zhang Z, Li Z, Wei P, Zhao D Q, Pan M X, Wang W L, Wang W H 2004 Acta Phys. Sin. 53 850 (in Chinese) [赵作峰, 张志, 李正, 闻平, 赵德乾, 潘明详, 王万录, 汪卫华 2004 物理学报 53 850]
[46]	Kirkwood J G 1939 J. Chem. Phys. 7 911
[47]	Oster G, Kirkwood J G 1943 J. Chem. Phys. 11 175
[48]	Dannhauser W, Cole R H 1955 J. Chem. Phys. 23 1762
[49]	Suresh S J, Naik V M 2000 J. Chem. Phys. 113 9727
[50]	Wohlfarth C 1991 Static Dielectric Constants of Pure Liquids and Binary Liquid Mixtures, (Vol. 6) (Berlin: Springer-Verlag)
[51]	Weber M J 2003 Handbook of Optical Materials (CRC Press, Lawrence Berkeley National Laboratory)
[52]	Cardarelli F 2005 Materials Handbook, (2nd Ed.) (Berlin: Springer-Verlag)
[53]	Zhang L L, Huang X R, Zhou H W, Huang Y N 2012 Acta Phys. Sin. 6 077701 (in Chinese) [张丽丽, 黄心茹, 周恒为, 黄以能 2012 物理学报 6 077701]
[54]	Weiss P 1907 J. de Phys. 6 661
[55]	Weiss P 1908 Physikalische Zeitschrift 9 358

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