Comparative investigations on α relaxation and conductivity of probe ions in a series of small molecular liquids

Zhao Xing-Yu; Wang Li-Na; Han Hong-Bo; Shang Jie-Ying

doi:10.7498/aps.73.20240478

Abstract

The coupling between translational motion and rotational motion in liquids is one of the long-standing concerns in condensed matter physics. The relaxation times of α relaxation and probe ion conductivities in a series of small molecular liquids, 15 types of single and binary small molecular liquids with different molecular shapes and functional groups when the number of carbon atoms is in a range from 3 to 14, are simultaneously obtained by dielectric spectroscopy method in this work. The results indicate that the coupling between translation and rotation is not directly related to the functional group of liquid molecules, nor very sensitive to the shape nor the size of molecules or ion size. However, the microstructure of liquid is a key factor affecting the coupling between translation and rotation. In other words, when the microstructure of the liquid is unchanged, the dependence of relaxation time on temperature is consistent with the dependence of conductivity reciprocal on temperature, whether in single small molecular liquids or in binary small molecular liquids, which provides a method for measuring relaxation time. The research results also show that the temperature dependence of the conductivity of the impurity ions carried by the liquid itself is consistent with the one of quantitatively doped ions, providing the ideas for investigating the ion conductivity behavior in organic small molecular liquids with low electrolyte solubilities. The experimental results of monohydroxy alcohol are consistent with the viewpoint that α relaxation rather than Debye relaxation corresponds to the system structure relaxation.

Keywords:

coupling between translation and rotation /
relaxation time /
probe ion conductivity /
small molecular liquid

Authors and contacts

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

Corresponding author: Wang Li-Na, wln_shuijin@163.com

Funds: Project supported by the Natural Science Foundation of Xinjiang Uygur Autonomous Region, China (Grant Nos. 2021D01C464, 2021D01C465) and the Special Project for Enhancing the Comprehensive Strength of Disciplines of Yili Normal University, China (Grant No. 22XKZY27).

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References

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[35]	Jakobsen B, Maggi C, Christensen T, Dyre J C 2008 J. Chem. Phys. 129 184502 Google Scholar
[36]	Gainaru C, Meier R, Schildmann S, Lederle C, Hiller W, Rössler E A, Böhmer R 2010 Phys. Rev. Lett. 105 258303 Google Scholar
[37]	Gainaru C, Kastner S, Mayr F, Lunkenheimer P, Schildmann S, Weber H J, Hiller W, Loidl A, Böhmer R 2011 Phys. Rev. Lett. 107 118304 Google Scholar
[38]	Bauer S, Burlafinger K, Gainaru C, Lunkenheimer P, Hiller W, Loidl A, Böhmer R 2013 J. Chem. Phys. 138 94505 Google Scholar
[39]	Lu G, Wang L N, Zhao X Y, He Y, Huang Y N 2021 Int. J. Mod. Phys. B 35 2150014 Google Scholar
[40]	Wang L N, Zhao X Y, Huang Y N 2019 Chin. Phys. Lett. 36 97701 Google Scholar
[41]	Ediger M D, Angell C A, Nagel S R 1996 J. Phys. Chem. 100 13200 Google Scholar
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Cited By

图 1 掺入0.5‰氯化钠的1, 3-丙二醇的$ \varepsilon '' $

Figure 1. $ \varepsilon '' $ of 1, 3-propanediol doped with 0.5‰ NaCl.

DownLoad: Full-Size Img PowerPoint

图 2 掺入0.5‰氯化钠的1,3-丙二醇的$ \omega \varepsilon '' $和$ \sigma $

Figure 2. $ \omega \varepsilon '' $ and $ \sigma $ of 1,3-propanediol doped with 0.5‰ NaCl.

DownLoad: Full-Size Img PowerPoint

图 3 1, 3-丙二醇原始样品的$ \omega \varepsilon '' $和$ \sigma $

Figure 3. $ \omega \varepsilon '' $ and $ \sigma $ of crude 1, 3-propanediol.

DownLoad: Full-Size Img PowerPoint

图 4 掺入0.5‰氯化钠的1,3-丙二醇及其原始样品的$ {\tau }_{{\mathrm{r}}} $和$ \sigma $

Figure 4. $ {\tau }_{{\mathrm{r}}} $ and $ \sigma $ of 1,3-propanediol doped with 0.5‰ NaCl and its crude sample.

DownLoad: Full-Size Img PowerPoint

图 5 掺入0.1‰氯化镁的三丙二醇和掺入0.1‰氯化钠的一缩二丙二醇及其原始样品的$ {\tau }_{{\mathrm{r}}} $和$ \sigma $

Figure 5. $ {\tau }_{{\mathrm{r}}} $ and $ \sigma $ of tripropylene glycol doped with 0.1‰ MgCl₂ and dipropylene glycol with 0.1‰ NaCl as well as their crude samples.

DownLoad: Full-Size Img PowerPoint

图 6 掺入1‰氯化钠的丙三醇^[16]及其原始样品^[33]的$ {\tau }_{{\mathrm{r}}} $和$ \sigma $

Figure 6. $ {\tau }_{{\mathrm{r}}} $ and $ \sigma $ of glycerol doped with 1‰ NaCl^[16] and its crude sample^[33].

DownLoad: Full-Size Img PowerPoint

图 7 邻苯二甲酸二乙酯和邻苯二甲酸二丙酯原始样品的$ {\tau }_{{\mathrm{r}}} $和$ \sigma $

Figure 7. $ {\tau }_{{\mathrm{r}}} $ and $ \sigma $ of crude diethyl phthalate and dipropyl phthalate.

DownLoad: Full-Size Img PowerPoint

图 8 掺入0.3‰氯化钠的70%1,2-丙二醇和30%1, 3-丙二醇混合液体与掺入0.3‰氯化镁的70%1,3-丁二醇和30%丙三醇混合液体及其原始样品的$ {\tau }_{{\mathrm{r}}} $和$ \sigma $

Figure 8. $ {\tau }_{{\mathrm{r}}} $ and $ \sigma $ of mixed liquid of 70% 1,2-propanediol and 30% 1,3-propanediol doped with 0.3‰ NaCl and mixed liquid of 70% 1,3-butanediol and 30% glycerol doped with 0.3‰ MgCl₂ as well as their crude samples.

DownLoad: Full-Size Img PowerPoint

图 9 2-乙基–1-丁醇的$ \varepsilon '' $

Figure 9. $ \varepsilon '' $ of 2-ethyl-1-butanol.

DownLoad: Full-Size Img PowerPoint

图 10 2-乙基–1-丁醇的$ {\tau }_{{\mathrm{r}}} $^[38], $ {\tau }_{{\mathrm{D}}} $和$ \sigma $

Figure 10. $ {\tau }_{{\mathrm{r}}} $^[38], $ {\tau }_{{\mathrm{D}}} $ and $ \sigma $ of 2-ethyl-1-butanol.

DownLoad: Full-Size Img PowerPoint

[1]	Shirai K, Watanabe K, Momida H 2022 J. Phys. : Condens. Matter 34 375902 Google Scholar
[2]	Ouyang L F, Shen J, Huang Y, Sun Y H, Bai H Y, Wang W H 2023 J. Appl. Phys. 133 85105 Google Scholar
[3]	Böhmer R, Gainaru C, Richert R 2014 Phys. Rep. 545 125 Google Scholar
[4]	Shen J, Zhang H P, Chen Z Q, Ouyang L F, Wang F R, Lu Z, Li M Z, Sun Y H, Bai H Y, Wang W H 2023 Acta Mater. 244 118554 Google Scholar
[5]	Singh A, Singh Y 2023 Phys. Rev. E 107 14119 Google Scholar
[6]	Volbers J C, Lauterböck L, Hofmann N, Glasmacher B 2016 Curr. Dir. Biomed. Eng. 2 315 Google Scholar
[7]	Zhu X C, Miller-Ezzy P, Gluis M, Zhao Y Y, Qin J G, Tang Y H, Liu Y B, Li X X 2023 Aquaculture 574 739650 Google Scholar
[8]	Novikov V N 2016 Chem. Phys. Lett. 659 133 Google Scholar
[9]	Dyre J C 2006 Rev. Mod. Phys. 78 953 Google Scholar
[10]	Kremer F 2002 J. Non-Cryst. Solids 305 1 Google Scholar
[11]	Iacob C, Sangoro J R, Serghei A, Naumov S, Korth Y, Kärger J, Friedrich C, Kremer F 2008 J. Chem. Phys. 129 234511 Google Scholar
[12]	Wang J, Cai Z Q, Kang H, Huo B K, Zhang Y H, Gao Y Q, Li Z J, Feng S D, Wang L M 2024 Mater. Design 238 112665 Google Scholar
[13]	Duan Y J, Nabahat M, Tong Y, Ortiz-Membrado L, Jiménez-Piqué E, Zhao K, Wang Y J, Yang Y, Wada T, Kato H, Pelletier J M, Qiao J C, Pineda E 2024 Phys. Rev. Lett. 132 56101 Google Scholar
[14]	Chen Y X, Feng S D, Lu X Q, Pan S P, Xia C Q, Wang L M 2023 J. Chem. Phys. 158 134511 Google Scholar
[15]	Duan Y J, Zhang L T, Qiao J C, Wang Y J, Yang Y, Wada T, Kato H, Pelletier J M, Pineda E, Crespo D 2022 Phys. Rev. Lett. 129 175501 Google Scholar
[16]	Zhao X Y, Wang L N, Yin H M, Zhou H W, Huang Y N 2019 Chin. Phys. B 28 86601 Google Scholar
[17]	Nernst W 1888 Z. Phys. Chem. 2 613 Google Scholar
[18]	Einstein A 1905 Ann. Phys. (Berlin) 17 549 Google Scholar
[19]	Claisse F, Koenig H P 1956 Acta Metallurgica 4 650 Google Scholar
[20]	Masuhr A, Waniuk T A, Busch R, Johnson W L 1999 Phys. Rev. Lett. 82 2290 Google Scholar
[21]	Wang L M and Sun M D 2010 J. Yanshan Univ. 34 471 [王利民, 孙明道 2010 燕山大学学报 34 471]Google Scholar Wang L M and Sun M D 2010 J. Yanshan Univ. 34 471 Google Scholar
[22]	Tarjus G, Kivelson D 1995 J. Chem. Phys. 103 3071 Google Scholar
[23]	Khrapak S A 2022 J. Mol. Liq. 354 118840 Google Scholar
[24]	Griffin P J, Sangoro J R, Wang Y, Holt A P, Novikov V N, Sokolov A P, Wojnarowska Z, Paluch M, Kremer F 2013 Soft Matter 9 10373 Google Scholar
[25]	Swiergiel J, Bouteiller L, Jadzyn J 2014 Soft Matter 10 8457 Google Scholar
[26]	Kawasaki T, Kim K 2019 Sci. Rep. 9 8118 Google Scholar
[27]	Power G, Vij J K, Johari G P 2007 J. Phys. Chem. B 111 11201 Google Scholar
[28]	Xiao H, Zhang L, Yi J, Li S, Zhao B G, Zhai Q J, Gao Y L 2022 Intermetallics 143 107494 Google Scholar
[29]	Charbonneau P, Jin Y, Parisi G, Zamponi F 2014 Proc. National Academy Sci. 111 15025 Google Scholar
[30]	Starzonek S, Rzoska S J, Drozd-Rzoska A, Pawlus S, Biała E, Martinez-Garcia J C, Kistersky L 2015 Soft Matter 11 5554 Google Scholar
[31]	Zhao X Y, Wang L N, He Y F, Zhou H, Huang Y N 2020 Chem. Phys. 528 110473 Google Scholar
[32]	Ishai P B, Talary M S, Caduff A, Levy E, Feldman Y 2013 Meas. Sci. Technol. 24 102001 Google Scholar
[33]	Lunkenheimer P, Schneider U, Brand R, Loidl A 2000 Contemp. Phys. 41 15 Google Scholar
[34]	Huth H, Wang L M, Schick C, Richert R 2007 J. Chem. Phys. 126 104503 Google Scholar
[35]	Jakobsen B, Maggi C, Christensen T, Dyre J C 2008 J. Chem. Phys. 129 184502 Google Scholar
[36]	Gainaru C, Meier R, Schildmann S, Lederle C, Hiller W, Rössler E A, Böhmer R 2010 Phys. Rev. Lett. 105 258303 Google Scholar
[37]	Gainaru C, Kastner S, Mayr F, Lunkenheimer P, Schildmann S, Weber H J, Hiller W, Loidl A, Böhmer R 2011 Phys. Rev. Lett. 107 118304 Google Scholar
[38]	Bauer S, Burlafinger K, Gainaru C, Lunkenheimer P, Hiller W, Loidl A, Böhmer R 2013 J. Chem. Phys. 138 94505 Google Scholar
[39]	Lu G, Wang L N, Zhao X Y, He Y, Huang Y N 2021 Int. J. Mod. Phys. B 35 2150014 Google Scholar
[40]	Wang L N, Zhao X Y, Huang Y N 2019 Chin. Phys. Lett. 36 97701 Google Scholar
[41]	Ediger M D, Angell C A, Nagel S R 1996 J. Phys. Chem. 100 13200 Google Scholar
[42]	Zhang H, Zhong C, Douglas J F, Wang X D, Cao Q P, Zhang D X, Jiang J Z 2015 J. Chem. Phys. 142 164506 Google Scholar
[43]	Moynihan C T, Macedo P B, Montrose C J, Gupta P K 1976 Ann. Ny. Acad. Sci. 279 15 Google Scholar

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