非晶材料玻璃转变过程中记忆效应的热力学

金肖; 王利民

doi:10.7498/aps.66.176406

摘要

低温下处于非平衡态的非晶材料升温到玻璃转变以上，要先后发生弛豫和回复最终达到平衡过冷液态，其中弛豫过程中释放的能量在回复过程中以等量的方式获取，表现出明显记忆行为.本文基于氧化物、金属与小分子等多种非晶形成体系，全面探讨了在围绕玻璃转变的一个冷却加热循环过程中的焓弛豫特征，建立了弛豫谱，发现弛豫焓在数值上与熔化焓密切相关.基于弛豫焓与非晶材料动力学Fragility之间的关联，展示了非晶体系在动力学极限（m=175）条件下的玻璃转变热力学基本特征，与热力学二级相变进行了对比.研究深化了对非晶弛豫与玻璃转变热力学的理解.

关键词:

玻璃转变 /
弛豫 /
强弱性因子

Abstract

The glass is in a non-equilibrium state in nature, and relaxation might occur towards the equilibrium state at a certain temperature. When heating a quenched glass, relaxation can be resolved as temperature approaches to the glass transition, and further heating leads to enthalpy recovery as the system turns into an equilibrium supercooled liquid. The released energy involving the relaxation relative to the original quenched state is, in magnitude, identical to the gained energy in enthalpy recovery, showing a memory effect. In this paper, we discuss the enthalpy behaviors involved in a cooling and reheating cycle around the glass transition in various glass forming systems such as oxides, metal alloys, and small molecular systems. The cooling and heating rates are fixed to be -/+ 20 K/min with the related cooling and heating heat capacity curves being determined. It is found that the relaxation enthalpy involved in the cooling/heating cycles is closely related to the enthalpy of fusion for the glass forming materials, and the basically linear correlation implies the similarity between the glass transition and melting behaviors with regard to the atomic rearrangements involved in the relaxation and solidification processes. The determining of the cooling and heating heat capacity curves also helps establish the enthalpy relaxation/recovery spectra of various glasses, and the symmetry of the spectrum is associated with the fragility of glass-forming material. For the material of low or medium fragilities, the symmetry of the enthalpy relaxation spectrum is observed to be somehow dependent on the fragility, while for the high fragility glass, the symmetry keeps almost constant. The dependence of fragility on the glass transition thermodynamics is also discussed, and low melting entropy and high fragility are shown to reduce effectively the liquid-crystal Gibbs free energy difference. Using the correlation between the relaxation enthalpy and kinetic fragility reported in our previous studies, the glass transition thermodynamics for the case of the most fragile glass with m= 175 is evaluated, especially compared with the second phase transition of thermodynamics. The results provide a new understanding of the thermodynamics of the relaxation in glassy material and the glass transition.

Keywords:

作者及机构信息

金肖,
王利民

1.
燕山大学材料科学与工程学院, 亚稳材料制备技术与科学国家重点实验室, 秦皇岛 066004

通信作者: 王利民, limin_wang@ysu.edu.cn

基金项目: 国家重点基础研究发展计划（批准号：2015CB856805）、国家自然科学基金（批准号：11474247）和河北省自然科学基金（批准号：A2014203260）资助的课题.

Authors and contacts

1.
State Key Laboratory of Metastable Materials Science and Technology, College of Materials Science and Engineering, Yanshan University, Qinhuangdao 066004, China

Corresponding author: Wang Li-Min, limin_wang@ysu.edu.cn

Funds: Project supported by the National Basic Research Program of China (Grant No. 2015CB856805), the National Natural Science Foundation of China (Grant No. 11474247), and the Natural Science Foundation of Hebei Province, China (Grant No. A2014203260).

参考文献

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[11]	Paluch M, Roland C M, Pawlus S, Ziolo J, Ngai K L 2003 Phys. Rev. Lett. 91 115701
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[13]	Richert R 2010 Phys. Rev. Lett. 104 085702
[14]	Johari G P, Goldstein M 1970 J. Chem. Phys. 53 2372
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[42]	Swallen S F, Kearns K L, Mapes M K, Kim Y S, McMahon R J, Ediger M D, Wu T, Yu L, Satija S 2007 Science 315 353
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[49]	Tool A Q 1946 J. Am. Ceram. Soc. 29 240
[50]	Narayanaswamy O S 1971 J. Am. Ceram. Soc. 54 491
[51]	Angell C A, Wang L M 2003 Biophys. Chem. 105 621
[52]	Badrinarayanan P, Zheng W, Li Q, Simon S L 2007 J. Non-Cryst. Solids 353 2603
[53]	Duvvuri K, Richert R 2002 J. Chem. Phys. 117 4414
[54]	Angell C A 2008 MRS Bull. 33 544
[55]	Molinero V, Sastry S, Angell C A 2006 Phys. Rev. Lett. 97 075701
[56]	Echeverria I, Su P C, Simon S L, Plazek D J 1995 J. Polym. Sci. Part B: Polym. Phys. 33 2457
[57]	Turnbull D 1969 Contemp. Phys. 10 473
[58]	Naumis G G 2006 Phys. Rev. B 73 172202
[59]	Naumis G G, Flores-Ruiz H M 2008 Phys. Rev. B 78 094203
[60]	Kato H, Chen H S, Inoue A 2008 Scripta Mater. 58 1106
[61]	Ke H B, Wen P, Zhao D Q, Wang W H 2010 Appl. Phys. Lett. 96 251902
[62]	Wang W H, Wen P, Zhao D Q, Pan M X, Wang R J 2003 J. Mater. Res. 18 2747
[63]	Wang W H 2013 Prog. Phys. 33 177 (in Chinese) [汪卫华 2013 物理学进展 33 177]
[64]	Deb S K, Wilding M, Somayazulu M, Mcmillan P F 2011 Nature 414 528
[65]	Kechin V V 2001 Phys. Rev. B 65 052102
[66]	Svenson M, Thirion L, Youngman R, Mauro J C, Bauchy M, Rzoska S J, Bockowski M, Smedskjaer M M 2016 Front Mater.: Glass Sci. 3 00014
[67]	Tonkov E Y, Ponyatovsky E G 2004 Phase Transformations of Elements under High Pressure (United States of America: CRC Press) pp172
[68]	Voigtmann T 2008 Phys. Rev. Lett. 101 095701
[69]	Drozd-Rzoska A 2005 Phys. Rev. E 72 041505
[70]	Li P F, Gao P, Liu Y D, Wang L M 2017 J. Alloys Compd. 696 754
[71]	Shadowspeaker L, Busch R 2004 Appl. Phys. Lett. 85 2508
[72]	Turnbull D 1950 J. Appl. Phys. 21 1022
[73]	Thompson C V, Spaepen F 1979 Acta Metall. 27 1855
[74]	Mondal K, Chatterjee U K, Murty B S 2003 Appl. Phys. Lett. 83 671
[75]	Inoue A, Takeuchi A 2002 Mater. Trans. 43 1892
[76]	Angell C A 1997 J. Res. Natl. Inst. Stand. Technol. 102 171
[77]	Angell C A, Smith D L 1982 J. Phys. Chem. 86 3845
[78]	Bendert J C, Gangopadhyay A K, Mauro N A, Kelton K F 2012 Phys. Rev. Lett. 109 185901
[79]	Fecht H J, Perepezko J H, Lee M C, Johnson W L 1990 J. Appl. Phys. 68 4494
[80]	Busch R, Kim Y J, Johnson W L 1995 J. Appl. Phys. 77 4039
[81]	Zaitsev A I, Zaitseva N E, Alekseeva Y P, Kuril'chenko E M, Dunaev S F 2003 Inorg. Mater. 39 816
[82]	Tanaka H 2005 J. Non-Cryst. Solids 351 678

施引文献

[1]	Angell C A 1995 Science 267 1924
[2]	Richert R 2011 Annu. Rev. Phys. Chem. 62 65
[3]	Huang D, Simon S L, McKenna G B 2005 J. Chem. Phys. 122 084907
[4]	Dyre J C 2006 Rev. Mod. Phys. 78 953
[5]	Ediger M D, Angell C A, Nagel S R 1996 J. Phys. Chem. 100 13200
[6]	Debenedetti P G, Stillinger F H 2001 Nature 410 259
[7]	Schönhals A, Kremer F, Schlosser E 1991 Phys. Rev. Lett. 67 999
[8]	Rivera A, León C, Varsamis C P E, Chryssikos G D, Ngai K L, Roland C M, Buckley L J 2002 Phys. Rev. Lett. 88 125902
[9]	Hu L, Yue Y 2009 J. Phys. Chem. C 113 15001
[10]	Capaccioli S, Paluch M, Prevosto D, Wang L M, Ngai K L 2012 J. Phys. Chem. Lett. 3 735
[11]	Paluch M, Roland C M, Pawlus S, Ziolo J, Ngai K L 2003 Phys. Rev. Lett. 91 115701
[12]	Ngai K L 2011 Relaxation and Diffusion in Complex Systems (New York: Springer Science & Business Media) p306
[13]	Richert R 2010 Phys. Rev. Lett. 104 085702
[14]	Johari G P, Goldstein M 1970 J. Chem. Phys. 53 2372
[15]	Kudlik A, Tschirwitz C, Benkhof S, Blochowicz T, Rössler E 1997 Europhys. Lett. 40 649
[16]	Luo P, Li Y Z, Bai H Y, Wen P, Wang W H 2016 Phys. Rev. Lett. 116 175901
[17]	Chen K, Ellenbroek W G, Zhang Z, Chen D T N, Yunker P J, Henkes S, Brito C, Dauchot O, Saarloos W V, Liu A J, Yodh A G 2010 Phys. Rev. Lett. 105 025501
[18]	Brand R, Lunkenheimer P, Loidl A 2002 J. Chem. Phys. 116 10386
[19]	Hodge I M 1994 J. Non-Cryst. Solids 169 211
[20]	Böhmer R, Ngai K L, Angell C A, Plazek D J 1993 J. Chem. Phys. 99 4201
[21]	Hodge I M 1996 J. Non-Cryst. Solids 202 164
[22]	Angell C A 1991 J. Non-Cryst. Solids 131 13
[23]	Kauzmann W 1948 Chem. Rev. 43 219
[24]	Sakka S, Mackenzie J D 1971 J. Non-Cryst. Solids 6 145
[25]	Wunderlich B 1960 J. Phys. Chem. 64 1052
[26]	Adam G, Gibbs J H 1965 J. Chem. Phys 43 139
[27]	Bestul A B, Chang S S 1964 J. Chem. Phys. 40 3731
[28]	Gutzow I, Hench D K L L, Freiman S W 1971 Advances in Nucleation and Crysallization in Glasses (American Ceramic Society) p116
[29]	Gutzow I, Dobreva A 1991 J. Non-Cryst. Solids 129 266
[30]	Simha R, Boyer R F 1962 J. Chem. Phys. 37 1003
[31]	Angell C A, Sichina W 1976 Ann. N. Y. Acad. Sci. 279 53
[32]	Angell C A 1985 J. Non-Cryst. Solids 73 1
[33]	Wang L M, Angell C A, Richert R 2006 J. Chem. Phys. 125 074505
[34]	Wang L M, Richert R 2007 Phys. Rev. B 76 064201
[35]	Qin Q, Mckenna G B 2006 J. Non-Cryst. Solids 352 2977
[36]	Privalko V P 1980 J. Phys. Chem. 84 3307
[37]	Chen Z M, Li Z J, Zhang Y Q, Liu R P, Tian Y J, Wang L M 2014 Eur. Phys. J. E Soft Matter 37 1
[38]	Angell C A, Klein I S 2011 Nature Phys. 7 750
[39]	Defay R, Bellemans A, Prigogine I 1966 Surface Tension and Adsorption (London: Longmans) p432
[40]	Wang L M, Liu R, Wang W H 2008 J. Chem. Phys. 128 164503
[41]	Rao C N R, Rao K J 1977 Phase Transitions in Solids (New York: McGraw-Hill) p115
[42]	Swallen S F, Kearns K L, Mapes M K, Kim Y S, McMahon R J, Ediger M D, Wu T, Yu L, Satija S 2007 Science 315 353
[43]	McKenna G B 2007 J. Non-Cryst. Solids 353 3820
[44]	Wang L M, Velikov V, Angell C A 2002 J. Chem. Phys. 117 10184
[45]	Chen Z M, Zhao L R, Tu W K, Li Z J, Gao Y Q, Wang L M 2016 J. Non-Cryst. Solids 433 20
[46]	Prigogine I, Defay R 1954 Chemical Thermodynamics (London: Longmans) p543
[47]	Moynihan C T, Gupta P K 1978 J. Non-Cryst. Solids 29 143
[48]	Gutzow I S, Mazurin O V, Schmelzer J W P, Todorova S V, Petroff B B, Priven A I 2011 Glasses and the Glass Transition (New Yorlk: John Wiley & Sons) p128
[49]	Tool A Q 1946 J. Am. Ceram. Soc. 29 240
[50]	Narayanaswamy O S 1971 J. Am. Ceram. Soc. 54 491
[51]	Angell C A, Wang L M 2003 Biophys. Chem. 105 621
[52]	Badrinarayanan P, Zheng W, Li Q, Simon S L 2007 J. Non-Cryst. Solids 353 2603
[53]	Duvvuri K, Richert R 2002 J. Chem. Phys. 117 4414
[54]	Angell C A 2008 MRS Bull. 33 544
[55]	Molinero V, Sastry S, Angell C A 2006 Phys. Rev. Lett. 97 075701
[56]	Echeverria I, Su P C, Simon S L, Plazek D J 1995 J. Polym. Sci. Part B: Polym. Phys. 33 2457
[57]	Turnbull D 1969 Contemp. Phys. 10 473
[58]	Naumis G G 2006 Phys. Rev. B 73 172202
[59]	Naumis G G, Flores-Ruiz H M 2008 Phys. Rev. B 78 094203
[60]	Kato H, Chen H S, Inoue A 2008 Scripta Mater. 58 1106
[61]	Ke H B, Wen P, Zhao D Q, Wang W H 2010 Appl. Phys. Lett. 96 251902
[62]	Wang W H, Wen P, Zhao D Q, Pan M X, Wang R J 2003 J. Mater. Res. 18 2747
[63]	Wang W H 2013 Prog. Phys. 33 177 (in Chinese) [汪卫华 2013 物理学进展 33 177]
[64]	Deb S K, Wilding M, Somayazulu M, Mcmillan P F 2011 Nature 414 528
[65]	Kechin V V 2001 Phys. Rev. B 65 052102
[66]	Svenson M, Thirion L, Youngman R, Mauro J C, Bauchy M, Rzoska S J, Bockowski M, Smedskjaer M M 2016 Front Mater.: Glass Sci. 3 00014
[67]	Tonkov E Y, Ponyatovsky E G 2004 Phase Transformations of Elements under High Pressure (United States of America: CRC Press) pp172
[68]	Voigtmann T 2008 Phys. Rev. Lett. 101 095701
[69]	Drozd-Rzoska A 2005 Phys. Rev. E 72 041505
[70]	Li P F, Gao P, Liu Y D, Wang L M 2017 J. Alloys Compd. 696 754
[71]	Shadowspeaker L, Busch R 2004 Appl. Phys. Lett. 85 2508
[72]	Turnbull D 1950 J. Appl. Phys. 21 1022
[73]	Thompson C V, Spaepen F 1979 Acta Metall. 27 1855
[74]	Mondal K, Chatterjee U K, Murty B S 2003 Appl. Phys. Lett. 83 671
[75]	Inoue A, Takeuchi A 2002 Mater. Trans. 43 1892
[76]	Angell C A 1997 J. Res. Natl. Inst. Stand. Technol. 102 171
[77]	Angell C A, Smith D L 1982 J. Phys. Chem. 86 3845
[78]	Bendert J C, Gangopadhyay A K, Mauro N A, Kelton K F 2012 Phys. Rev. Lett. 109 185901
[79]	Fecht H J, Perepezko J H, Lee M C, Johnson W L 1990 J. Appl. Phys. 68 4494
[80]	Busch R, Kim Y J, Johnson W L 1995 J. Appl. Phys. 77 4039
[81]	Zaitsev A I, Zaitseva N E, Alekseeva Y P, Kuril'chenko E M, Dunaev S F 2003 Inorg. Mater. 39 816
[82]	Tanaka H 2005 J. Non-Cryst. Solids 351 678

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