Elemental and cooperative diffusion in a liquid, supercooled liquid and glass resolved

被引:24
|
作者
Cassar, Daniel R. [1 ]
Lancelotti, Ricardo F. [1 ]
Nuernberg, Rafael [1 ]
Nascimento, Marcio L. F. [2 ]
Rodrigues, Alisson M. [1 ]
Diz, Luiza T. [1 ]
Zanotto, Edgar D. [1 ]
机构
[1] Univ Fed Sao Carlos, Dept Mat Engn, CeRTEV Ctr Res Technol & Educ Vitreous Mat, BR-13565905 Sao Carlos, SP, Brazil
[2] Univ Fed Bahia, Polytech Sch, Dept Chem Engn, PROTEC,PEI,Grad Program Ind Engn, Rua Aristides Novis 2, BR-40210630 Salvador, BA, Brazil
来源
JOURNAL OF CHEMICAL PHYSICS | 2017年 / 147卷 / 01期
基金
巴西圣保罗研究基金会;
关键词
LEAD SILICATE-GLASSES; HAVEN RATIO; CRYSTALLIZATION; TRANSITION; VISCOSITY; TEMPERATURE; DYNAMICS; OXIDE;
D O I
10.1063/1.4986507
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The diffusion mechanisms controlling viscous flow, structural relaxation, liquid-liquid phase separation, crystal nucleation, and crystal growth in multicomponent glass-forming liquids are of great interest and relevance in physics, chemistry, materials, and glass science. However, the diffusing entities that control each of these important dynamic processes are still unknown. The main objective of this work is to shed some light on this mystery, advancing the knowledge on this phenomenon. For that matter, we measured the crystal growth rates, the viscosity, and lead diffusivities in PbSiO3 liquid and glass in a wide temperature range. We compared our measured values with published data covering 16 orders of magnitude. We suggest that above a certain temperature range Td (1.2Tg-1.3Tg), crystal growth and viscous flow are controlled by the diffusion of silicon and lead. Below this temperature, crystal growth and viscous flow are more sluggish than the diffusion of silicon and lead. Therefore, Td marks the temperature where decoupling between the (measured) cationic diffusivity and the effective diffusivities calculated from viscosity and crystal growth rates occurs. We reasonably propose that the nature or size of the diffusional entities controlling viscous flow and crystal growth below Td is quite different; the slowest is the one controlling viscous flow, but both processes require cooperative movements of some larger structural units rather than jumps of only one or a few isolated atoms. Published by AIP Publishing.
引用
收藏
页数:10
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