Suppr超能文献

笼维有序参数的维度研究在玻璃化转变处。

Dimensional study of the caging order parameter at the glass transition.

机构信息

Department of Chemistry, Duke University, Durham, NC 27708, USA.

出版信息

Proc Natl Acad Sci U S A. 2012 Aug 28;109(35):13939-43. doi: 10.1073/pnas.1211825109. Epub 2012 Aug 13.

Abstract

The glass problem is notoriously hard and controversial. Even at the mean-field level, little is agreed upon regarding why a fluid becomes sluggish while exhibiting but unremarkable structural changes. It is clear, however, that the process involves self-caging, which provides an order parameter for the transition. It is also broadly assumed that this cage should have a gaussian shape in the mean-field limit. Here we show that this ansatz does not hold. By performing simulations as a function of spatial dimension d, we find the cage to keep a nontrivial form. Quantitative mean-field descriptions of the glass transition, such as mode-coupling theory, density functional theory, and replica theory, all miss this crucial element. Although the mean-field random first-order transition scenario of the glass transition is qualitatively supported here and non-mean-field corrections are found to remain small on decreasing d, reconsideration of its implementation is needed for it to result in a coherent description of experimental observations.

摘要

玻璃化转变问题一直以来都极具争议性和困难。即使在平均场水平,对于为什么当流体只表现出不显著的结构变化时却变得迟缓,人们也几乎没有达成共识。然而,很明显,这个过程涉及自囚禁,它为转变提供了一个序参量。人们也普遍认为,在平均场极限下,这个牢笼应该具有高斯形状。在这里,我们表明这种假设并不成立。通过执行作为空间维度 d 的函数的模拟,我们发现牢笼保持着非平凡的形状。玻璃化转变的定量平均场描述,如模式耦合理论、密度泛函理论和复制理论,都忽略了这个关键元素。尽管这里定性地支持玻璃化转变的平均场随机一级相变情景,并且发现非平均场修正在降低 d 时仍然很小,但需要重新考虑其实现,以便对实验观察结果进行一致的描述。

相似文献

1
Dimensional study of the caging order parameter at the glass transition.笼维有序参数的维度研究在玻璃化转变处。
Proc Natl Acad Sci U S A. 2012 Aug 28;109(35):13939-43. doi: 10.1073/pnas.1211825109. Epub 2012 Aug 13.
2
Supercooled liquids: equivalence between mode-coupling theory and the replica approach.过冷液体:模式耦合理论与副本方法之间的等效性。
Phys Rev E Stat Nonlin Soft Matter Phys. 2013 Feb;87(2):022135. doi: 10.1103/PhysRevE.87.022135. Epub 2013 Feb 22.
4
Why glass elasticity affects the thermodynamics and fragility of supercooled liquids.为什么玻璃弹性会影响过冷液体的热力学和脆性。
Proc Natl Acad Sci U S A. 2013 Apr 16;110(16):6307-12. doi: 10.1073/pnas.1300534110. Epub 2013 Apr 1.
10
Dimensional study of the dynamical arrest in a random Lorentz gas.随机洛伦兹气体中动力学阻滞的维度研究。
Phys Rev E Stat Nonlin Soft Matter Phys. 2015 Apr;91(4):042313. doi: 10.1103/PhysRevE.91.042313. Epub 2015 Apr 27.

引用本文的文献

1
Understanding, predicting, and tuning the fragility of vitrimeric polymers.理解、预测和调控玻璃态聚合物的脆性。
Proc Natl Acad Sci U S A. 2019 Dec 10;116(50):25013-25022. doi: 10.1073/pnas.1912571116. Epub 2019 Nov 25.
2
3
Quantitative field theory of the glass transition.定量场论玻璃化转变。
Proc Natl Acad Sci U S A. 2012 Nov 13;109(46):18725-30. doi: 10.1073/pnas.1216578109. Epub 2012 Oct 29.

本文引用的文献

1
Quantitative field theory of the glass transition.定量场论玻璃化转变。
Proc Natl Acad Sci U S A. 2012 Nov 13;109(46):18725-30. doi: 10.1073/pnas.1216578109. Epub 2012 Oct 29.
2
Glass transition and random close packing above three dimensions.三维以上的玻璃转变和随机密堆积。
Phys Rev Lett. 2011 Oct 28;107(18):185702. doi: 10.1103/PhysRevLett.107.185702. Epub 2011 Oct 25.
3
Field theory of fluctuations in glasses.玻璃中涨落的场论。
Eur Phys J E Soft Matter. 2011 Sep;34(9):102. doi: 10.1140/epje/i2011-11102-0. Epub 2011 Sep 26.
4
Renormalization group analysis of the random first-order transition.重整化群分析随机一阶相变。
Phys Rev Lett. 2011 Mar 18;106(11):115705. doi: 10.1103/PhysRevLett.106.115705. Epub 2011 Mar 17.
6
Glass transition of hard spheres in high dimensions.高维空间中硬球的玻璃化转变
Phys Rev E Stat Nonlin Soft Matter Phys. 2010 Apr;81(4 Pt 1):041502. doi: 10.1103/PhysRevE.81.041502. Epub 2010 Apr 9.
7
Numerical and theoretical study of a monodisperse hard-sphere glass former.单分散硬球玻璃形成体的数值与理论研究
Phys Rev E Stat Nonlin Soft Matter Phys. 2010 Apr;81(4 Pt 1):040501. doi: 10.1103/PhysRevE.81.040501. Epub 2010 Apr 14.
8
Hard-sphere crystallization gets rarer with increasing dimension.随着维度增加,硬球结晶变得更加罕见。
Phys Rev E Stat Nonlin Soft Matter Phys. 2009 Dec;80(6 Pt 1):061110. doi: 10.1103/PhysRevE.80.061110. Epub 2009 Dec 8.
9

文献检索

告别复杂PubMed语法,用中文像聊天一样搜索,搜遍4000万医学文献。AI智能推荐,让科研检索更轻松。

立即免费搜索

文件翻译

保留排版,准确专业,支持PDF/Word/PPT等文件格式,支持 12+语言互译。

免费翻译文档

深度研究

AI帮你快速写综述,25分钟生成高质量综述,智能提取关键信息,辅助科研写作。

立即免费体验