Inherent structure energy is a good indicator of molecular mobility in glasses

被引:29
作者
Helfferich, Julian [1 ]
Lyubimov, Ivan [1 ]
Reid, Daniel [1 ]
de Pablo, Juan J. [1 ,2 ]
机构
[1] Univ Chicago, Inst Mol Engn, 5640 South Ellis Ave, Chicago, IL 60637 USA
[2] Argonne Natl Lab, Div Mat Sci, 9700 S Cass Ave, Argonne, IL 60439 USA
基金
美国国家科学基金会;
关键词
VAPOR-DEPOSITION; STABLE GLASSES; ULTRASTABLE GLASSES; INDOMETHACIN; RELAXATION; TRANSITION; LIQUIDS;
D O I
10.1039/c6sm00810k
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
Glasses produced via physical vapor deposition can display greater kinetic stability and lower enthalpy than glasses prepared by liquid cooling. While the reduced enthalpy has often been used as a measure of the stability, it is not obvious whether dynamic measures of stability provide the same view. Here, we study dynamics in vapor-deposited and liquid-cooled glass films using molecular simulations of a bead-spring polymer model as well as a Lennard-Jones binary mixture in two and three dimensions. We confirm that the dynamics in vapor-deposited glasses is indeed slower than in ordinary glasses. We further show that the inherent structure energy is a good reporter of local dynamics, and that aged systems and glasses prepared by cooling at progressively slower rates exhibit the same behavior as vapor-deposited materials when they both have the same inherent structure energy. These findings suggest that the stability inferred from measurements of the energy is also manifested in dynamic observables, and they strengthen the view that vapor deposition processes provide an effective strategy for creation of stable glasses.
引用
收藏
页码:5898 / 5904
页数:7
相关论文
共 36 条
[1]  
[Anonymous], MONTE CARLO MOL DYNA
[2]   Theoretical perspective on the glass transition and amorphous materials [J].
Berthier, Ludovic ;
Biroli, Giulio .
REVIEWS OF MODERN PHYSICS, 2011, 83 (02) :587-645
[3]   Enthalpy and high temperature relaxation kinetics of stable vapor-deposited glasses of toluene [J].
Bhattacharya, Deepanjan ;
Sadtchenko, Vlad .
JOURNAL OF CHEMICAL PHYSICS, 2014, 141 (09)
[4]  
Binder K., 2011, Glassy Materials and Disordered Solids
[5]   Perspective: The glass transition [J].
Biroli, Giulio ;
Garrahan, Juan P. .
JOURNAL OF CHEMICAL PHYSICS, 2013, 138 (12)
[6]   Structural relaxation made simple [J].
Bitzek, Erik ;
Koskinen, Pekka ;
Gaehler, Franz ;
Moseler, Michael ;
Gumbsch, Peter .
PHYSICAL REVIEW LETTERS, 2006, 97 (17)
[7]   Glass transitions in one-, two-, three-, and four-dimensional binary Lennard-Jones systems [J].
Bruening, Ralf ;
St-Onge, Denis A. ;
Patterson, Steve ;
Kob, Walter .
JOURNAL OF PHYSICS-CONDENSED MATTER, 2009, 21 (03)
[8]   Dynamics of glass-forming liquids. XVI. Observation of ultrastable glass transformation via dielectric spectroscopy [J].
Chen, Z. ;
Sepulveda, A. ;
Ediger, M. D. ;
Richert, R. .
JOURNAL OF CHEMICAL PHYSICS, 2013, 138 (12)
[9]   Molecular Orientation in Stable Glasses of Indomethacin [J].
Dalal, Shakeel S. ;
Ediger, M. D. .
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2012, 3 (10) :1229-1233
[10]   Molecular packing in highly stable glasses of vapor-deposited tris-naphthylbenzene isomers [J].
Dawson, Kevin ;
Kopff, Laura A. ;
Zhu, Lei ;
McMahon, Robert J. ;
Yu, Lian ;
Richert, Ranko ;
Ediger, M. D. .
JOURNAL OF CHEMICAL PHYSICS, 2012, 136 (09)